Updated on 2024/02/08

写真a

 
Sakuda Atsushi
 
Organization
Graduate School of Engineering Division of Science and Engineering for Materials, Chemistry and Biology Associate Professor
School of Engineering Department of Applied Chemistry
Title
Associate Professor
Affiliation
Institute of Engineering
Contact information
メールアドレス

Position

  • Graduate School of Engineering Division of Science and Engineering for Materials, Chemistry and Biology 

    Associate Professor  2022.04 - Now

  • School of Engineering Department of Applied Chemistry 

    Associate Professor  2022.04 - Now

Degree

  • 博士(工学) ( Osaka Prefecture University )

Research Areas

  • Nanotechnology/Materials / Inorganic compounds and inorganic materials chemistry

Research Interests

  • Ionic Conductor

  • All-Solid-State Batteries

  • Materials Chemistry

  • 正極活物質

  • 常温加圧焼結

  • 固体電解質

  • All-solid-state batteries

  • メカノケミカル法

Research subject summary

  • 次世代電池材料の研究

  • 全固体電池材料の研究

Professional Memberships

  • 日本化学会

    2018.01 - Now   Domestic

  • 固体イオニクス学会

    2014.03 - Now   Domestic

  • 日本セラミックス協会

    2013.01 - Now   Domestic

  • 電池技術委員会

    2012.06 - Now   Domestic

  • 電気化学会

    2007.03 - Now   Domestic

Committee Memberships (off-campus)

  • 第64回電池討論会 実行委員   電池技術委員会  

    2023.03 - 2023.12 

  • 電気化学会編集委員   公益社団法人電気化学会 編集委員会  

    2022.03 - Now 

  • 役員(事務局長補佐)   日本セラミックス協会ガラス部会   

    2020.04 - Now 

  • 関西電気化学研究会 世話人   電気化学会関西支部  

    2019.04 - Now 

  • 役員   日本セラミックス協会関西支部  

    2019.04 - Now 

  • 企画委員会委員   日本セラミックス協会関西支部  

    2019.04 - Now 

  • ガラス技術シンポジウム ワーキンググループ委員   ガラス産業連合会(GIC)  

    2019.04 - 2020.03 

  • 第60回ガラスおよびフォトニクス材料討論会 事務局補佐   日本セラミックス協会ガラス部会  

    2019.04 - 2019.12 

  • 第44固体イオニクス討論会 実行委員会委員   日本固体イオニクス学会  

    2018.04 - 2018.12 

  • 第59回電池討論会 実行委員   電池技術委員会  

    2018.01 - 2018.12 

  • 電気化学会第83回大会 実行委員   電気化学会  

    2016.03 

  • 第54回電池討論会 実行委員   電池技術委員会  

    2013.04 - 2013.12 

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Awards

  • 2022 ANNUALLY MOST DOWNLOADED PAPERS Ranked 10th for Electrochemistry

    2023.01   "AC Impedance Analysis of the Degeneration and Recovery of Argyrodite Sulfide-Based Solid Electrolytes under Dry-Room-Simulated Condition"

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    Country:Japan

  • 2022 BIMONTHLY MOST DOWNLOADED PAPERS Ranked 2nd for Electrochemistry from March to April 2022

    2022.05   "AC Impedance Analysis of the Degeneration and Recovery of Argyrodite Sulfide-Based Solid Electrolytes under Dry-Room-Simulated Condition"

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    Country:Japan

  • 令和2年度科学技術分野の文部科学大臣表彰 若手科学者賞

    2020.04   文部科学省  

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    Country:Japan

  • 2019年度電気化学会論文賞(Electrochemistry)

    2020.03   電気化学会  

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    Country:Japan

  • 第7回大阪府立大学TT-netワークショップポスター賞

    2019.10   大阪府立大学テニュアトラック推進会議  

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    Country:Japan

  • Best Poster Award

    2019.06   The 22nd International Conference on Solid State Ionics(SSI-22)  

  • 進歩賞(佐野賞)

    2019.03   電気化学会  

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    Country:Japan

  • 進歩賞

    2018.06   日本セラミックス協会  

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    Country:Japan

  • 倉田 元治 賞

    2013   日本セラミックス協会  

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    Country:Japan

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Papers

  • Addition of Na<sub>3</sub>PO<sub>4</sub> for Enhanced Positive Electrode Performance in All-Solid-State Sodium Batteries Reviewed

    KWON Neung, MOTOHASHI Kota, HOTEHAMA Chie, SAKUDA Atsushi, HAYASHI Akitoshi

    Electrochemistry   advpub ( 0 )   2024( ISSN:13443542

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    Authorship:Corresponding author   Publishing type:Research paper (scientific journal)   International / domestic magazine:International journal  

    DOI: 10.5796/electrochemistry.23-00143

  • Na<inf>6</inf>Ge<inf>2</inf>S<inf>6</inf>O-ionic conductor: Synthesis, structure and ionic transportation

    Ben Yahia H.

    Solid State Ionics   403   2023.12( ISSN:01672738

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  • Latest Trends in Negative Electrode Materials for Next-generation Batteries

    SAKUDA Atsushi, OKUBO Masashi

    Denki Kagaku   91 ( 4 )   370 - 371   2023.12( ISSN:24333255

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  • Crystallization process of Li<inf>3</inf>PS<inf>4</inf> investigated by X-ray total scattering measurement and the reverse Monte Carlo method

    Yoshimoto M.

    Solid State Ionics   401   2023.11( ISSN:01672738

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  • An Electron/Ion Dual Conductive Integrated Cathode Using Cationic/Anionic Redox for High‐Energy‐Density All‐Solid‐State Lithium‐Sulfur Batteries Reviewed

    Wenli Pan, Kentaro Yamamoto, Toshiyuki Matsunaga, Toshiki Watanabe, Mukesh Kumar, Neha Thakur, Tomoki Uchiyama, Masayuki Uesugi, Akihisa Takeuchi, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago, Yoshiharu Uchimoto

    Batteries &amp; Supercaps   7 ( 1 )   2023.10( ISSN:2566-6223

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    Publishing type:Research paper (scientific journal)  

    All‐solid‐state lithium‐sulfur batteries (ASSLSB), composed of sulfur cathode and lithium metal anode with high theoretical capacity, have a potentially higher energy density by weight than a typical lithium‐ion battery (LIB). However, due to insulating sulfur, a relatively large proportion of electronic (carbon) and ionic (solid electrolyte) conductors are mixed for cathode fabrication, leading to inferior practical capacity. Herein, we report that a novel integrated cathode Li2S‐LiI‐MoS2 which has relatively high electronic and ionic conductivities (the order of 10‐4 S cm‐1) without any carbon and solid electrolyte. The ASSLSB with integrated Li2S‐LiI‐MoS2 cathode deliver a remarkably high energy density of 1020 Wh kg‐1 at the cathode level at room temperature. By applying precise X‐ray diffraction, pair distribution function analysis and X‐ray computed tomography, it is found that the formation of an ionic conducting phase composed mainly of LiI during discharge is responsible for the high rate capability. Furthermore, X‐ray absorption fine structure (XAFS) has also revealed the charge compensation mechanism and ascertain the involvement of both Mo 3d and S 3p orbitals during the charging and discharging process. It is believed the strategy will pave the way for developing high practical energy density at room temperature for all‐solid‐state batteries.

    DOI: 10.1002/batt.202300427

  • 3D observation using TEM tomography of solid electrolyte–electrode interface in all-solid-state Li-ion batteries Reviewed

    Satoru Oshiro, Hirofumi Tsukasaki, Hiroshi Nakajima, Keigo Sakamoto, Yuki Hayashi, Atsushi Sakuda, Akitoshi Hayashi, Shigeo Mori

    Journal of Solid State Electrochemistry   2023.10( ISSN:14328488

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    Publishing type:Research paper (scientific journal)  

    DOI: 10.1007/s10008-023-05714-4

  • Ex situ TEM observations of the SnB<inf>2</inf>O<inf>4</inf> glass electrode in all-solid-state lithium-ion batteries after charge–discharge process

    Hirofumi Tsukasaki, Keigo Sakamoto, Yuki Hayashi, Hiroshi Nakajima, Takuya Kimura, Atsushi Sakuda, Akitoshi Hayashi, Shigeo Mori

    Solid State Ionics   399   2023.10( ISSN:0167-2738

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    Publishing type:Research paper (scientific journal)  

    As an environmentally friendly Pb-free material, SnO–B2O3 glass is considered a next-generation negative-electrode active material for all-solid-state lithium-ion batteries. Using SnB2O4 (50SnO·50B2O3) as a negative-electrode active material, the all-solid-state cells exhibit a high initial discharge capacity of approximately 950 mAh g−1. In this study, the microstructures of the SnB2O4 glassy electrode composites are investigated to clarify the charge–discharge behavior and charge–discharge mechanisms of the SnB2O4 glassy electrode composites using transmission electron microscopy (TEM). Here, ex situ TEM observations capture Sn and Li–Sn alloy nanocrystallites in the amorphous matrix. Li+ is incorporated into Sn, and Li–Sn alloy nanocrystallites are formed after initial lithiation. Further, Li+ is extracted from Li–Sn alloys to form Sn nanocrystallites after initial delithiation. In particular, Sn is lithiated and delithiated during the first cycle. However, as the cycle number increases, the capacity deteriorates. Ex situ TEM observations further reveal that Li–Sn alloys remain unchanged even after delithiation, and the crystallite size increases significantly. It is thus found that the capacity deterioration is attributed to the irreversible Li insertion/extraction between Sn and Li–Sn alloys.

    DOI: 10.1016/j.ssi.2023.116288

  • Synthesis, structure and properties of Na<inf>4</inf>GeS<inf>4</inf>

    Ben Yahia H.

    Journal of Alloys and Compounds   960   2023.10( ISSN:09258388

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  • Metal Polysulfides as High Capacity Electrode Active Materials — Toward Superior Secondary Batteries Based on Sulfur Chemistry

    SAKUDA Atsushi

    Electrochemistry   91 ( 10 )   102003 - 102003   2023.10( ISSN:13443542

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    <p>Lithium/transition-metal polysulfide batteries are a promissing candidate for next-generation batteries with high energy densities. Transition metal polysulfides and lithium- or sodium-containing transition metal sulfides exhibit large reversible capacities based on multi-electron processes, owing to the redox reactions of S in addition to the transition metal. This comprehensive paper aims to address the idea, research, and development of transition metal polysulfide electrode active materials and summarizes the author’s views on the concept of transition metal polysulfide electrodes. Furthermore, the diversity of coordination structures and unique structural changes during charging and discharging will be discussed.</p>

    DOI: 10.5796/electrochemistry.23-00030

  • Synthesis and ionic conductivity of an argyrodite-type Li6SbS5I electrolyte

    Takuya Kimura, Ryo Izawa, Chie Hotehama, Kotaro Fujii, Atsushi Sakuda, Masatomo Yashima, Masahiro Tatsumisago, Akitoshi Hayashi

    Solid State Ionics   399   116287 - 116287   2023.10( ISSN:0167-2738

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    Publishing type:Research paper (scientific journal)  

    DOI: 10.1016/j.ssi.2023.116287

  • Mechanism Exploration of Li<inf>2</inf>S-Li<inf>2</inf>O-LiI Positive Electrodes with High Capacity and Long Cycle Life via TEM Observation

    Jiong Ding, Yushi Fujita, Hirofumi Tsukasaki, Hiroshi Nakajima, Atsushi Sakuda, Akitoshi Hayashi, Shigeo Mori

    ACS Applied Energy Materials   6 ( 18 )   9737 - 9742   2023.09

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    Publishing type:Research paper (scientific journal)  

    All-solid-state rechargeable batteries with Li2S-based positive electrode active materials have received much attention due to their safety and high capacity. Since Li2S has quite a low electronic and ionic conductivity, Li2S in the positive electrode is combined with conductive agents, such as conductive carbons and sulfide solid electrolytes, to improve its cycle performance. Recently, we developed a remarkable Li2S-based positive electrode active material: Li2S-Li2O-LiI. Particularly, Li2S-(66.7Li2O·33.3LiI) exhibited high capacity and long-term cycle performance. In this research, we investigated the microstructural changes of the Li2S-(66.7Li2O·33.3LiI) positive electrode by using transmission electron microscopy (TEM) to clarify the long-term cycling factor. TEM observation revealed that Li2S becomes amorphous after charge processes, while the Li2S antifluorite structure is restored after discharge processes, indicating reversible microstructural changes in Li2S. Moreover, we discovered that numerous Li2S nanocrystals can maintain a size of less than 10 nm during discharge processes. This factor significantly contributes to the long-term rechargeability of these active materials.

    DOI: 10.1021/acsaem.3c01858

  • Latest Trends in Large Storage Batteries for Stationary Use

    KOBAYASHI Hironori, SAKUDA Atsushi

    Denki Kagaku   91 ( 3 )   293 - 294   2023.09( ISSN:24333255

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  • Mechanochemical Synthesis and Characterization of Na<sub>3−</sub><i><sub>x</sub></i>In<sub>1−</sub><i><sub>x</sub></i>Zr<i><sub>x</sub></i>Cl<sub>6</sub> Solid Electrolyte

    OKADA Yuya, KIMURA Takuya, MOTOHASHI Kota, SAKUDA Atsushi, HAYASHI Akitoshi

    Electrochemistry   91 ( 7 )   077009 - 077009   2023.07( ISSN:13443542

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    <p>All-solid-state batteries (ASSBs) have attracted significant attention as alternatives to Li-ion batteries. In ASSBs, solid electrolytes (SEs) play a key role. While many halide Li-ion conductors have been reported, only a few Na-ion conductors have been reported. In this study, a new phase of Na<sub>3</sub>InCl<sub>6</sub> with a cryolite-type monoclinic structure was prepared using a mechanochemical method. The new phase showed higher conductivity than the previously reported trigonal Na<sub>3</sub>InCl<sub>6</sub> and underwent a phase transition to trigonal phase when heat-treated at 90 °C. A Zr-substituted system of Na<sub>3−</sub><i><sub>x</sub></i>In<sub>1−</sub><i><sub>x</sub></i>Zr<i><sub>x</sub></i>Cl<sub>6</sub> was mechanochemically prepared. The obtained solid solutions with monoclinic structures based on Na<sub>3</sub>InCl<sub>6</sub> were formed in the compositions of <i>x</i> = 0.1–0.9. The Rietveld refinement results showed a decrease in Na occupancy at the octahedral sites and slight change at the prismatic sites. Bond valence sum mapping results showed that Na ions diffused alternately through two types of sites, suggesting that the introduction of Na vacancies at either site had a positive effect on Na-ion conduction. The ionic conductivity increased to approximately 10<sup>−5</sup> S cm<sup>−1</sup> with an increase in the number of Na vacancies when <i>x</i> was greater than 0.6. This report describes one of the few Na-ion conducting chlorides with high conductivity.</p>

    DOI: 10.5796/electrochemistry.23-00054

  • High-Packing-Density Electrodes by Self-forming Ion Conduction Pathway During Charge Process for All-Solid-State Lithium Ion Batteries Reviewed

    Kentaro Yamamoto, Yao Xiao, Toshiki Watanabe, Atsushi Sakuda, Masakuni Takahashi, Wenli Pan, Koji Nakanishi, Toshiyuki Matsunaga, Masayuki Uesugi, Akihisa Takeuchi, Kentaro Uesugi, Akitoshi Hayashi, Masahiro Tatsumisago, Yoshiharu Uchimoto

    The Journal of Physical Chemistry C   127 ( 30 )   14656 - 14665   2023.07( ISSN:1932-7447

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    Publishing type:Research paper (scientific journal)  

    DOI: 10.1021/acs.jpcc.3c02851

  • Hydrogen Components of a Sulfide-based Argyrodite-Type Solid Electrolyte after Moisture Exposure

    Morino Y.

    Journal of Physical Chemistry C   127 ( 28 )   13616 - 13622   2023.07( ISSN:19327447

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  • Fabrication of Li Metal-Sulfide Solid Electrolyte Interface Using Ultrasonic-Assisted Fusion Welding Process

    Kitaura H.

    Journal of Physical Chemistry C   127 ( 26 )   12477 - 12483   2023.07( ISSN:19327447

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  • Stabilizing High-Temperature α-Li<inf>3</inf>PS<inf>4</inf> by Rapidly Heating the Glass

    Kimura T.

    Journal of the American Chemical Society   145 ( 26 )   14466 - 14474   2023.07( ISSN:00027863

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  • Stack Pressure Dependence of Li Stripping/Plating Performance in All-Solid-State Li Metal Cells Containing Sulfide Glass Electrolytes

    Asakura T.

    ACS Applied Materials and Interfaces   15 ( 26 )   31403 - 31408   2023.07( ISSN:19448244

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  • Mechanochemical Synthesis and Structure of the Alkali Metal Magnesium Chalcogenide Na<inf>6</inf>MgS<inf>4</inf>

    Ben Yahia H.

    Inorganic Chemistry   62 ( 26 )   10440 - 10449   2023.07( ISSN:00201669

  • Nanoscale coexistence of polar-nonpolar domains underlying oxygen storage properties in Ho(Mn,Ti)O3+δ

    Hiroshi Nakajima, Kento Uchihashi, Hirofumi Tsukasaki, Daisuke Morikawa, Hiroyuki Tanaka, Tomohiro Furukawa, Kosuke Kurushima, Jun Yamasaki, Hiroki Ishibashi, Yoshiki Kubota, Atsushi Sakuda, Akitoshi Hayashi, Shigeo Mori

    Physical Review Research   5 ( 2 )   2023.06( ISSN:26431564

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    Publishing type:Research paper (scientific journal)  

    DOI: 10.1103/PhysRevResearch.5.023203

  • Spectroscopic Investigation of Li<sub>3</sub>PS<sub>4</sub>-LiI Sulfide-Based Glass-Ceramic Solid Electrolytes after Moisture Exposure Reviewed

    Yusuke Morino, Hikaru Sano, Koji Kawamoto, Hiroyuki Higuchi, Noriyuki Yamamoto, Atsunori Matsuda, Ken-ichi Fukui, Atsushi Sakuda, Akitoshi Hayashi

    The Journal of Physical Chemistry C   127 ( 25 )   12342 - 12348   2023.06( ISSN:1932-7447

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    Sulfide-based solid electrolytes (SEs) have been extensively studied because of their high lithium-ion conductivities. Among the solid electrolytes, glass or glass-ceramic SEs have suitable thermoplastic characteristics for battery manufacturing processes. However, sulfide-based SEs react strongly with moisture, resulting in toxic H2S gas generation and reduced lithium-ion conductivity. Although the effects of moisture exposure on sulfide-based SEs have been investigated by some researchers, related studies are scarce and further research is required. In this study, X-ray photoelectron spectroscopy (XPS) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) were performed to investigate the structural changes in a glass-ceramic sulfide-based SE, viz., Li3PS4-0.2LiI before and after exposure to moisture, focusing on the changes in the surface chemical species, adsorbed H2O, and related species. In addition, SE samples exposed to moist air were subjected to recovery treatment by vacuum heating. XPS and DRIFTS analyses revealed that the main reason for the decrease in the lithium-ion conductivity of the glass-ceramic SE after moisture exposure is the adsorption of water onto the SE surface and/or its hydration. In particular, the H2O layer adsorbed to the SE surface physically and/or chemically decreases the lithium-ion conductivity at the grain boundaries (i.e., SE/SE interface), although the bulk conduction is maintained.

    DOI: 10.1021/acs.jpcc.3c02399

  • Tin Interlayer at the Li/Li<inf>3</inf>PS<inf>4</inf> Interface for Improved Li Stripping/Plating Performance

    Inaoka T.

    Journal of Physical Chemistry C   127 ( 22 )   10453 - 10458   2023.06( ISSN:19327447

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  • Crystal structure changes of thio-LISICON electrolytes in humid atmosphere

    Kimura Takuya, Nakano Takumi, Sakuda Atsushi, Tatsumisago Masahiro, Hayashi Akitoshi

    Journal of the Ceramic Society of Japan   131 ( 6 )   166 - 171   2023.06( ISSN:18820743

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    <p>Sulfide electrolytes are among the most notable materials because of their high ionic conductivity and ductility. Their primary drawback is that they are sensitive to humidity and must be handled in an inert atmosphere to prevent degradation. Understanding the degradation mechanism is necessary to establish methods for overcoming it; however, whether or not it depends on the composition of the electrolytes is not yet clear. In this study, we systematically investigated the crystal structure changes in a humid atmosphere for crystalline sulfide electrolytes (thio-LISICONs). Eight thio-LISICONs, Li<i><sub>x</sub></i>MS<sub>4</sub> (<i>x</i> = 3–5; M = Al, Ga, Si, Ge, Sn, P, As, and Sb), were prepared using a mechanochemical process and subsequent heat treatment. The exposure behavior was observed using in situ humidity exposure X-ray diffraction (XRD). In a humid atmosphere with a dew point of −8 °C, the electrolytes, transformed into new hydrates, all except for Li<sub>5</sub>AlS<sub>4</sub> and Li<sub>5</sub>GaS<sub>4</sub>, which did not change. Hydrated Li<sub>4</sub>MS<sub>4</sub> (M = Si and Ge) has the same crystal structure as that of the known hydrate Li<sub>4</sub>SnS<sub>4</sub>·13H<sub>2</sub>O. The crystal structures of hydrated Li<sub>3</sub>MS<sub>4</sub> (M = P, As, and Sb) were identical to each other but different from those of Li<sub>3</sub>AsS<sub>4</sub>·8H<sub>2</sub>O. This study revealed that the hydration behavior of the sulfide electrolytes depends on their central element groups.</p>

    DOI: 10.2109/jcersj2.23015

  • Preparation of Li<sub>4</sub>GeO<sub>4</sub>–Li<sub>3</sub>VO<sub>4</sub> based electrolytes via mechanochemical treatment

    Okushima Chihiro, Yoneda Yohei, Kimura Takuya, Motohashi Kota, Sakuda Atsushi, Tatsumisago Masahiro, Hayashi Akitoshi

    Journal of the Ceramic Society of Japan   131 ( 6 )   141 - 145   2023.06( ISSN:18820743

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    <p>Pseudo-binary electrolytes of (100 − <i>x</i>)Li<sub>4</sub>GeO<sub>4</sub>·<i>x</i>Li<sub>3</sub>VO<sub>4</sub> (<i>x</i> = 0, 10, 20, 30, 40, and 50 mol %) and pseudo-ternary electrolytes of 45Li<sub>4</sub>GeO<sub>4</sub>·45Li<sub>3</sub>VO<sub>4</sub>·10Li<i><sub>a</sub></i>MO<i><sub>b</sub></i> (M = B, Si, P, S, Mo, and W) with lithium superionic conductor (LISICON) type structures were prepared by mechanochemical treatment and subsequent heat treatment. For the (100 − <i>x</i>)Li<sub>4</sub>GeO<sub>4</sub>·<i>x</i>Li<sub>3</sub>VO<sub>4</sub> heated samples with LISICON-type structure, the activation energy decreased with increasing Li<sub>3</sub>VO<sub>4</sub> content, and the <i>x</i> = 50 sample showed a high conductivity of 1.1 × 10<sup>−4</sup> S cm<sup>−1</sup> at 25 °C. The 45Li<sub>4</sub>GeO<sub>4</sub>·45Li<sub>3</sub>VO<sub>4</sub>·10Li<i><sub>a</sub></i>MO<i><sub>b</sub></i> heated samples with LISICON-type structure showed a conductivity of approximately 10<sup>−5</sup> S cm<sup>−1</sup> at 25 °C, and the larger “<i>a</i>” as the Li content in Li<i><sub>a</sub></i>(Ge<sub>0.45</sub>M<sub>0.1</sub>V<sub>0.45</sub>)O<i><sub>b</sub></i> contributed to improving the ionic conduction properties of this system.</p>

    DOI: 10.2109/jcersj2.23014

  • Surface Degeneration of Li<sub>3</sub>PS<sub>4</sub>–LiI Glass-Ceramic Electrolyte by Exposure to Humidity-Controlled Air and Its Recovery by Thermal Treatment

    SANO Hikaru, MORINO Yusuke, MATSUMURA Yasuyuki, KAWAMOTO Koji, HIGUCHI Hiroyuki, YAMAMOTO Noriyuki, MATSUDA Atsunori, TSUKASAKI Hirofumi, MORI Shigeo, SAKUDA Atsushi, HAYASHI Akitoshi

    Electrochemistry   91 ( 5 )   057004 - 057004   2023.05( ISSN:13443542

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    <p>Sulfide-based solid electrolytes are desirable for use in all-solid-state batteries owing to their high ionic conductivity and plasticity. However, they generally degrade upon exposure to water and can generate toxic hydrogen sulfide even in dry-room atmospheres. To prevent their degradation, surface stabilization is required and further research into the degradation mechanism is necessary. In the present study, the stability of Li<sub>3</sub>PS<sub>4</sub>–LiI glass ceramic (LPSI) has been examined under low-humidity conditions. In contrast to an argyrodite-type solid electrolyte, exposure of LPSI to dry air with a dew point of −20 °C resulted in low H<sub>2</sub>S-gas generation and reduced ionic conductivity of LPSI. Since the conductivity mostly recovered after vacuum heating at 100 °C, the H<sub>2</sub>S generation is not considered to be the major reason for the reduction in conductivity. On the contrary, it is suggested that water molecules are present on the LPSI powder particles after dry-air exposure, resulting in the formation of a degraded LPSI layer and low ionic conductivity, and that most of the water molecules are removed during vacuum heating, resulting in the recovery of conductivity. Furthermore, optimal vacuum-heating conditions were obtained from X-ray diffraction and temperature-programmed desorption-mass spectrometry measurements, indicating an optimal temperature and heating time of 100 °C and 2 h, respectively. Impedance measurements were used to probe the degradation of the surface layer. The condition of the surface layer was affected by the pellet-forming pressure, and it was easier to detect the degradation of the surface layer when the pellets were formed at low pressures. This paper contributes to the formulation of guidelines for the development of water-resistant solid electrolytes.</p>

    DOI: 10.5796/electrochemistry.23-00029

  • Twinned single crystal structure of Li<inf>4</inf>P<inf>2</inf>S<inf>6</inf>

    Ben Yahia H.

    Zeitschrift fur Kristallographie - Crystalline Materials   238 ( 5-6 )   209 - 216   2023.05( ISSN:21944946

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  • Degradation of an Argyrodite-type Sulfide Solid Electrolyte by a Trace of Water: A Spectroscopic Analysis Reviewed

    Y. Morino, H. Sano, K. Kawamoto, K. Fukui, M. Takeuchi, A. Sakuda and A. Hayashi

    Solid State Ionics   392 ( (116162) )   1 - 7   2023.04

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    Kind of work:Joint Work  

    DOI: https://doi.org/10.1016/j.ssi.2023.116162

  • Degradation of an argyrodite-type sulfide solid electrolyte by a trace of water: A spectroscopic analysis Reviewed

    Yusuke Morino, Hikaru Sano, Koji Kawamoto, Ken-ichi Fukui, Masato Takeuchi, Atsushi Sakuda, Akitoshi Hayashi

    Solid State Ionics   392   116162 - 116162   2023.04( ISSN:0167-2738

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    Publishing type:Research paper (scientific journal)  

    DOI: 10.1016/j.ssi.2023.116162

  • Hard Carbon–Sulfide Solid Electrolyte Interface in All-Solid-State Sodium Batteries

    YOSHIDA Wataru, NASU Akira, MOTOHASHI Kota, TATSUMISAGO Masahiro, SAKUDA Atsushi, HAYASHI Akitoshi

    Electrochemistry   91 ( 3 )   037009 - 037009   2023.03( ISSN:13443542

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    Publishing type:Research paper (scientific journal)  

    <p>Hard carbon is a promising negative electrode material for sodium-ion batteries that operate at low potentials. However, reversible and high-capacity charging and discharging in all-solid-state sodium batteries with hard carbon electrodes using sulfide solid electrolytes have not been reported. This study reports that reductive decomposition of the sulfide solid electrolyte occurs at both the negative composite electrode and the interface between the negative electrode layer and the solid electrolyte layer. In the first cycle, the all-solid-state cell with a composite electrode containing a Na<sub>3</sub>PS<sub>4</sub> solid electrolyte exhibited a large irreversible capacity of 561 mAh g<sup>−1</sup> because of the reductive decomposition of Na<sub>3</sub>PS<sub>4</sub> to Na<sub>2</sub>S and Na<sub>3</sub>P. The use of a Na<sub>3</sub>BS<sub>3</sub> glass electrolyte with reduction stability can lead to the successful charging and discharging of all-solid-state cell that utilizes hard carbon. This glass electrolyte can serve as a solid electrolyte for the negative composite electrode and as a buffer layer between the negative electrode layer and the solid electrolyte layer. Hence, it can also help suppress the irreversible capacity of the cell to 122 mAh g<sup>−1</sup>.</p>

    DOI: 10.5796/electrochemistry.23-00009

  • Positive Electrode Performance of All-Solid-State Battery with Sulfide Solid Electrolyte Exposed to Low-Moisture Air

    MORINO Yusuke, SANO Hikaru, SHIOTA Akihiro, KAWAMOTO Koji, TAKAHASHI Tsukasa, MIYASHITA Norihiko, SAKUDA Atsushi, HAYASHI Akitoshi

    Electrochemistry   91 ( 3 )   037005 - 037005   2023.03( ISSN:13443542

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    <p>All-solid-state batteries (ASSBs) using sulfide solid electrolytes (SEs) are attractive candidates as next-generation energy devices having longer lifetimes than liquid-type lithium-ion batteries (LIBs) using organic solvents. Sulfide SEs are known that to suffer a decrease in their ionic conductivity and generate toxic hydrogen sulfide when exposed to moisture even in an environment such as in a dry room. However, the influence of the exposure to moisture on the ASSB cell performance has not been fully elucidated so far. Aiming at filling this gap of knowledge, this paper describes the investigation of the influence of moisture on the durability of an ASSB positive electrode with sulfide SE unexposed or exposed to dry-room-simulated air with dew point of −20 °C in this study. After the cell durability evaluation, time-of-flight secondary-ion mass spectrometry (ToF-SIMS) measurements were performed on positive electrode, and a characteristic degradation mode was observed in the cell using the exposed SE.</p>

    DOI: 10.5796/electrochemistry.23-00003

  • Vacancies Introduced during the Crystallization Process of the Glass-Ceramics Superionic Conductor, Na<sub>3</sub>PS<sub>4</sub>, Investigated by Neutron Total Scattering and Reverse Monte Carlo Method

    Kazutaka Ikeda, Takuya Kimura, Koji Ohara, Toyoto Sato, Hidetoshi Ohshita, Atsushi Sakuda, Akitoshi Hayashi

    The Journal of Physical Chemistry C   127 ( 13 )   6199 - 6206   2023.03( ISSN:1932-7447

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    DOI: 10.1021/acs.jpcc.3c00414

  • Lithium ion transport environment by molecular vibrations in ion‐conducting glasses Reviewed

    Hiroki Yamada, Koji Ohara, Satoshi Hiroi, Atsushi Sakuda, Kazutaka Ikeda, Takahiro Ohkubo, Kengo Nakada, Hirofumi Tsukasaki, Hiroshi Nakajima, Laszlo Temleitner, Laszlo Pusztai, Shunsuke Ariga, Aoto Matsuo, Jiong Ding, Takumi Nakano, Takuya Kimura, Ryo Kobayashi, Takeshi Usuki, Shuta Tahara, Koji Amezawa, Yoshitaka Tateyama, Shigeo Mori, Akitoshi Hayashi

    ENERGY & ENVIRONMENTAL MATERIALS   2023.03( ISSN:2575-0356

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    Publishing type:Research paper (scientific journal)  

    DOI: 10.1002/eem2.12612

  • Crystalline/Amorphous LiCoO2-Li2SO4 Nanoheterostructured Materials for High-Voltage All-Solid-State Lithium Batteries Reviewed

    T. Hakari, M. Deguchi, A. Sakuda, M. Tatsumisago and A. Hayashi

    J. Power Sources   562 ( 1(232739) )   1 - 7   2023.02

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    Kind of work:Joint Work  

    DOI: https://doi.org/10.1016/j.jpowsour.2023.232739

  • Hydration and Dehydration Behavior of Li<inf>4</inf>SnS<inf>4</inf> for Applications as a Moisture-Resistant All-Solid-State Battery Electrolyte

    Kimura T.

    Journal of Physical Chemistry C   127 ( 3 )   1303 - 1309   2023.01( ISSN:19327447

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  • Hydration and Dehydration Behavior of Li4SnS4 for Applications as a Moisture-Resistat All-Solid-State Battery Electrolyte Reviewed

    T. Kimura, T. Nakano, A. Sakuda, M. Tatsumisago and A. Hayashi

    J. Phys. Chem. C   127 ( 3 )   1303 - 1309   2023.01

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    DOI: https://doi.org/10.1021/acs.jpcc.2c06593

  • Unique lithium precipitation behavior inside Li<sub>3</sub>PS<sub>4</sub> solid electrolyte observed via multimodal/multiscale <i>operando</i> X-ray computed tomography

    Jaehee Park, Toshiki Watanabe, Kentaro Yamamoto, Tomoki Uchiyama, Tsuyoshi Takami, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago, Yoshiharu Uchimoto

    Chemical Communications   59 ( 50 )   7799 - 7802   2023( ISSN:1359-7345

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    Problem of lithium dendrite must be addressed for the practical lithium metal all-solid-state batteries. Herein, three-dimensional morphological changes within Li<sub>3</sub>PS<sub>4</sub> electrolyte away from anode were observed using operando X-ray computed...

    DOI: 10.1039/d2cc05224e

    PubMed

  • Structural Investigation of Li<inf>2</inf>O-LiI Amorphous Solid Electrolytes

    Yushi Fujita, Takuya Kimura, Minako Deguchi, Kota Motohashi, Atsushi Sakuda, Masahiro Tatsumisago, Hirofumi Tsukasaki, Shigeo Mori, Kazutaka Ikeda, Koji Ohara, Naoaki Kuwata, Koji Amezawa, Akitoshi Hayashi

    Journal of Physical Chemistry C   127 ( 30 )   14687 - 14693   2023( ISSN:1932-7447

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    All-solid-state lithium-ion batteries with flame-retardant inorganic solid electrolytes are promising because of their safety. Oxide-based solid electrolytes are attractive, owing to their high chemical stability and lithium-ion conductivity. The development of new oxide-based solid electrolytes with high ionic conductivity and ductility is crucial for improving the overall performance of all-solid-state batteries. Recently, the synthesis of amorphous solid electrolytes using mechanochemical processes was explored. Among them, a Li2O-LiI amorphous solid electrolyte has been shown to have high ionic conductivity (10-5 S cm-1 at 25 °C) and ductility comparable to those of sulfide solid electrolytes. However, the detailed structure and the ionic conduction mechanism of the Li2O-LiI electrolyte are not well understood. In this study, structural analysis of the Li2O-LiI electrolyte was conducted to elucidate its structure and conduction mechanism using neutron diffraction, transmission electron microscopy, 7Li magic-angle spinning nuclear magnetic resonance, and X-ray photoelectron spectroscopy. These structural analyses suggested that the Li2O-LiI electrolyte was primarily composed of amorphous components, mainly iodide and oxide ions, with high ionic mobility. The results of this study are useful for the further development of oxide-based solid electrolytes.

    DOI: 10.1021/acs.jpcc.3c03876

  • Mechanochemical Synthesis and Characterization of K<inf>2+x</inf>Zr<inf>1-x</inf>Y<inf>x</inf>Cl<inf>6</inf>: Potassium-Ion-Conducting Chloride

    Yuya Okada, Akira Nasu, Takuya Kimura, Hirofumi Tsukasaki, Shigeo Mori, Hamdi Ben Yahia, Kota Motohashi, Atsushi Sakuda, Akitoshi Hayashi

    Chemistry of Materials   35 ( 18 )   7422 - 7429   2023( ISSN:0897-4756

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    K-ion batteries are attracting attention as rechargeable batteries following Li-ion and Na-ion batteries. However, their safety is of concern owing to the use of organic electrolytes. The use of solid electrolytes instead of organic electrolytes can resolve this problem. Chloride solid electrolytes have attracted attention in recent years as Li- and Na-ion conductors, but reports on chloride K-ion conductors have been scarce. In this study, new K-ion-conducting chlorides, K2+xZr1-xYxCl6 (x = 0-1), were prepared by a mechanochemical method. The X-ray powder diffraction (XRPD) patterns of the prepared solid electrolytes exhibited broad Bragg peaks, and the high-resolution transmission electron microscopy observations revealed the presence of nanocrystals dispersed in amorphous matrixes. New crystalline phases, closely related to monoclinic K2TeCl6, were precipitated in the K2+xZr1-xYxCl6 matrixes at x = 0-0.4. The Rietveld refinements of the XRPD patterns for the new phases revealed that the excess of K, introduced by Y substitution, occupied the vacant B′ octahedral site of the cation-deficient double perovskite A2BB′X6 structure. The conductivity at 25 °C of the K2+xZr1-xYxCl6 chlorides exceeded 10-7 S cm-1 at x = 0-0.4, and a maximum conductivity of 9.2 × 10-7 S cm-1 was achieved at x = 0.3. Heat treatment above 400 °C of the K2+xZr1-xYxCl6 electrolyte with x = 0.3 resulted in crystallization of the amorphous components, decomposition of the phase into a mixture of K2ZrCl6 and K3YCl6, and a decrease of the ionic conductivity. In addition to the K concentration and crystalline phase in the electrolytes, the amorphous components also play a key role in the high ionic conductivity of the K2+xZr1-xYxCl6 chlorides.

    DOI: 10.1021/acs.chemmater.3c00185

  • Improving electrochemical performance of Li<sub>2</sub>S cathode based on point defect control with cation/anion dual doping

    Pan Wenli, Kentaro Yamamoto, Nobuya Machida, Toshiyuki Matsunaga, Mukesh Kumar, Neha Thakur, Toshiki Watanabe, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago, Yoshiharu Uchimoto

    Journal of Materials Chemistry A   11 ( 45 )   24637 - 24643   2023( ISSN:2050-7488

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    Li<sub>2</sub>S is a promising cathode candidate for all-solid-state batteries (ASSBs) because of its high theoretical capacity and availbility of coupling with Li-free anode or anode less electrode. However, ionically insulating...

    DOI: 10.1039/d3ta05426h

  • High Capacity Li<inf>2</inf>S–Li<inf>2</inf>O–LiI Positive Electrodes with Nanoscale Ion-Conduction Pathways for All-Solid-State Li/S Batteries

    Yushi Fujita, Atsushi Sakuda, Yuki Hasegawa, Minako Deguchi, Kota Motohashi, Ding Jiong, Hirofumi Tsukasaki, Shigeo Mori, Masahiro Tatsumisago, Akitoshi Hayashi

    Small   19 ( 36 )   e2302179   2023( ISSN:1613-6810

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    All-solid-state lithium–sulfur (Li/S) batteries are promising next-generation energy-storage devices owing to their high capacities and long cycle lives. The Li2S active material used in the positive electrode has a high theoretical capacity; consequently, nanocomposites composed of Li2S, solid electrolytes, and conductive carbon can be used to fabricate high-energy-density batteries. Moreover, the active material should be constructed with both micro- and nanoscale ion-conduction pathways to ensure high power. Herein, a Li2S–Li2O–LiI positive electrode is developed in which the active material is dispersed in an amorphous matrix. Li2S–Li2O–LiI exhibits high charge–discharge capacities and a high specific capacity of 998 mAh g−1 at a 2 C rate and 25 °C. X-ray photoelectron spectroscopy, X-ray diffractometry, and transmission electron microscopy observation suggest that Li2O–LiI provides nanoscale ion-conduction pathways during cycling that activate Li2S and deliver large capacities; it also exhibits an appropriate onset oxidation voltage for high capacity. Furthermore, a cell with a high areal capacity of 10.6 mAh cm–2 is demonstrated to successfully operate at 25 °C using a Li2S–Li2O–LiI positive electrode. This study represents a major step toward the commercialization of all-solid-state Li/S batteries.

    DOI: 10.1002/smll.202302179

    PubMed

  • Vacancy-Stabilized Superionic State in Na<inf>3- x</inf>Sb<inf>1- x</inf>W<inf>x</inf>S<inf>4</inf>

    Shin Ichi Nishimura, Akitoshi Hayashi, Atsushi Sakuda, Atsuo Yamada

    ACS Applied Energy Materials   5 ( 11 )   14053 - 14058   2022.11

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    The discovery of numerous superionic conductors has accelerated the development of solid-state energy storage systems. Among all alkaline ionic conductors known thus far, Na3-xSb1-xWxS4 exhibits the highest ionic conductivity of >30 mS cm-1 at ambient temperature, even surpassing the conductivity of the best lithium superionic conductor. The origin of the peculiar high Na+ diffusivity was investigated by the in-depth crystallographic analysis of Na3-xSb1-xWxS4 through combined X-ray diffraction and molecular dynamics simulations, emphasizing the accurate three-dimensional disordered nature of sodium in the crystalline matrix. The important features induced by the aliovalent tungsten substitution were (i) tetragonal to cubic transformation, (ii) the creation of sodium vacancies that are evenly distributed throughout the crystal without the local condensation around W, and (iii) the effective formation of sodium positional disordering by sodium vacancy. These features inherent to the best alkaline-ion conducting phase reported thus far would provide invaluable insights toward the further development of superionic conductors.

    DOI: 10.1021/acsaem.2c02627

  • Li<inf>2</inf>S-V<inf>2</inf>S<inf>3</inf>-LiI Bifunctional Material as the Positive Electrode in the All-Solid-State Li/S Battery

    Tatsuki Shigedomi, Yushi Fujita, Takuma Kishi, Kota Motohashi, Hirofumi Tsukasaki, Hiroshi Nakajima, Shigeo Mori, Masahiro Tatsumisago, Atsushi Sakuda, Akitoshi Hayashi

    Chemistry of Materials   34 ( 21 )   9745 - 9752   2022.11( ISSN:0897-4756

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    All-solid-state batteries with sulfur-based positive electrode active materials have been attracting global attention, owing to their safety and long cycle life. Li2S and S are promising positive electrode active materials for high energy density in these batteries because of high theoretical capacities. All-solid-state batteries with these active materials generally require the addition of solid electrolytes (SEs) and conductive carbons to the positive electrode layer to form ionic and electronic conducting pathways due to their insulating nature. In this study, we developed electrode-electrolyte bifunctional materials in the system Li2S-V2S3-LiI with high ionic and electronic conductivity. All-solid-state batteries with Li2S-V2S3-LiI in the positive electrode layer work without SEs and conductive carbons. In particular, an all-solid-state battery with 90(0.75Li2S·0.25V2S3)·10LiI (mol %) showed a high capacity of 370 mA h g-1at 25 °C and retained 83% of the initial discharge capacity even after 100 cycles. 90(0.75Li2S·0.25V2S3)·10LiI were composed of LiVS2and Li2S-LiI nanoparticles embedded in the amorphous matrix. Both LiVS2and Li2S-LiI solid solution showed electrode activity, which contribute to the high reversible capacity. Our findings offer new solutions for increasing the energy density of all-solid-state batteries.

    DOI: 10.1021/acs.chemmater.2c02645

  • Vacancy-Stabilized Superionic State in Na3-xSb1-xWxS4 Reviewed

    S.-I. Nishimura, A. Hayashi, A. Sakuda and A. Yamada

    ACS Appl. Energy Mater.   5 ( 11 )   14053 - 14058   2022.11

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    Kind of work:Joint Work  

    DOI: https://doi.org/10.1021/acsaem.2c02627

  • 電極電位測定の基礎と実際~水系・非水系・固体系~(その2)

    松本 一彦, 宮崎 晃平, 黄 珍光, 山本 貴之, 作田 敦

    関西電気化学テキストシリーズ   2022.2 ( 0 )   23 - 42   2022.10

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  • 電極電位測定の基礎と実際~水系・非水系・固体系~(その1)

    松本 一彦, 宮崎 晃平, 黄 珍光, 山本 貴之, 作田 敦

    関西電気化学テキストシリーズ   2022.2 ( 0 )   1 - 22   2022.10

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  • Electrode Potentials Part 1: Fundamentals and Aqueous Systems

    MATSUMOTO Kazuhiko, MIYAZAKI Kohei, HWANG Jinkwang, YAMAMOTO Takayuki, SAKUDA Atsushi

    Electrochemistry   90 ( 10 )   102001 - 102001   2022.10( ISSN:13443542

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    <p>Electrochemistry deals with the interrelationship between electrical and chemical energy. Various potentials appear in electrochemistry and pertain to one another in practical cells. Understanding the electrode potential is an important step in acquiring basic knowledge of electrochemistry and extending it to specific applications. This comprehensive paper outlines the fundamentals and related subjects of electrode potentials, including electrochemical cells and liquid junction potentials. Aqueous solution systems are ideal for connecting the theoretical background of electrode potentials to practical electrochemical measurements. Accordingly, the basic electrode chemistry in aqueous systems is described in this paper, as well as several advanced concepts introduced in recent studies.</p>

    DOI: 10.5796/electrochemistry.22-66075

  • Electrode Potentials Part 2: Nonaqueous and Solid-State Systems

    HWANG Jinkwang, YAMAMOTO Takayuki, SAKUDA Atsushi, MATSUMOTO Kazuhiko, MIYAZAKI Kohei

    Electrochemistry   90 ( 10 )   102002 - 102002   2022.10( ISSN:13443542

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    <p>This comprehensive paper, Electrode Potentials Part 2, is a continuation of Electrode Potentials Part 1: Fundamentals and Aqueous Systems. Determining the electrode potential is crucial for understanding the nature of the electrochemical properties of materials or systems; however, an accurate evaluation of the potential of a target electrode has always been a challenge. The electrode potential can be used to predict the reaction mechanisms in electrochemistry and can be directly applied to the study of electrochemical applications. This paper introduces the methodologies and strategies for measuring electrode potentials in nonaqueous and solid-state electrolytes, including organic solvent electrolytes, ionic liquid electrolytes, and oxide and sulfide solid electrolytes. Experimental details are described for basic to state-of-the-art strategies, focusing on practical methods and know-how.</p>

    DOI: 10.5796/electrochemistry.22-66088

  • Ionic Conductivity and Microstructure of Li<sub>4</sub>GeO<sub>4</sub>-Based Solid Electrolytes

    Ding Jiong, Tsukasaki Hirofumi, Nakajima Hiroshi, Yoneda Yohei, Kimura Takuya, Sakuda Atsushi, Hayashi Akitoshi, Mori Shigeo

    MATERIALS TRANSACTIONS   63 ( 10 )   1390 - 1395   2022.10( ISSN:13459678

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    Publishing type:Research paper (scientific journal)  

    <p>Li<sub>4</sub>GeO<sub>4</sub>-based solid electrolytes can be synthesized at low temperatures, and their formability is improved by adding Li<sub>2</sub>SO<sub>4</sub>. Glass–ceramic Li<sub>4</sub>GeO<sub>4</sub> exhibits a relatively high ionic conductivity of approximately 10<sup>−6</sup> S cm<sup>−1</sup> at room temperature, which is higher than that of glass Li<sub>4</sub>GeO<sub>4</sub>. Thus, Li<sub>4</sub>GeO<sub>4</sub> has promising applications in all-solid-state lithium ion batteries. To understand the correlation between the ionic conductivity, formability, and microstructure of the synthesized materials, the microstructures and crystallization process of glass and glass–ceramic Li<sub>4</sub>GeO<sub>4</sub> and 80Li<sub>4</sub>GeO<sub>4</sub>·20Li<sub>2</sub>SO<sub>4</sub> (Li<sub>3.6</sub>Ge<sub>0.8</sub>S<sub>0.2</sub>O<sub>4</sub>) were observed by transmission electron microscopy (TEM). Since Li<sub>3.6</sub>Ge<sub>0.8</sub>S<sub>0.2</sub>O<sub>4</sub> glass exhibits a halo diffraction pattern, the addition of Li<sub>2</sub>SO<sub>4</sub> to Li<sub>4</sub>GeO<sub>4</sub> stabilizes its amorphous phase. In addition, glass–ceramic samples were found to be characterized by an amorphous state containing nanocrystallites with a crystallinity degree of approximately 40%, which improves the ionic conductivity of the material.</p>

    DOI: 10.2320/matertrans.mt-m2022094

  • Ionic Conductivity and Microstructure of Li4GeO4-Based Solid Electrolytes Reviewed

    J. Ding, H. Tsukasaki, H. Nakajima, Y. Yoneda, T. Kimura, A. Sakuda, A. Hayashi and S. Mori

    Mater. Trans.   63 ( 10 )   1390 - 1395   2022.10

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    Kind of work:Joint Work  

    DOI: https://doi.org/10.2320/matertrans.MT-M2022094

  • Li2S-V2S3--LiI Bifunctional Material as the Positive Electrode in the All-Solid-State Li/S Battery Reviewed

    T. Shigedomi, Y. Fujita, T. Kishi, K. Motohashi, H. Tsukasaki, H. Nakajima, S. Mori, M. Tatsumisago, A. Sakuda and A. Hayashi

    Chem. Mater.   34 ( 21 )   9745 - 9752   2022.10

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    Kind of work:Joint Work  

    DOI: https://doi.org/10.1021/acs.chemmater.2c02645

  • Electrode Potentials Part 1: Fundamentals and Aqueous Systems Reviewed

    K. Matsumoto, K. Miyazaki, J. Hwang, T. Yamamoto and A. Sakuda

    Electrochemistry   90 ( 10(102001) )   1 - 9   2022.10

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    Kind of work:Joint Work  

    DOI: https://doi.org/10.5796/electrochemistry.22-66075

  • Electrode Potentials Part2: Nonaqueous and Solid-State Systems Reviewed

    J. Hwang, T. Yamamoto, A. Sakuda, K. Matsumoto and K. Miyazaki

    Electrochemistry   90 ( 10(102002) )   1 - 8   2022.10

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    Kind of work:Joint Work  

    DOI: https://doi.org/10.5796/electrochemistry.22-66088

  • Thermally stable bulk-type all-solid-state capacitor with a highly deformable oxide solid electrolyte

    Takashi Hakari, Shunsuke Yoshimi, Kenji Nagao, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    Journal of Power Sources   543   2022.09( ISSN:0378-7753

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    Publishing type:Research paper (scientific journal)  

    The development of all-solid-state capacitors (ASSCs) based on inorganic solid electrolytes (SEs) with high thermal stability is desired. However, because of their high cell resistance, such capacitors have lower capacitances and rate capabilities than conventional electric double-layer capacitors (EDLCs) that use aqueous solutions and organic liquid electrolytes. The high resistance is caused by the mechanical and electrochemical properties of the SE. In this study, a highly deformable Li-ion conducting oxide SE was investigated to improve the electrochemical performance of ASSCs. Bulk-type symmetric ASSCs, with a 33Li3BO3·33Li2SO4·33Li2CO3 (LBSC) SE layer between two electrode layers of an LBSC-CNT composite, showed low resistance and were operable at 100–300 °C. Additionally, the highest capacitance at the highest current reported for ASSCs till date was achieved. The highly deformable SE will facilitate the design of ASSCs and expand the potential range of applications of EDLCs.

    DOI: 10.1016/j.jpowsour.2022.231821

  • Mechanochemical synthesis of Na<sub>3</sub>NbS<sub>4</sub> metastable phase as positive electrode materials for all-solid-state sodium batteries

    Nasu Akira, Sakuda Atsushi, Tatsumisago Masahiro, Hayashi Akitoshi

    Journal of the Ceramic Society of Japan   130 ( 9 )   789 - 793   2022.09( ISSN:18820743

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    <p>Transition metal sulfides have been reported to be active materials with high capacities by using anionic redox reactions. Modifying the structure to favor the extraction/insertion of sodium is beneficial in achieving the theoretical capacity of these sulfides. In this study, we synthesized three new phases of Na<sub>3</sub>NbS<sub>4</sub> via a mechanochemical (MC) process. Under moderate MC conditions, amorphous Na<sub>3</sub>NbS<sub>4</sub> was obtained. Under harsher MC conditions, metastable phases I and II of Na<sub>3</sub>NbS<sub>4</sub> were obtained at different process times of 10 and 40 h, respectively. The conductivities of the three Na<sub>3</sub>NbS<sub>4</sub> materials were higher than that of orthorhombic Na<sub>3</sub>NbS<sub>4</sub>. In particular, the metastable phase I of Na<sub>3</sub>NbS<sub>4</sub> showed the highest conductivity of 3.2 × 10<sup>−6</sup> S cm<sup>−1</sup>, and the all-solid-state sodium cells with metastable phase I as an electrode active material showed the highest capacity of 240 mAh g<sup>−1</sup>. Thus, the MC process is useful for synthesizing positive electrode active materials on transition metal sulfides with an advantageous structure to achieve a high capacity.</p>

    DOI: 10.2109/jcersj2.22056

  • Iron Sulfide Na2FeS2 as Positive Electrode Material with High Capacity and Reversibility Derived from Anion-Cation Redox in All-Solid-State Sodium Batteries Reviewed

    A. Nasu, A. Sakuda, T. Kimura, M. Deguchi, A. Tsuchimoto, M. Okubo, A. Yamada, M. Tatsumisago and A. Hayashi

    Small   18 ( 42 )   2203383   2022.09

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    DOI: https://doi.org/10.1002/smll.202203383

  • Mechanochemical Synthesis of Na3NbS4 Metastable Phase as Positive Electrode Materials for All-Solid-State Sodium Batteries Reviewed

    A. Nasu, A. Sakuda, M. Tatsumisago and A. Hayashi

    J. Ceram. Soc. Jpn.   130 ( 9 )   789 - 793   2022.09

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    DOI: https://doi.org/10.2109/jcersj2.22056

  • Li<inf>2</inf>S-LiI Solid Solutions with Ionic Conductive Domains for Enhanced All-Solid-State Li/S Batteries

    Yushi Fujita, Takashi Hakari, Atsushi Sakuda, Minako Deguchi, Yusuke Kawasaki, Hirofumi Tsukasaki, Shigeo Mori, Masahiro Tatsumisago, Akitoshi Hayashi

    ACS Applied Energy Materials   5 ( 8 )   9429 - 9436   2022.08

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    Publishing type:Research paper (scientific journal)  

    Lithium sulfur (Li/S) batteries are promising next-generation battery candidates owing to their high energy densities. In particular, the fast solid-state S/Li2S redox reactions are crucial to increase the energy density and extend the cycle life of such batteries. However, the poor electronic and ionic conductivities of S and Li2S result in a low reversible capacity. Therefore, an electrode design is required to achieve high-energy-density Li/S batteries. In this study, we investigated the charge-discharge mechanism of a solid solution of Li2S and LiI (Li2S-LiI) in all-solid-state batteries showing excellent electrochemical properties, including cycling performance. We found that a high reversible capacity was achieved despite the high conversion of Li2S into S because the ionic conductivity of the positive electrode was maintained during charging and discharging, and this was a result of the formation of an ionic conductive structure comprising LiI-rich domains. Crucially, essentially fully solid phase S/Li2S reactions in all-solid-state batteries were attained by fully eliminating the sulfide solid electrolyte from the positive electrode. These findings enable the design of S- and Li2S-based positive electrodes for solid phase redox reactions for use in high-energy-density Li/S batteries.

    DOI: 10.1021/acsaem.2c00978

  • Amorphous Positive Electrode Materials Prepared Using LiMn<sub>1.5</sub>Ni<sub>0.5</sub>O<sub>4</sub> and Lithium Oxyacid Salts

    Kwon Neung, Nasu Akira, Sakuda Atsushi, Tatsumisago Masahiro, Hayashi Akitoshi

    Chemistry Letters   51 ( 8 )   815 - 818   2022.08( ISSN:03667022

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    <p>LiNi<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> is an attractive choice for a high-voltage positive electrode material for all-solid-state batteries. However, its use in all-solid-state batteries is challenging because of low ionic conductivity. In this study, we synthesized new amorphous electrode materials from LiMn<sub>1.5</sub>Ni<sub>0.5</sub>O<sub>4</sub> and lithium oxyacid salts. The synthesized amorphous electrodes exhibited higher ionic conductivity and capacity than a LiMn<sub>1.5</sub>Ni<sub>0.5</sub>O<sub>4</sub> crystal in both liquid- and solid-type cells. Among these electrodes, amorphous 80LiMn<sub>1.5</sub>Ni<sub>0.5</sub>O<sub>4</sub>·20Li<sub>3</sub>PO<sub>4</sub> (mol %) demonstrated a high reversible capacity of 220 mAh g<sup>−1</sup> in a liquid-type cell.</p>

    DOI: 10.1246/cl.220132

  • Ionic conduction of glasses and their potential applications

    Daiko Yusuke, Sakuda Atsushi, Honma Tsuyoshi, Hayashi Akitoshi

    Journal of the Ceramic Society of Japan   130 ( 8 )   552 - 557   2022.08( ISSN:18820743

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    <p>Materials with high ionic conductivity are attracting a great deal of attention because they are indispensable for improving the performance of batteries, sensors, and capacitors. Solid electrolytes, in particular, have a potential to compensate for the shortcomings of liquid electrolytes, and are the subject of intense research and development worldwide. One of the big characteristics of glass is its high formability. Here we are focusing on glass-electrolytes. Differences between “superionic conductive glasses” and “ordinary glasses”, as well as the mixed alkali effect will be overviewed. In addition, glasses can retain large residual stress inside that can reach the order of several GPa depending on the cooling conditions. These residual stresses also affect ionic conductivity. Recent results on the application of glass formability and softening fluidity to the formation of interfaces in all-solid-state batteries, and to ion emission from sharpened glasses are reviewed.</p>

    DOI: 10.2109/jcersj2.22035

  • Amorphous Positive Electrode Materials Prepared Using LiMn1.5Ni0.5O4 and Lithium Oxyacid Salts Reviewed

    N. Kwon, A. Nasu, A. Sakuda, M. Tatsumisago and A. Hayashi

    ACS Appl. Mater. Interfaces   14 ( 21 )   24480 - 24485   2022.08

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    DOI: https://doi.org/10.1246/cl.220132

  • Ionic Conduction of Glasses and their Potential Applications Reviewed

    Y. Daiko, A. Sakuda, T. Honma and A. Hayashi

    J. Ceram. Soc. Jpn.   130 ( 8 )   552 - 557   2022.08

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    DOI: https://doi.org/10.2109/jcersj2.22035

  • Li2S-LiI Solid Solutions with Ionic Conductive Domains for Enhanced All-Solid-State Li/S Batteries Reviewed

    Y. Fujita, T. Hakari, A. Sakuda, M. Deguchi, Y. Kawasaki, H. Tsukasaki, S. Mori, M. Tatsumisago and A. Hayashi

    ACS Appl. Energy Mater.   5 ( 8 )   9429 - 9436   2022.08

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    DOI: https://doi.org/10.1021/acsaem.2c00978

  • Preparation and Characterization of Na2.88Sb0.88W0.12S4-xOx Solid Electrolyte Reviewed

    T. Takayanagi, A. Nasu, F. Tsuji, K. Motohashi, A. Sakuda, M. Tatsumisago and A. Hayashi

    Electrochemistry,   90 ( 6(067009) )   1 - 5   2022.07

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    DOI: https://doi.org/10.2109/jcersj2.22017

  • Room-Temperature Preparation of All-Solid-State Lithium Batteries Using TiO<inf>2</inf>Anodes and Oxide Electrolytes

    Hiroyuki Usui, Yasuhiro Domi, Shin Ichiro Izaki, Akira Nasu, Atsushi Sakuda, Akitoshi Hayashi, Hiroki Sakaguchi

    Journal of Physical Chemistry C   126 ( 25 )   10320 - 10326   2022.06( ISSN:1932-7447

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    We tried to prepare solid-state batteries consisting of TiO2anodes and a Li3BO3-Li2SO4-Li2CO3solid electrolyte only by room-temperature pressing without any sintering process. The solid-state batteries successfully operated at 90 °C and showed reversible capacity in the range of 278-331 mA h g-1in the first cycles at 0.01C. In addition to this, the rate capability was remarkably improved by the doping of Nb or Ta into TiO2: the doped TiO2electrodes exhibited a capacity of 140 mA h g-1at 0.1C, whereas the undoped TiO2showed only 10 mA h g-1. The charge-transfer resistance of TiO2was reduced by the doping of Nb or Ta. The improvement in the anode performance was attributed to the improved electronic conductivity and the expanded interlayer distance by doping. These results demonstrated for the first time that the oxide anodes can operate in bulk-type oxide-based solid-state batteries prepared only by room-temperature pressing.

    DOI: 10.1021/acs.jpcc.2c02497

  • Formation of Passivate Interphases by Na<inf>3</inf>BS<inf>3</inf>-Glass Solid Electrolytes in All-Solid-State Sodium-Metal Batteries

    Akira Nasu, Takeaki Inaoka, Fumika Tsuji, Kota Motohashi, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    ACS Applied Materials and Interfaces   14 ( 21 )   24480 - 24485   2022.06( ISSN:1944-8244

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    Interphase formation at the interface between a solid electrolyte and negative electrode is one of the main factors limiting the practical use of all-solid-state sodium batteries. Sulfide-type solid electrolytes with group 15 elements (P and Sb) exhibit high ductility and ionic conductivity, comparable to those of organic liquid electrolytes. However, the electronically conductive interphase formed at the interface between Na3PS4and sodium metal increases the cell resistance and deteriorates its electrochemical properties. Contrarily, Na3BS3, containing boron as an electrochemically inert element, forms an electronically insulating thin passivate interphase, facilitating reversible sodium plating and stripping. Sodium-metal symmetric cells with Na3BS3exhibit steady operation over 1000 cycles. Thus, reduction-stable solid electrolytes can be developed by substitution with an electrochemically inert element versus sodium.

    DOI: 10.1021/acsami.2c05090

    PubMed

  • Na<inf>2</inf>S–NaI solid solution as positive electrode in all-solid-state Na/S batteries

    Yushi Fujita, Akira Nasu, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    Journal of Power Sources   532   2022.06( ISSN:0378-7753

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    All-solid-state sodium-sulfur (Na/S) batteries are promising next-generation batteries with high safety and high energy density. Sodium sulfide (Na2S) has application as active material in positive electrodes owing to its advantages such as low cost, low toxicity, and a large theoretical capacity. However, the electronic and sodium ion conductivities of Na2S are significantly low, and ascertaining the entire contribution of the active materials to cell capacities is challenging. Therefore, facilitating an electronic and ionic conduction path in the positive electrode is essential. In this study, Na2S was mixed with sodium iodide (NaI) via a mechanochemical process and was used as an active material in an all-solid-state Na/S battery. Consequently, a Na2S–NaI solid solution was formed, and the ionic conductivity of Na2S–NaI increased by five orders of magnitude compared to that of Na2S. Na2S–NaI showed large charge–discharge capacities and cycle capability. In particular, 90Na2S·10NaI showed a large capacity and high cycle efficiency, and 94% of Na2S acted as an active material. The result of this study leads to the development of all-solid-state Na/S batteries with high capacities, high rates, and high cycles.

    DOI: 10.1016/j.jpowsour.2022.231313

  • Lithium-Ion Conductivity and Crystallization Temperature of Multicomponent Oxide Glass Electrolytes Reviewed

    K. Nagao, M. Shigeno, A. Inoue, M. Deguchi, H. Kowada, C. Hotehama, A. Sakuda, M. Tatsumisago and A. Hayashi

    Adv. Funct. Mater.   32 ( 5(2106174) )   1 - 13   2022.06

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    DOI: https://doi.org/10.1016/j.nocx.2022.100089

  • Na2S-NaI Solid Solution as Positive Electrode in All-Solid-State Na/S Batteries Reviewed

    Y. Fujita, A. Nasu, A. Sakuda, M. Tatsumisago and A. Hayashi

    J. Non-Cryst. Solids: X   14 ( (100089) )   1 - 8   2022.06

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    DOI: https://doi.org/10.1016/j.jpowsour.2022.231313

  • Sodium-Ion Conducting Solid Electrolytes in the Na2S-In2S3 System Reviewed

    K. Motohashi, A. Nasu, T. Kimura, C. Hotehama, A. Sakuda, M. Tatsumisago and A. Hayashi

    Chem. Lett.   51 ( 8 )   815 - 818   2022.06

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    DOI: https://doi.org/10.5796/electrochemistry.22-00037

  • Room-Temperature Preparation of All-Solid-State Lithium Batteries Using TiO2 Anodes and Oxide Electrolytes Reviewed

    H. Usui, Y. Domi, S. Izaki, A. Nasu, A. Sakuda, A. Hayashi and H. Sakaguchi

    J. Phys. Chem. C   126 ( 25 )   10320 - 10326   2022.06

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    DOI: https://doi.org/10.1021/acs.jpcc.2c02497

  • Lithium-ion conductivity and crystallization temperature of multicomponent oxide glass electrolytes

    Kenji Nagao, Manari Shigeno, Ayane Inoue, Minako Deguchi, Hiroe Kowada, Chie Hotehama, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    Journal of Non-Crystalline Solids: X   14   2022.06

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    Lithium-ion-conducting oxide glass electrolytes in the multicomponent systems Li2O–B2O3–SiO2–P2O5-LiX (LiX = Li3N, Li2SO4, Li2CO3, and LiI) were synthesized using a mechanochemical technique. The crystallization temperature and ionic conductivity of multicomponent glasses with added lithium salts or Li3N were evaluated. Because the crystallization temperature is a measure of the ability of glasses to resist crystallization at high temperature, glasses with high conductivity and high crystallization temperature are desirable electrolytes. In this study, the lithium-ion conductivity of the glasses was found to be correlated with the crystallization temperature, and it was difficult to increase both the conductivity and crystallization temperature. The addition of lithium salts (Li2SO4, Li2CO3, and LiI) increased the conductivity but decreased the crystallization temperature. Nitrogen doping by the addition of Li3N improved both these properties of the oxide glass electrolyte. Therefore, oxynitride glasses are desirable electrolytes owing to their thermal stability and lithium-ion conductivity.

    DOI: 10.1016/j.nocx.2022.100089

  • Characterizing the Structural Change of Na<inf>3</inf>PS<inf>4</inf>Solid Electrolytes in a Humid N<inf>2</inf>Atmosphere

    Takumi Nakano, Takuya Kimura, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    Journal of Physical Chemistry C   126 ( 17 )   7383 - 7389   2022.05( ISSN:1932-7447

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    Publishing type:Research paper (scientific journal)  

    Sulfide solid electrolytes (SSEs) show a higher ionic conductivity than oxide solid electrolytes. However, SSEs generally exhibit a moisture-sensitive nature. This study focused on the degradation mechanisms of SSEs in a humid N2atmosphere, and Na3PS4(NPS) was selected as the SSE. The structural changes during exposure to humidified N2were monitored using a system comprising an X-ray diffractometer, a humidity regulator, and an H2S sensor. Structural evaluations revealed that the exposed NPS was a hydrate, and it was recovered to the NPS crystal phase by the removal of adsorbed/hydrated water molecules using regenerating treatments, such as heating at 200 °C or drying under reduced pressure with/without heating. The regenerated NPS showed an ionic conductivity of 5.3 × 10-5S cm-1at 25 °C, which is 40 times that of the exposed NPS. These results suggest that exposed NPS can be structurally and conductively regenerated to the NPS crystal phase using regeneration treatments.

    DOI: 10.1021/acs.jpcc.2c00421

  • Crystalline Precursor Derived from Li3PS4 and Ethylenediamine for Ionic Conductors Reviewed

    T. Kimura, A. Ito, T. Nakano, C. Hotehama, H. Kowada, A. Sakuda, M. Tatsumisago and A. Hayashi

    Electrochemistry   90 ( 4(047005) )   1 - 5   2022.05

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    DOI: https://doi.org/10.1007/s10971-022-05824-x

  • Formation of Passivate Interphases by Na3BS3-Glass Solid Electrolytes in All-Solid-State Sodium-Metal Batteries Reviewed

    A. Nasu, T. Inaoka, F. Tsuji, K. Motohashi, A. Sakuda, M. Tatsumisago and A. Hayashi

    J. Sol-Gel. Sci. Technol.   104 ( 3 )   627 - 634   2022.05

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    DOI: https://doi.org/10.1021/acsami.2c05090

  • Mechanochemical Synthesis of Amorphous MoSx (x=3,4,5,6, and 7) Electrode for All-Solid-State Sodium Battery Reviewed

    G. Shirota, A. Nasu, M. Deguchi, A. Sakuda, M. Tatsumisago and A. Hayashi

    Electrochemistry   90 ( 3(037012) )   1 - 4   2022.04

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    DOI: https://doi.org/10.2109/jcersj2.21177

  • Characterizing the Structural Change of Na3PS4 Solid Electrolytes in a Humid N2 Atmosphere Reviewed

    T. Nakano, T. Kimura, A. Sakuda, M. Tatsumisago and A. Hayashi

    J. Ceram. Soc. Jpn.   130 ( 4 )   308 - 312   2022.04

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    DOI: https://doi.org/10.1021/acs.jpcc.2c00421

  • Mechanochemically Prepared Highly Conductive Na2.88Sb0.88W0.12S4-NaI Composite Electrolytes for All-Solid-State Sodium Battery Reviewed

    T. Takayanagi, A. Nasu, F. Tsuji, A. Sakuda, M. Tatsumisago and A. Hayashi

    J. Phys. Chem. C   126 ( 17 )   7383 - 7389   2022.04

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    DOI: https://doi.org/10.5796/electrochemistry.22-00016

  • Studies on the Inhibition of Lithium Dendrite Formation in Sulfide Solid Electrolytes Doped with LiX(X=Br,I) Reviewed

    S.H. Yang, M. Takahashi, K. Yamamoto, K. Ohara, T. Watanabe, T. Uchiyama, T. Takami, A. Sakuda, A. Hayashi, M. Tatsumisago and Y. Uchimoto

    Solid State Ionics   377 ( (115869) )   1 - 7   2022.04

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    DOI: https://doi.org/10.1016/j.ssi.2022.115869

  • Mechanochemical synthesis of amorphous MoSx (x = 3, 4, 5, 6, and 7) electrode for all-solid-state sodium battery

    Gaku Shirota, Akira Nasu, Minako Deguchi, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    Journal of the Ceramic Society of Japan   130 ( 4 )   308 - 312   2022.04( ISSN:1882-0743

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    Publishing type:Research paper (scientific journal)  

    All-solid-state sodium secondary batteries have garnered significant attention as next-generation batteries with high safety. To realize an all-solid-state sodium secondary battery with a high energy density, it is necessary to develop a high-capacity electrode active material. In this study, we prepared amorphous molybdenum polysulfide (a-MoSx, x = 37) using a mechanochemical process as electrode active material in all-solid-state cells using Na3PS4 sulfide electrolyte. In all-solid-state cells, a-MoS3, a-MoS4, a-MoS5, a-MoS6, and a-MoS7 showed high reversible capacities of 260, 330, 470, 540, and 510mAhg 1, respectively. X-ray photoelectron spectroscopy analyses suggested that the dischargecharge reaction in a-MoSx proceeds mainly by anion redox with dissociation and formation of disulfide bonds. Amorphous sulfur-rich MoSx is thus a promising electrode active material with high capacity in all-solid-state sodium batteries.

    DOI: 10.2109/jcersj2.21177

  • Studies on the inhibition of lithium dendrite formation in sulfide solid electrolytes doped with LiX (X = Br, I)

    Seunghoon Yang, Masakuni Takahashi, Kentaro Yamamoto, Koji Ohara, Toshiki Watanabe, Tomoki Uchiyama, Tsuyoshi Takami, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago, Yoshiharu Uchimoto

    Solid State Ionics   377   115869 - 115869   2022.04( ISSN:0167-2738

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    A promising method to increase the energy density of all-solid-state batteries (ASSBs) featuring lithium ions as carriers is to employ Li metal as the anode. However, this has been accompanied by safety problems like flammable accidents associated with lithium dendrites originating from reactions with the solid electrolyte, leading to reduced battery performance. To overcome this issue toward the commercialization of ASSBs, various approaches have been proposed by many researchers. Among the suggested solutions, the use of lithium-halide-doped Li3PS4, to suppress lithium dendrite formation, has attracted attention. LiI-doped Li3PS4 has shown the highest lithium dendrite growth suppression among lithium-halide-doped systems, but the reason for this is unclear. Thus, we attempted to clarify the cause of this suppression by comparing LiBr-doped Li3PS4 with LiI-doped Li3PS4. Investigation using various methods such as electrochemical evaluation, X-ray absorption spectroscopy, X-ray computed tomography, and pair distribution function analysis revealed that two factors affect the suppression of Li dendrite growth: the suppression of the current density distribution by improving the ionic conductivity and the stable interfacial layer. This is the main reason LiI-doped Li3PS4 shows excellent Li dendrite suppression.

    DOI: 10.1016/j.ssi.2022.115869

  • Molybdenum Polysulfide Electrode with High Capacity for All-Solid-State Sodium Battery Reviewed

    G. Shirota, A. Nasu, M. Deguchi, A. Sakuda, M. Tatsumisago and A. Hayashi

    Solid State Ionics   376 ( (115848) )   1 - 7   2022.03

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    DOI: https://doi.org/10.1016/j.ssi.2021.115848

  • Mechanochemical Synthesis of Pyrite Ni1-xFexS2 Electrode for All-Solid-State Sodium Battery Reviewed

    G. Shirota, A. Nasu, A. Sakuda, M. Deguchi, K. Motohashi, M. Tatsumisago and A. Hayashi

    J. Power Sources   532 ( (231313) )   1 - 6   2022.03

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    DOI: https://doi.org/10.5796/electrochemistry.22-00007

  • AC Impedance Analysis of the Degeneration and Recovery of Argyrodite Sulfide-Based Solid Electrolytes under Dry-Room-Simulated Condition Reviewed

    H. Sano, Y. Morino, A. Yabuki, S. Sato, N. Itayama, Y. Matsumura, M. Iwasaki, M. Takehara, T. Abe, Y. Ishiguro, T. Takahashi, N. Miyashita, A. Sakuda and A. Hayashi

    Electrochemistry   90 ( 3(037011) )   1 - 6   2022.03

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    DOI: https://doi.org/10.5796/electrochemistry.22-00013

  • Molybdenum polysulfide electrode with high capacity for all-solid-state sodium battery

    Gaku Shirota, Akira Nasu, Minako Deguchi, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    Solid State Ionics   376   2022.03( ISSN:0167-2738

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    Publishing type:Research paper (scientific journal)  

    All-solid-state sodium secondary batteries have attracted significant attention as an alternative for post‑lithium-ion batteries. However, to obtain all-solid-state sodium secondary batteries with high-energy density, it is necessary to develop a high-capacity positive electrode material. In this study, two types of amorphous (a-)MoSx (x ≃ 6) active electrode materials were prepared using a mechanochemical (MC) process and through the thermal decomposition (TD) of (NH4)2Mo2S12·2H2O. Herein, X-ray diffraction (XRD), thermogravimetric analysis (TGA), and X-ray photoelectron spectroscopy (XPS) analyses were conducted, and the results revealed significantly different local structures of a-MoSx (MC) and a-MoSx (TD). The all-solid-state sodium cells with a-MoSx (MC) and a-MoSx (TD) possessed high reversible capacities of 510 and 690 mAh g−1, as well as high-capacity retention rates of 80% and 92% for the 2nd to 30th cycles, respectively. XPS analysis of the discharge–charge products further suggested that dissociation and formation of disulfide bonds occurred reversibly during the discharge–charge reaction. This study shows that a-MoSx (MC) and a-MoSx (TD) are promising active electrode materials for all-solid-state sodium batteries.

    DOI: 10.1016/j.ssi.2021.115848

  • Characteristics of a Li<inf>3</inf>BS<inf>3</inf> Thioborate Glass Electrolyte Obtained via a Mechanochemical Process

    Takuya Kimura, Ayane Inoue, Kenji Nagao, Takeaki Inaoka, Hiroe Kowada, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    ACS Applied Energy Materials   5 ( 2 )   1421 - 1426   2022.02

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    To improve the ionic conductivity of solid electrolytes, it is generally thought that anions with high polarizability should be used. However, the relationship between polarization and conductivity is not clear because conductivity largely depends on the crystal structure. In this study, we focus on amorphous materials with no long-range ordered structure. The conductivity and ductility properties of lithium boron oxide (Li3BO3), lithium boron nitride (Li3BN2), and lithium boron sulfide (Li3BS3) are compared. Li3BS3 glass is prepared from Li2S, B, and S using heat treatment and a mechanochemical process. It has high ductility and a higher ionic conductivity (3.6 × 10-4 S cm-1 at 25 °C) than that of Li3BO3 and Li3BN2 glass with a low activation energy of 32 kJ mol-1. Li3BS3 glass is therefore suitable as an ionic conductor with high conductivity. The electronegativity of anions and glass properties such as ionic conductivity and ductility are correlated, and it is proposed that this relationship can be used as a basis for investigating fast ionic conductors.

    DOI: 10.1021/acsaem.1c02452

  • Synthesis of an AlI3-doped Li2S positive electrode with superior performance in all-solid-state batteries

    Hirotada Gamo, Takaki Maeda, Kazuhiro Hikima, Minako Deguchi, Yushi Fujita, Yusuke Kawasaki, Atsushi Sakuda, Hiroyuki Muto, Nguyen Huu Huy Phuc, Akitoshi Hayashi, Masahiro Tatsumisago, Atsunori Matsuda

    Materials Advances   3 ( 5 )   2488 - 2494   2022.02

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    A (100 − <italic>x</italic>)Li<sub>2</sub>S·<italic>x</italic>AlI<sub>3</sub> (0 ≤ <italic>x</italic> ≤ 30) positive electrode was prepared by the planetary ball-milling method for application in all-solid-state Li–S batteries.

    DOI: 10.1039/d1ma01228b

  • Synthesis of an AlI3-doped Li2S Positive Electrode with Superior Performance in All-Solid-State Batteries Reviewed

    H. Gamo, T. Maeda, K. Hikima, M. Deguchi, Y. Fujita, Y. Kawasaki, A. Sakuda, H. Muto, N.H.H. Phuc, A. Hayashi, M. Tatsumisago and A. Matsuda

    Mater. Adv.   3 ( 5 )   2488 - 2494   2022.02

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    DOI: https://doi.org/10.1039/D1MA01228B

  • Solid Electrolyte with Oxidation Tolerance Provides a High-Capacity Li<inf>2</inf>S-Based Positive Electrode for All-Solid-State Li/S Batteries

    Takashi Hakari, Yushi Fujita, Minako Deguchi, Yusuke Kawasaki, Misae Otoyama, Yohei Yoneda, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    Advanced Functional Materials   32 ( 5 )   2022.01( ISSN:1616-301X

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    The electrochemical window of solid electrolytes (SEs) plays a crucial role in designing active material–SE interfaces in high-energy-density all-solid-state batteries (ASSBs). However, the suitable electrochemical window for individual active materials is not yet investigated, as the electrochemical window of SEs is overestimated. In this study, the oxidation onset voltages (OOVs) of several SEs, namely those compatible with Li2S as a high-capacity positive electrode material are determined. Results reveal that SEs with low OOVs decrease the capacity and increase the interfacial resistance of the corresponding ASSBs. The OOVs of SEs must exceed that of Li2S by more than 0.2 V to achieve high capacity, which in turn depends on SE ionic conductivity. Therefore, an Li2S positive electrode is combined with pseudobinary Li-oxyacid salts as SEs, exhibiting high OOVs and ionic conductivities, to afford a high-capacity (500 Wh kg−1) ASSB with high Li2S content.

    DOI: 10.1002/adfm.202106174

  • High Rate Capability from a Graphite Anode through Surface Modification with Lithium Iodide for All-Solid-State Batteries

    Seunghoon Yang, Kentaro Yamamoto, Xiaohan Mei, Atsushi Sakuda, Tomoki Uchiyama, Toshiki Watanabe, Tsuyoshi Takami, Akitoshi Hayashi, Masahiro Tatsumisago, Yoshiharu Uchimoto

    ACS Applied Energy Materials   5 ( 1 )   667 - 673   2022.01( ISSN:2574-0962

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    Publishing type:Research paper (scientific journal)  

    All-solid-state batteries (ASSBs) have been attracting attention as a potential paradigm for batteries in the future, as they are safer because they do not leak and are stable at high temperatures compared to lithium-ion batteries (LIBs) that use liquid electrolytes; further, the use of a bipolar structure is expected to improve energy density. For ASSBs, graphite is one of the most promising practical anode materials because of its superior power density in LIBs. However, the power density of ASSBs is unsatisfactory for practical applications and is lower than that of LIBs. One reason for this is the slow lithium ion transport at the interface between the graphite anode and solid electrolyte (SE). Because of the low redox potential for lithium ion intercalation into graphite (close to the lithium reduction potential), sulfide SEs undergo reductive decomposition, which impedes lithium ion transport at the interface with graphite. To address this problem, we attempted to coat LiI, which is stable at the lithium deposition potential, directly onto the graphite surface and examined the effect on the sulfide SE and electrochemical performance. The electrochemical measurements showed that the graphite composite without LiI showed a discharge capacity of 248 mA h g-1, while that with 5 wt % LiI showed a relatively high discharge capacity of approximately 348 mA h g-1. Impedance spectroscopy and S and P K-edge X-ray absorption spectroscopy indicated that the LiI-coated graphite composites displayed a stable interface behavior, in contrast to the uncoated graphite composite, after the lithiation process.

    DOI: 10.1021/acsaem.1c03166

  • Liquid-Phase Synthesis of Li3PS4 Solid Electrolyte Using Ethylenediamine Reviewed

    A. Ito, T. Kimura, A. Sakuda, M. Tatsumisago and A. Hayashi

    Solid State Ionics   377 ( (115869) )   1 - 7   2022.01

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    DOI: https://doi.org/10.1007/s10971-021-05524-y

  • High Rate Capability from a Graphite Anode through Surface Modification with Lithium Iodide for All-Solid-State Batteries Reviewed

    S.H. Yang, K. Yamamoto, X.H. Mei, A. Sakuda, T. Uchiyama, T. Watanabe, T. Takami, A. Hayashi, M. Tatsumisago and Y. Uchimoto

    J. Sol-Gel. Sci. Technol.   101 ( 1 )   2 - 7   2022.01

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    DOI: https://doi.org/10.1021/acsaem.1c03166

  • Solid Electrolyte with Oxidation Tolerance Provides a High-Capacity Li2S-Based Positive Electrode for All-Solid-State Li/S Batteries Reviewed

    T. Hakari, Y. Fujita, M. Deguchi, Y. Kawasaki, M. Otoyama, Y. Yoneda, A. Sakuda, M. Tatsumisago and A. Hayashi

    ACS Appl. Energy Mater.   5 ( 1 )   667 - 673   2022.01

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    Kind of work:Joint Work  

    DOI: https://doi.org/10.1002/adfm.202106174

  • Characteristics of a Li3BS3 Thioborate Glass Electrolyte Obtained via a Mechanochemical Process Reviewed

    T. Kimura, A. Inoue, K. Nagao, T. Inaoka, H. Kowada, A. Sakuda, M. Tatsumisago and A. Hayashi

    ACS Appl. Energy Mater.   5 ( 2 )   1421 - 1426   2022.01

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    Kind of work:Joint Work  

    DOI: https://doi.org/10.1021/acsaem.1c02452

  • Liquid-phase synthesis of Li<inf>3</inf>PS<inf>4</inf> solid electrolyte using ethylenediamine

    Akane Ito, Takuya Kimura, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    Journal of Sol-Gel Science and Technology   101 ( 1 )   2 - 7   2022.01( ISSN:0928-0707

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    Li3PS4 is the most typical solid electrolyte for all-solid-state lithium batteries. However, to date, there are few reports on Li3PS4 solid electrolyte synthesized using the solution process. Here, β-Li3PS4 solid electrolytes were prepared via liquid-phase synthesis by dissolving Li2S and P2S5 in ethylenediamine (EDA) to form a homogeneous solution of Li3PS4. Since EDA is a basic protonic solvent, it effectively suppressed the decomposition of Li3PS4. An intermediate phase consisting of Li3PS4 and EDA was formed as a precursor after drying the EDA solution at 200 °C under vacuum. After heat treatment at temperatures above 260 °C, β-Li3PS4 was crystallized from the precursor. The ionic conductivity of the prepared β-Li3PS4 was 5.0 × 10−5 S cm−1 at 25 °C and the activation energy for conduction was 35 kJ mol−1. The obtained EDA solution of Li3PS4 will be effective in forming electrolyte-electrode interfaces with the large contact areas in all-solid-state batteries. [Figure not available: see fulltext.]

    DOI: 10.1007/s10971-021-05524-y

  • Sodium-Ion Conducting Solid Electrolytes in the Na<inf>2</inf>S–In<inf>2</inf>S<inf>3</inf> System

    Kota Motohashi, Akira Nasu, Takuya Kimura, Chie Hotehama, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    Electrochemistry   90 ( 6 )   2022( ISSN:1344-3542

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    The development of solid electrolytes is necessary for practical applications of all-solid-state Na-ion batteries. In this study, we systematically developed sulfide Na-ion conductors with central In cations, prepared by solid-state reaction and mechanochemical methods. Thermodynamically stable crystals of Na5InS4 and NaInS2 were obtained by the solid-state reaction method, whereas amorphous and/or metastable phases were produced by the mechanochemical method. Two new metastable phases, Na5InS4 and NaInS2, are expected to be examined in the future as end-members of sulfide Na-ion conductors with central In cations.

    DOI: 10.5796/ELECTROCHEMISTRY.22-00037

  • Mechanochemically Prepared Highly Conductive Na<inf>2.88</inf>Sb<inf>0.88</inf>W<inf>0.12</inf>S<inf>4</inf>-NaI Composite Electrolytes for All-Solid-State Sodium Battery

    Takuma Takayanagi, Akira Nasu, Fumika Tsuji, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    Electrochemistry   90 ( 4 )   2022( ISSN:1344-3542

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    Solid electrolytes with high ionic conductivity, high formability, and high electrochemical properties are required to improve the performance of all-solid-state sodium batteries. In this study, we focus on a combination of Na2.88Sb0.88W0.12S4 and NaI for preparing composite electrolytes Na2.88Sb0.88W0.12S4·xNaI, and investigate their crystal structures, microstructures, and electrochemical properties. NaI is uniformly dispersed in the composites without forming a solid solution with Na2.88Sb0.88W0.12S4. Na2.88Sb0.88W0.12S4·0.50NaI shows a high ionic conductivity of 3.6 × 10−2 S cm−1 after sintering at 275 °C for only 1.5 h. The charge-discharge characteristics of all-solid-state cells using the Na2.88Sb0.88W0.12S4·xNaI composite are also improved.

    DOI: 10.5796/ELECTROCHEMISTRY.22-00016

  • Mechanochemical Synthesis of Pyrite Ni<inf>1−x</inf>Fe<inf>x</inf>S<inf>2</inf> Electrode for All-solid-state Sodium Battery

    Gaku Shirota, Akira Nasu, Atsushi Sakuda, Minako Deguchi, Kota Motohashi, Masahiro Tatsumisago, Akitoshi Hayashi

    Electrochemistry   90 ( 3 )   2022( ISSN:1344-3542

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    All-solid-state sodium secondary batteries are expected to be low-cost, next-generation batteries. NiS2 and FeS2 are potential candidates as positive electrode materials owing to their high theoretical capacities. However, it is difficult to achieve sufficient capacity with bulk FeS2. In this study, pyrite Ni1−xFexS2 (x = 0, 0.3, 0.5, 0.7, 0.9, and 1) electrodes are prepared by a mechanochemical process. The all-solid-state sodium cells with Ni1−xFexS2 show higher discharge-charge potentials than those with NiS2, and higher capacities than those with FeS2. In addition, Ni1−xFexS2 exhibits a higher rate performance than those of NiS2 and FeS2. The all-solid-state cells using Ni1−xFexS2 (x = 0.3, 0.5, and 0.7) are discharged and charged with a high capacity of approximately 390 mAh g−1, without significant capacity fading for at least 30 cycles. The solid-solution formation of NiS2 and FeS2 results in lower material cost, higher rate performance, higher discharge-charge potential than those of NiS2, and higher capacity than that of FeS2. Pyrite Ni1−xFexS2 is a promising positive electrode material for all-solid-state sodium secondary batteries.

    DOI: 10.5796/ELECTROCHEMISTRY.22-00007

  • Iron Sulfide Na<inf>2</inf>FeS<inf>2</inf> as Positive Electrode Material with High Capacity and Reversibility Derived from Anion–Cation Redox in All-Solid-State Sodium Batteries

    Akira Nasu, Atsushi Sakuda, Takuya Kimura, Minako Deguchi, Akihisa Tsuchimoto, Masashi Okubo, Atsuo Yamada, Masahiro Tatsumisago, Akitoshi Hayashi

    Small   18 ( 42 )   e2203383   2022( ISSN:1613-6810

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    It is desirable for secondary batteries to have high capacities and long lifetimes. This paper reports the use of Na2FeS2 with a specific structure consisting of edge-shared and chained FeS4 as the host structure and as a high-capacity active electrode material. An all-solid-state sodium cell that uses Na2FeS2 exhibits a high capacity of 320 mAh g−1, which is close to the theoretical two-electron reaction capacity of 323 mAh g−1, and operates reversibly for 300 cycles. The excellent electrochemical properties of all-solid-state sodium cells are derived from the anion–cation redox and rigid host structure during charging/discharging. In addition to the initial one-electron reaction of NaxFeS2 (1 ≤ x ≤ 2) activated Fe2+/Fe3+ redox as the main redox center, the reversible sulfur redox further contributes to the high capacity. Although the additional sulfur redox affects the irreversible crystallographic changes, stable and reversible redox reactions are observed without capacity fading, owing to the local maintenance of the chained FeS4 in the host structure. Sodium iron sulfide Na2FeS2, which combines low-cost elements, is one of the candidates that can meet the high requirements of practical applications.

    DOI: 10.1002/smll.202203383

    PubMed

  • Crystalline precursor derived from Li<inf>3</inf>PS<inf>4</inf> and ethylenediamine for ionic conductors

    Takuya Kimura, Akane Ito, Takumi Nakano, Chie Hotehama, Hiroe Kowada, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    Journal of Sol-Gel Science and Technology   104 ( 3 )   627 - 634   2022( ISSN:0928-0707

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    Liquid-phase syntheses of sulfide materials are attractive for the mass production of solid electrolytes for all-solid-state batteries. In liquid-phase synthesis, the precursor of the solid electrolyte is obtained. The precursors are important for producing electrolytes of the same quality because they decompose into electrolytes by heat treatment. However, only a few studies have focused on the formation mechanism and structure of precursors. This study proposes a formation mechanism for Li3PS4 during liquid-phase synthesis using ethylenediamine (EDA) as a solvent and clarifies the crystal structure of Li3PS4·NH2CH2CH2NH2 (Li3PS4·EDA). Raman spectroscopy and nuclear magnetic resonance revealed that intermediate P2S62− units were generated in the EDA solution. Crystal structure analysis of Li3PS4·EDA showed that the terminal nitrogen atom of EDA coordinates with two lithium atoms. Ionic conductivity of Li3PS4·EDA was 2.8 × 10−9 S cm−1 at 25 °C. The analysis of precursors of solid electrolytes provides insight into the behavior of solvent molecules as ligands in the synthesis of sulfide electrolytes. [Figure not available: see fulltext.]

    DOI: 10.1007/s10971-022-05824-x

  • AC Impedance Analysis of the Degeneration and Recovery of Argyrodite Sulfide-Based Solid Electrolytes under Dry-Room-Simulated Condition

    Hikaru Sano, Yusuke Morino, Akinori Yabuki, Shimpei Sato, Naohiko Itayama, Yasuyuki Matsumura, Masahiro Iwasaki, Masahiro Takehara, Takeshi Abe, Yasuo Ishiguro, Tsukasa Takahashi, Norihiko Miyashita, Atsushi Sakuda, Akitoshi Hayashi

    Electrochemistry   90 ( 3 )   2022( ISSN:1344-3542

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    Toward the development of all-solid-state batteries with enhanced performance, this study describes the investigation of the degeneration mechanism under low-humid conditions of an argyrodite-type sulfide-based solid electrolyte. The degeneration of the electrolyte with moisture occurs even under the condition of super-low humidity in a dry room with a dew point (dp) as low as −50 °Cdp. Formation of hydrogen sulfide is detected when the electrolyte is exposed to dry air with −20 °Cdp. The results of impedance measurements suggest that the grain surface of the electrolyte is degenerated with moisture, resulting in a decrease in the lithium-ion conductivity at the grain boundary. The degenerated electrolyte surface can be partially recovered by heating at 170 °C in vacuo, although a small degeneration in bulk may occur in the heating process.

    DOI: 10.5796/ELECTROCHEMISTRY.22-00013

  • In situ observation of the deterioration process of sulfide-based solid electrolytes using airtight and air-flow TEM systems

    Hirofumi Tsukasaki, Keisuke Igarashi, Akiko Wakui, Toshie Yaguchi, Hiroshi Nakajima, Takuya Kimura, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi, Shigeo Mori

    Microscopy   70 ( 6 )   519 - 525   2021.12( ISSN:2050-5698

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    Sulfide-based solid electrolytes (SEs) exhibiting high ionic conductivity are indispensable battery materials for next-generation all-solid-state batteries. However, sulfide-based SEs have a major drawback in their low chemical stability in air. When exposed to H2O or O2 gas, toxic H2S is generated, and their ionic conductivity considerably declines. However, their degradation mechanism caused by air exposure has not been understood yet. To clarify the degradation process, in this study, we developed a transmission electron microscope (TEM) system to evaluate the air stability of battery materials. Using a vacuum transfer double-tilt TEM holder with a gas-flow system, the in situ observation of the degradation process was conducted for a sulfide-based Li4SnS4 glass ceramic under an air-flow environment. Consequently, electron diffraction (ED) patterns and TEM images could clearly capture morphological changes and the amorphization process caused by air exposure. Moreover, based on the analysis of ED patterns, it is observed that Li4SnS4 is likely to decompose because of the reaction with H2O in air. Therefore, this airtight and air-flow TEM system should be effective in clarifying the process of the deterioration of sulfur-based SEs during exposure to air.

    DOI: 10.1093/jmicro/dfab022

    PubMed

  • Development, Structure, and Mechanical Properties of Sulfide Solid Electrolytes Reviewed

    K. Ohara, A. Sakuda and A. Hayashi

    Encyclopedia of Materials: Technical Ceramics and Glasses   3   38 - 48   2021.12

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  • Crystallization behaviors in superionic conductor Na<inf>3</inf>PS<inf>4</inf>

    Hiroshi Nakajima, Hirofumi Tsukasaki, Jiong Ding, Takuya Kimura, Takumi Nakano, Akira Nasu, Akihiko Hirata, Atsushi Sakuda, Akitoshi Hayashi, Shigeo Mori

    Journal of Power Sources   511   2021.11( ISSN:0378-7753

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    All-solid-state batteries using sodium are promising candidates for next-generation rechargeable batteries due to the limited lithium resources. A practical sodium battery requires an electrolyte with high conductivity. Cubic Na3PS4 exhibiting high conductivity of over 10−4 S cm−1 is obtained by crystallizing amorphous Na3PS4 synthesized by ball milling. Amorphous Na3PS4 crystallizes in a cubic structure and then is transformed into a tetragonal phase upon heating. In this study, in situ observation by transmission electron microscopy demonstrates that the crystallite size drastically increases during the transition from the cubic phase to the tetragonal phase. Moreover, an electron diffraction analysis reveals that amorphous domains and nano-sized crystallites coexist in the cubic Na3PS4 specimen, while the tetragonal phase contains micro-sized crystallites. The nano-sized crystallites and the composite formed by crystallites and amorphous domains are most likely responsible for the increase in conductivity in the cubic Na3PS4 specimens.

    DOI: 10.1016/j.jpowsour.2021.230444

  • Mechanochemical synthesis and characterization of Na<sub>3-x</sub>In<sub>1-x</sub>Zr<sub>x</sub>Cl<sub>6</sub> solid electrolytes

    岡田侑也, 木村拓哉, 作田敦, 林晃敏

    電池討論会PDF要旨集(CD-ROM)   62nd   2021.09( ISSN:0378-7753

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    All-solid-state sodium batteries are attracting attention as next-generation batteries, owing to their improved safety and abundance of sodium resources. To realize all-solid-state sodium batteries, solid electrolytes with high sodium-ion conductivities are required. In this study, Na3PS4 electrolytes with partial substitution of P5+ with W6+ were investigated. The Na3–xP1–xWxS4 sulfide-based solid electrolytes were prepared via a mechanochemical process and consecutive heat treatment. The Na2.85P0.85W0.15S4 electrolyte with Na vacancies exhibited an ionic conductivity of 8.8 × 10−3 S cm−1 at 25 °C, which was higher than that of Na3PS4 solid electrolyte. The all-solid-state batteries (Na-Sn/Na2.85P0.85W0.15S4/TiS2) exhibited a reversible capacity of 140 mA h g−1 at a current density of 0.038 mA cm−2 and retained the capacity of 115 mAh g−1 for 40 cycles at 0.130 mA cm−2 at 25 °C. The Na3–xP1–xWxS4 samples prepared via mechanochemistry are homogeneous electrolytes free of crystalline WS2 impurities and are effective for application to all-solid-state sodium batteries.

    DOI: 10.1016/j.jpowsour.2021.230100

    J-GLOBAL

  • Crystallization Behaviors in Superionic Conductor Na3PS4 Reviewed

    H. Nakajima, H. Tsukasaki, J. Ding, T. Kimura, T. Nakano, A. Nasu, A. Hirata, A. Sakuda, A. Hayashi, S. Mori

    Jounal of Power Sources 雑誌   511 ( 230444 )   1 - 7   2021.08

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  • Investigation of the suppression of dendritic lithium growth with a lithium-iodide-containing solid electrolyte

    Masakuni Takahashi, Toshiki Watanabe, Kentaro Yamamoto, Koji Ohara, Atsushi Sakuda, Takuya Kimura, Seunghoon Yang, Koji Nakanishi, Tomoki Uchiyama, Masao Kimura, Akitoshi Hayashi, Masahiro Tatsumisago, Yoshiharu Uchimoto

    Chemistry of Materials   33 ( 13 )   4907 - 4914   2021.07( ISSN:0897-4756

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    Publishing type:Research paper (scientific journal)  

    All-solid-state lithium batteries that use lithium metal as the anode have extremely high energy densities. However, for lithium metal anodes to be used, lithium dendrite formation must be addressed. Recently, the addition of lithium iodide (LiI) to sulfide solid electrolytes was found to suppress lithium dendrite formation. It is unclear whether the cause of this suppression is the improvement of the ionic conductivity of the solid electrolyte itself or the electrochemical properties of the lithium metal/solid electrolyte interface. In this study, the cause of the suppression was quantitatively elucidated. The effect of the interphase on the dendrite growth of doping LiI into Li3PS4 was determined using X-ray absorption spectroscopy and X-ray computed tomography measurements. The results revealed that LiI-doped Li3PS4 suppressed the dendrite formation by maintaining the interface due to inhibition of the reductive decomposition of Li3PS4. In addition, annealed LiI-doped Li3PS4 showed a greater dendrite suppression ability as the ionic conductivity increased. From these results, we not only found that the physical properties of the lithium metal/solid electrolyte interface and the bulk ionic conductivity contribute to lithium dendrite suppression but also quantitatively determined the proportions of the contributions of these two factors.

    DOI: 10.1021/acs.chemmater.1c00270

  • Structures and conductivities of stable and metastable Li<inf>5</inf>GaS<inf>4</inf>solid electrolytes

    Takuya Kimura, Chie Hotehama, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    RSC Advances   11 ( 41 )   25211 - 25216   2021.07

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    Publishing type:Research paper (scientific journal)  

    Understanding the differences in the structures and defects in the stable crystalline phase and metastable phase is important for increasing the ionic conductivities of a solid electrolyte. The metastable phase often has higher conductivity than the stable phase. In this study, metastable lithium thiogallate, Li5GaS4, was synthesizedviamechanochemistry and stable Li5GaS4was obtained by heating the metastable phase. The metastable Li5GaS4sample was found to have an antifluorite-type crystal structure with cationic disorder, while the stable phase was found to have a monoclinic crystal structure, similar to that of another solid electrolyte, Li5AlS4. In both the structures, the Ga3+cations were surrounded by four S2−anions in tetrahedral coordination. The conductivity of the metastable phase was determined to be 2.1 × 10−5S cm−1at 25 °C, which is 1000 times greater than that of the monoclinic phase. The high conductivity of the metastable phase was achieved owing to cation disorder in the crystal structure.

    DOI: 10.1039/d1ra03194e

  • Glassy oxide electrolytes in the system Li<inf>4</inf>SiO<inf>4</inf>Li<inf>2</inf>SO<inf>4</inf> with excellent formability

    Yohei Yoneda, Chie Hotehama, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    Journal of the Ceramic Society of Japan   129 ( 7 )   458 - 463   2021.07( ISSN:1882-0743

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    Publishing type:Research paper (scientific journal)  

    All-solid-state batteries using oxide electrolytes are regarded as safe batteries. However, most crystalline oxide solid electrolytes require high-temperature sintering for densification. Oxide electrolytes with high formability, which enable the construction of high-performance batteries, are thus required. In this study, Li4SiO4Li2SO4 glasses and glass-ceramics were prepared by mechanochemical treatment and subsequent heat treatment at 270 °C to achieve electrolytes with high formability. As the Li2SO4 content was increased, the formability of the electrolyte increased. The 90Li4SiO4·10Li2SO4 glass-ceramic electrolyte with a hexagonal structure (a P63/mmc space group) showed the highest ionic conductivity of 2.2 © 1016 S cm11 at 25 °C. In this crystal structure, oxygen anions form a hexagonal close-packed structure, and silicon and sulfur cations randomly occupy the tetrahedral sites formed by oxygen anions. An all-solid-state LiIn/LiNi1/3Mn1/3Co1/3O2 cell using a 90Li4SiO4·10Li2SO4 glass-ceramic electrolyte operated at 100 °C as a secondary battery without high-temperature sintering. These oxide materials are promising solid electrolytes for oxide-type all-solid-state batteries.

    DOI: 10.2109/jcersj2.21027

  • Glassy Oxide Electrolytes in the System Li4SiO4-Li2SO4 with Excellent Formability Reviewed

    Y. Yoneda, C. Hotehama, A. Sakuda, M. Tatsumisago and A. Hayashi

    Journal of the Ceramic Society of Japan 雑誌   129 ( 7 )   458 - 463   2021.07

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    Kind of work:Joint Work  

  • Amorphous Li2O-LiI Solid Electrolytes Compatible to Li Metal Reviewed

    Y. Fujita, Y. Kawasaki, T. Inaoka, T. Kimura, A. Sakuda, M. Tatsumisago and A. Hayashi

    Electrochemistry 雑誌   89 ( 4 )   334 - 336   2021.07

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  • Microstructure and Charge-Discharge Mechanism of a Li<inf>3</inf>CuS<inf>2</inf>Positive Electrode Material for All-Solid-State Lithium-Ion Batteries

    Tomoji Ayama, Hirofumi Tsukasaki, Yusuke Kawasaki, Hiroshi Nakajima, Masahiro Tatsumisago, Atsushi Sakuda, Akitoshi Hayashi, Shigeo Mori

    ACS Applied Energy Materials   4 ( 6 )   6290 - 6295   2021.06

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    Publishing type:Research paper (scientific journal)  

    To develop all-solid-state lithium batteries, high-capacity positive electrode materials are necessary. An antifluorite-type material, Li2S, exhibits a high theoretical capacity. However, Li2S cannot be used as a positive electrode for the all-solid-state cell because of its insulating behavior. To provide electronic and ionic conduction, recently, antifluorite-type Li3CuS2 has been developed by activation of Li2S by Cu substitution. Li3CuS2 is a favorable candidate for positive electrodes as sulfide-based all-solid-state cells with Li3CuS2 exhibit high charge-discharge performance. However, structural changes and redox species during the charge-discharge cycle have not been understood yet. To clarify the charge-discharge mechanism of Li3CuS2, in this study, we examined the microstructural changes in a Li3CuS2-Li3PS4 positive electrode composite during charge and discharge by transmission electron microscopy (TEM). The hollow-cone dark-field imaging technique was employed to evaluate the crystallite size distribution. The result shows that the crystallite size of Li3CuS2 reversibly decreases and increases in the charging and discharging states, respectively. The electron diffraction pattern shows that LiCuS2 was formed during charging, which is attributed to Li+ extraction from Li3CuS2. In the discharging state, the crystallite size increased and Li3CuS2 was reproduced. The TEM results suggest that the reversible structural changes (Li3CuS2 ⇆ LiCuS2 + 2Li+ + 2e-) would contribute to high charge-discharge characteristics.

    DOI: 10.1021/acsaem.1c01074

  • Solid electrolytes Na10+xSn1+xP2-xS12 prepared via a mechanochemical process

    Fumika TSUJI, Kah Loong HOH, Kwang Hyun KIM, Atsushi SAKUDA, Masahiro TATSUMISAGO, Steve W. MARTIN, Akitoshi HAYASHI

    Journal of the Ceramic Society of Japan   129 ( 6 )   323 - 328   2021.06( ISSN:1882-0743

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    Solid electrolytes are important materials for enhancing the performance of all-solid-state sodium rechargeable batteries. Na10+xSn1+xP2-xS12 (0 ≤ x ≤ 1.2) samples were prepared using a mechanochemical process, followed by heat treatment and their structures and ionic conductivities were investigated. Glassy samples were obtained via the mechanochemical process; the samples with the Na11Sn2PS12 type crystal structure were obtained for all the prepared compositions through the heat treatment of the glasses. The Na11Sn2PS12 (x = 1) sample obtained by heat treatment at 300°C exhibited an ionic conductivity of 2.6

    DOI: 10.2109/jcersj2.21010

  • Mechanochemical Synthesis and Characterization of Na3-xP1-xWxS4 Solid Electrolytes Reviewed

    F. Tsuji, A. Nasu, A. Sakuda, M. Tatsumisago and A. Hayashi

    Journal of Power Sourses 雑誌   506 ( 230100 )   1 - 8   2021.06

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  • Investigation of the Suppression of Dendritic Lithium Growth with a Lithium-Iodide-Containing Solid Electrolyte Reviewed

    M. Takahashi, T. Watanabe, K. Yamamoto, K. Ohara, A. Sakuda, T. Kimura, S.H. Yang, K. Nakanishi, T. Uchiyama, M, Kimura, A. Hayashi, M. Tatsumisago and Y. Uchimoto

    Chem. Mater. 雑誌   33   4907 - 4914   2021.06

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  • In Situ Observation of the Deterioration Process of Sulfide-based Solid Electrolytes Using Airtight and Air-Flow TEM Systems Reviewed

    H. Tsukasaki, K. Igarashi, A. Wakui, T. Yaguchi, H. Nakajima, T. Kimura, A. Sakuda, M. Tatsumisago, A. Hayashi and S. Mori

    Microscopy 雑誌   2021   1 - 7   2021.06

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    Kind of work:Joint Work  

  • Importance of Li-Metal/Sulfide Electrolyte Interphase Ionic Conductivity in Suppressing Short-Circuiting of All-Solid-State Li-Metal Batteries Reviewed

    M. Suyama, S. Yubuchi, M. Deguchi, A. Sakuda, M. Tatsumisago and A. Hayashi

    Journal of The Electrochemical Society 雑誌   168 ( 060542 )   1 - 6   2021.06

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  • Electrode Performance of Amorphous MoS3 in All-Solid-State Sodium Secondary Batteries Reviewed

    G. Shirota, A. Nasu, M. Deguchi, A. Sakuda, M. Tatsumisago and A. Hayashi

    Journal of Power Sources Advances 雑誌   10 ( 100061 )   1 - 7   2021.06

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  • Solid Electrolytes Na10+xSn1+xP2-xS12 Prepared via a Mechanochemical Process Reviewed

    F. Tsuji, K.L. Hoh, K.H. Kim, A. Sakuda, M. Tatsumisago, S.W. Martin and A. Hayashi

    Journal of the Ceramic Society of Japan 雑誌   129 ( 6 )   323 - 328   2021.06

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    Kind of work:Joint Work  

  • Microstructure and Charge-Discharge Mechanism of a Li3CuS2 Positive Electrode Material for All-Solid-State Lithium-Ion Batteries Reviewed

    T. Ayama, H. Tsukasaki, Y. Kawasaki, H. Nakajima, M. Tatsumisago, A. Sakuda, A. Hayashi and S. Mori

    ACS Appl. Energy Mater.   4   6290 - 6295   2021.06

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  • Importance of li-metal/sulfide electrolyte interphase ionic conductivity in suppressing short-circuiting of all-solid-state li-metal batteries

    Motoshi Suyama, So Yubuchi, Minako Deguchi, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    Journal of the Electrochemical Society   168 ( 6 )   2021.06( ISSN:0013-4651

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    Publishing type:Research paper (scientific journal)  

    The electronic and ionic conductivities of the interphase that forms between Li metal and solid electrolytes (SEs) are key parameters in determining battery cell performance. In this study, we evaluated the effect of the interphase on Li dissolution/deposition behaviors. The reduction of Li2S-P2S5 glasses to Li2S and Li3P by Li metal occurred at the Li/SE interface. The Li dissolution/deposition performance at 100 °C was improved by increasing the Li3P content in the interphase, and the cell with a Li4P2S6 glass electrolyte functioned without short-circuiting at a current density of 1.3 mA cm-2. The ionic conductivity of the Li/SE interphase was evaluated by preparing Li-SE compounds using mechanochemical processing. The milled sample prepared from Li metal and Li4P2S6 glass showed a one order of magnitude higher conductivity of 10-4 S cm-1 at 100 °C than that of the Li-Li3PS4 milled sample, indicating that the ionic conductivity of the interphase formed at the Li/SE interface is an important factor for improving the short-circuiting tolerance of all-solid-state Li-metal batteries.

    DOI: 10.1149/1945-7111/ac0995

  • Development, structure, and mechanical properties of sulfide solid electrolytes

    Koji Ohara, Atsushi Sakuda, Akitoshi Hayashi

    Encyclopedia of Materials: Technical Ceramics and Glasses   3-3   38 - 48   2021.05( ISBN:9780128222331

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    Publishing type:Part of collection (book)  

    DOI: 10.1016/B978-0-12-803581-8.12133-2

  • Preparation and characterization of Li<sub>4</sub>GeO<sub>4</sub>-based oxide glass-ceramic electrolytes via the mechanochemical method

    米田陽平, 作田敦, 辰巳砂昌弘, 林晃敏

    電気化学会大会講演要旨集(CD-ROM)   88th   2021.05( ISSN:0167-2738

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    A new lithium-ion conducting oxide, hexagonal Li4GeO4, with a space group of P63/mmc, was prepared by mechanochemical treatment and subsequent heat treatment at 250 °C. The crystal structure was found in sulfide Li4SnS4, and this is the first study to report an oxide system. In addition, (100-x)Li4GeO4·xLi2MO4 (M = S or W; x = 10, 20, 30, and 40 mol%) glass-ceramic electrolytes with the hexagonal phase were prepared by crystallization of their mother glasses. The formability of the electrolytes improved as the quantity of Li2SO4 increased, and the 90Li4GeO4·10Li2SO4 glass-ceramic electrolyte showed the highest ionic conductivity of 2.9 × 10−6 S cm−1 at 25 °C. Compared with the experimental results, the bond valence sum (BVS) analysis results indicated that ionic conduction paths are easily connected along the c-axis in the hexagonal phase, suggesting that the relatively small lattices in the a- and b-axes are more advantageous for three-dimensional ionic conduction.

    DOI: 10.1016/j.ssi.2021.115605

    J-GLOBAL

  • High Ionic Conductivity of Liquid-Phase-Synthesized Li3PS4 Solid Electrolyte, Comparable to That Obtained via Ball Milling Reviewed

    K. Yamamoto, S.H. Yang, M. Takahashi , K. Ohara, T. Uchiyama, T. Watanabe, A. Sakuda, A. Hayashi, M. Tatsumisago, H. Muto, A. Matsuda and Y. Uchimoto

    ACS Appl. Energy Mater. 雑誌   4   2275 - 2281   2021.04

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    Kind of work:Joint Work  

  • Synthesis and Electrochemical Properties of Li3CuS2 as a Positive Electrode Material for All-Solid-State Batteries Reviewed

    Y. Kawasaki, H. Tsukasaki, T. Ayama, S. Mori, M. Deguchi, M. Tatsumisago, A. Sakuda and A. Hayashi

    ACS Appl. Energy Mater. 雑誌   4   20 - 24   2021.04

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  • Preparation and Characterization of Hexagonal Li4GeO4-based Glass-Ceramic Electrolytes Reviewed

    Y. Yoneda, M. Shigeno, T. Kimura, K. Nagao, C. Hotehama, A. Sakuda, M. Tatsumisago and A. Hayashi

    Solid State Ionics 雑誌   363 ( 115605 )   1 - 7   2021.04

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  • Improvement of Electrochemical Property of VS4 Electrode Material by Amorphization via Mechanical Milling Process Reviewed

    K. Koganei, A. Sakuda, T. Takeuchi, H. Kiuchi and H. Sakaebe

    Electrochemistry 雑誌   89 ( 3 )   239 - 243   2021.04

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  • Visualizing Local Electrical Properties of Composite Electrodes in Sulfide All-Solid-State Batteries by Scanning Probe Microscopy Reviewed

    M. Otoyama, T. Yamaoka, H. Ito, Y. Inagi, A. Sakuda, M. Tatsumisago and A. Hayashi

    J. Phys. Chem. C 雑誌   125   2841 - 2849   2021.04

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  • High Ionic Conductivity of Liquid-Phase-Synthesized Li<inf>3</inf>PS<inf>4</inf>Solid Electrolyte, Comparable to That Obtained via Ball Milling

    Kentaro Yamamoto, Seunghoon Yang, Masakuni Takahashi, Koji Ohara, Tomoki Uchiyama, Toshiki Watanabe, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago, Hiroyuki Muto, Atsunori Matsuda, Yoshiharu Uchimoto

    ACS Applied Energy Materials   4 ( 3 )   2275 - 2281   2021.03( ISSN:2574-0962

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    Recently, several sulfide solid electrolytes have been synthesized by liquid-phase synthesis for the commercialization of all-solid-state batteries. Unfortunately, the ionic conductivity for most of these electrolytes is unsatisfactory compared to that of solid electrolytes synthesized by conventional ball milling. This problem is attributed to different mechanisms between the liquid phase and the solid phase in reaction and formation. However, to the best of our knowledge, the effect of the solvent on the ionic conductivity of solid electrolytes has not been extensively investigated, although the identification of these properties is a key point in understanding the liquid-phase synthesis. Herein, the correlation between ionic conductivity and crystallinity originating from the solvents used has been investigated. As a result, the ionic conductivity of the electrolyte was found to be strongly dependent on polarity (δP) with low crystallinity. The highest ionic conductivity (5.09 × 10-4 S cm-1 at 25 °C) was obtained using butyl acetate, which exhibited the lowest δP. Moreover, the highest ionic conductivity of Li3PS4 produced by liquid-phase synthesis using butyl acetate was very comparable to that obtained by ball milling (5.14 × 10-4 S cm-1).

    DOI: 10.1021/acsaem.0c02771

  • Improvement of lithium ionic conductivity of Li<inf>3</inf>PS<inf>4</inf> through suppression of crystallization using low-boiling-point solvent in liquid-phase synthesis

    Masakuni Takahashi, Seunghoon Yang, Kentaro Yamamoto, Koji Ohara, Nguyen Huu Huy Phuc, Toshiki Watanabe, Tomoki Uchiyama, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago, Hiroyuki Muto, Atsunori Matsuda, Yoshiharu Uchimoto

    Solid State Ionics   361   115568 - 115568   2021.03( ISSN:0167-2738

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    Liquid-phase synthesis for solid electrolytes has received considerable attention owing to its shape control, with the potential to produce particles easily on a large scale, and its low cost and energy consumption. However, solid electrolytes prepared through liquid-phase synthesis have been shown to have lower ionic conductivity than solid electrolytes prepared through the mechanical milling method. Recently, following various efforts, our group found that the crystallinity and remaining intermediate are the reasons for the low ionic conductivity of these materials. By using tetrahydrofuran (THF), we successfully improved the ionic conductivity of Li3PS4 to 1.85 × 10−4 S cm−1 at 25 °C, higher than that afforded by ethyl propionate, which was reported to produce the highest ionic conductivity among the solvents used for liquid-phase synthesis. High-energy X-ray diffraction (XRD) measurements coupled with pair distribution function (PDF) analysis were employed to analyze the synthesized materials in order to determine why the ionic conductivity was higher than that of a sample prepared using ethyl propionate. The PDF analysis revealed that the crystallization of Li3PS4 can be suppressed using THF, which has a lower boiling point than ethyl propionate. Moreover, it was revealed that the solvent could not be removed completely when the material has an amorphous structure, and thus, the ionic conductivity was lower than that of a material prepared using the solid-phase synthesis method.

    DOI: 10.1016/j.ssi.2021.115568

  • Visualizing local electrical properties of composite electrodes in sulfide all-solid-state batteries by scanning probe microscopy

    Atsushi Sakuda, Misae Otoyama, Takehiro Yamaoka, Hiroyuki Ito, Yuki Inagi, Masahiro Tatsumisago, Akitoshi Hayashi

    Journal of Physical Chemistry C   125 ( 5 )   2841 - 2849   2021.02( ISSN:1932-7447

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    Studies on local conduction paths in composite electrodes are essential to the realization of high-performance sulfide all-solid-state lithium batteries. Here, we directly evaluate the electrical properties of individual LiNi1/3Mn1/3Co1/3O2 (NMC) electrode active material particles in composite positive electrodes by scanning probe microscopy (SPM) techniques. Kelvin probe force microscopy (KPFM) and scanning spreading resistance microscopy (SSRM) are combined. The results indicate that all NMC particles exhibit a charged state with increasing potential, but low electronic conduction paths exist at point of contacts of some NMC particles. Furthermore, the I-V characteristics measured by conductive atomic force microscopy (C-AFM) suggest that these specific NMC particles show low charge-discharge reactivity. The results of the SPM techniques indicate that poor conduction locally limits the charge-discharge reactivity of electrode active materials, leading to the degradation of battery performance. Such an SPM combination accelerates the morphological optimization of composite electrodes by facilitating the investigation of the intrinsic electrical properties of the electrodes.

    DOI: 10.1021/acs.jpcc.0c10148

  • Visualization and Control of Chemically Induced Crack Formation in All-Solid-State Lithium-Metal Batteries with Sulfide Electrolyte

    Misae Otoyama, Motoshi Suyama, Chie Hotehama, Hiroe Kowada, Yoshihiro Takeda, Koichiro Ito, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    ACS Applied Materials and Interfaces   13 ( 4 )   5000 - 5007   2021.02( ISSN:1944-8244

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    The application of lithium metal as a negative electrode in all-solid-state batteries shows promise for optimizing battery safety and energy density. However, further development relies on a detailed understanding of the chemo-mechanical issues at the interface between the lithium metal and solid electrolyte (SE). In this study, crack formation inside the sulfide SE (Li3PS4: LPS) layers during battery operation was visualized using in situ X-ray computed tomography (X-ray CT). Moreover, the degradation mechanism that causes short-circuiting was proposed based on a combination of the X-ray CT results and scanning electron microscopy images after short-circuiting. The primary cause of short-circuiting was a chemical reaction in which LPS was reduced at the lithium interface. The LPS expanded during decomposition, thereby forming small cracks. Lithium penetrated the small cracks to form new interfaces with fresh LPS on the interior of the LPS layers. This combination of reduction-expansion-cracking of LPS was repeated at these new interfaces. Lithium clusters eventually formed, thereby generating large cracks due to stress concentration. Lithium penetrated these large cracks easily, finally causing short-circuiting. Therefore, preventing the reduction reaction at the interface between the SE and lithium metal is effective in suppressing degradation. In fact, LPS-LiI electrolytes, which are highly stable to reduction, were demonstrated to prevent the repeated degradation mechanism. These findings will promote all-solid-state lithium-metal battery development by providing valuable insight into the design of the interface between SEs and lithium, where the selection of a suitable SE is vital.

    DOI: 10.1021/acsami.0c18314

    PubMed

  • Preparation and Characterization of Sodium-Ion Conductive Na3BS3 Glass and Glass-Ceramic Electrolytes Reviewed

    F. Tsuji, A. Nasu, C. Hotehama, A. Sakuda, M. Tatsumisago and A. Hayashi

    Mater. Adv. 雑誌   2   1676 - 1682   2021.02

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  • Comparison of Sulfur Cathode Reactions between a Concentrated Liquid Electrolyte System and a Solid-State Electrolyte System by Soft X-Ray Absorption Spectroscopy

    Yao Xiao, Kentaro Yamamoto, Yukiko Matsui, Toshiki Watanabe, Atsushi Sakuda, Koji Nakanishi, Tomoki Uchiyama, Akitoshi Hayashi, Shoso Shingubara, Masahiro Tatsumisago, Masashi Ishikawa, Masayoshi Watanabe, Yoshiharu Uchimoto

    ACS Applied Energy Materials   4 ( 1 )   186 - 193   2021.01( ISSN:2574-0962

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    Sulfur is one of the promising next-generation cathode materials because of its low cost and high theoretical gravimetric capacity. However, the reaction mechanism of the sulfur cathode is largely influenced by the electrolyte and the intermediate sulfur species during the first discharge process has not been quantitatively explored in different electrolytes. In this study, we elucidated the reaction mechanism of sulfide cathodes by using three different electrolyte systems, viz., a conventional liquid electrolyte [LiPF6/ethylene carbonate (EC)/ethylene-methyl carbonate (EMC)], a concentrated liquid electrolyte [lithium bis(trifluorosulfonyl)amide (LiTFSA)/tetraglyme (G4):1,1,2,2-tetrafluoroethyl 2,2,3,3-tetrafluoropropyl ether (HFE)], and a solid-state electrolyte (Li3PS4). Soft X-ray absorption spectroscopy was used to examine the reaction mechanism of the sulfur cathode in the liquid and solid-state electrolytes during the first discharge process. In the conventional electrolyte, the sulfur cathode was reduced to long-chain polysulfide (S62-) during the first discharge process, and the polysulfide subsequently dissolved into the electrolyte. In the concentrated electrolyte, the sulfur cathode was reduced to midchain polysulfide (S42-) at the initial stage of the first discharge process and then reduced to short-chain polysulfide (S22-) and Li2S, followed by the formation of long-chain polysulfide (S62-). In the solid-state electrolyte, the sulfur cathode was reduced to long-chain polysulfide (S62-) at the initial stage of the first discharge process and was gradually reduced to mid-chain polysulfide (S42-), short-chain polysulfide (S22-), and Li2S. The differences in these reaction pathways govern electrochemical properties such as the difference in discharge voltage.

    DOI: 10.1021/acsaem.0c02063

  • Synthesis and Electrochemical Properties of Li<inf>3</inf>CuS<inf>2</inf>as a Positive Electrode Material for All-Solid-State Batteries

    Yusuke Kawasaki, Hirofumi Tsukasaki, Tomoji Ayama, Shigeo Mori, Minako Deguchi, Masahiro Tatsumisago, Atsushi Sakuda, Akitoshi Hayashi

    ACS Applied Energy Materials   4 ( 1 )   20 - 24   2021.01

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    All-solid-state batteries using flame-retardant inorganic solid electrolytes boast of advantages such as safety and wide usable temperature ranges. Although Li2S with an antifluorite-type structure has a high theoretical capacity, it is challenging to use in all-solid-state batteries because of the insulating nature. Here, we report an antifluorite-type Li3CuS2 as a sulfide positive electrode active material with high electronic conductivity. All-solid-state batteries using Li3CuS2 were successfully operated without the addition of conductive additives to the positive electrode. The Li3CuS2 exhibited an initial charge-discharge capacity of 380 mAh g-1 with an average discharge voltage of 2.1 V vs Li+/Li.

    DOI: 10.1021/acsaem.0c02657

  • Visualization and Control of Chemically Induced Crack Formation in All-Solid-State Lithium-Metal Batteries with Sulfide Electrolyte Reviewed

    M. Otoyama, M. Suyama, C. Hotehama, H. Kowada, Y. Takeda, K. Ito, A. Sakuda, M. Tatsumisago and A. Hayashi

    ACS Appl. Mater. Interfaces 雑誌   13   5000 - 5007   2021.01

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    Kind of work:Joint Work  

  • Comparison of Sulfur Cathode Reactions between a Concentrated Liquid Electrolyte System and a Solid-State Electrolyte System by Soft X-Ray Absorption Spectroscopy Reviewed

    Y. Xiao, K. Yamamoto, Y. Matsui, T. Watanabe, A. Sakuda, K. Nakanishi, T. Uchiyama, A. Hayashi, S. Shingubara, M. Tatsumisago, M. Ishikawa, M. Watanabe and Y. Uchimoto

    ACS Appl. Energy Mater. 雑誌   4   186 - 193   2021.01

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  • Improvement of Lithium Ionic Conductivity of Li3PS4 through Suppression of Crystallization Using Low-Boiling-Point Solvent in Liquid-phase Synthesis Reviewed

    M. Takahashi, S. H. Yang, K. Yamamoto, K. Ohara, N. H. H. Phuc, T. Watanabe, T. Uchiyama, A. Sakuda, A. Hayashi, M. Tatsumisago, H. Muto, A. Matsuda and Y. Uchimoto

    Solid State Ionics 雑誌   361 ( 115568 )   1 - 5   2021.01

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  • Amorphous Li<inf>2</inf>O-lii solid electrolytes compatible to li metal

    Yushi Fujita, Yusuke Kawasaki, Takeaki Inaoka, Takuya Kimura, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    Electrochemistry   89 ( 4 )   334 - 336   2021( ISSN:1344-3542

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    Development of oxide solid electrolytes for all-solid-state batteries is attracting increasing attention. In this study, amorphous Li2O-LiI materials are prepared via a mechanochemical process to achieve high lithium ionic conductivity and good compatibility to lithium metal. Amorphous 66.7Li2O·33.3LiI (mol%) electrolyte shows a high ionic conductivity of 3.1 × 10−5 S cm−1 at 25 °C with a relative density of 96 %. An all-solid-state Li symmetric cell (Li/66.7Li2O·33.3LiI/Li) operates without an increase in overvoltage. A simple combination of lithium oxide and lithium iodide exhibits high ionic conductivity, ductility, and stability to lithium metal.

    DOI: 10.5796/electrochemistry.21-00049

  • Improvement of electrochemical property of VS<inf>4</inf>electrode material by amorphization via mechanical milling process

    Kazuto KOGANEI, Atsushi SAKUDA, Tomonari TAKEUCHI, Hisao KIUCHI, Hikari SAKAEBE

    Electrochemistry   89 ( 3 )   239 - 243   2021( ISSN:1344-3542

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    Amorphous VS4(a-VS4) electrode material was synthesized by mechanical milling of crystalline VS4(c-VS4). The columbic efficiency of the a- VS4cell was significantly improved (ca. 86 %) at the first cycle as compared with the c-VS4cell (ca. 77 %), resulting in the improved capacity retention for prolonged cycling. Pair distribution function (PDF) analysis obtained from X-ray total scattering data, revealed that the radial atomic distribution of a-VS4at initial stage was similar to that of the low-crystalline VS4appeared after the first cycle of c-VS4. This is suggestive that the amorphization via mechanical milling process gave rise to the preparation of "first cycled VS4" which would contribute to the improved columbic efficiency at the first cycle and the resulting improved capacity retention for prolonged cycling. The structure of a-VS4could be visualized by first-principles molecular dynamic calculation of "first-cycled VS4".

    DOI: 10.5796/electrochemistry.21-00015

  • Preparation and Characterization of Cation-Substituted Na<inf>3</inf>SbS<inf>4</inf> Solid Electrolytes

    Fumika Tsuji, Naoki Masuzawa, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    ACS Applied Energy Materials   3 ( 12 )   11706 - 11712   2020.12

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    To realize all-solid-state sodium-ion batteries, the ionic conductivities and stabilities of solid electrolytes must be improved. The sulfide Na3SbS4 electrolyte is known to show a high sodium-ion conductivity of over 10-3 S cm-1 at room temperature. In this study, cation-substituted Na3SbS4 solid electrolytes with excess Na or Na vacancies were prepared, and the effects of substitution on the material conductivity were examined. The ionic conductivities of the Na3+xSb1-xMxS4 (M = Si, Ge, Sn) electrolytes, which were doped with excess Na, were lower than that of the Na3SbS4 electrolyte; in contrast, the conductivities of the Na3-xSb1-xMoxS4 electrolytes, which were doped with Na vacancies, were higher. The Na2.88Sb0.88Mo0.12S4 electrolyte showed the highest room-temperature ionic conductivity of 3.9 × 10-3 S cm-1 and the lowest activation energy for conduction of 21 kJ mol-1. To improve the ionic conductivity of the Na3SbS4 electrolyte, introducing Na vacancies instead of excess Na was found to be effective.

    DOI: 10.1021/acsaem.0c01823

  • Exothermal behavior and microstructure of a LiNi<inf>1/3</inf>Mn<inf>1/3</inf>Co<inf>1/3</inf>O<inf>2</inf> electrode layer using a Li<inf>4</inf>SnS<inf>4</inf> solid electrolyte

    Hirofumi Tsukasaki, Misae Otoyama, Takuya Kimura, Shigeo Mori, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago

    Journal of Power Sources   479   2020.12( ISSN:0378-7753

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    © 2020 Elsevier B.V. A positive electrode containing Li3PS4 (LPS) glasses and LiNi1/3Mn1/3Co1/3O2 (NMC) is a promising candidate for sulfide-based all-solid-state lithium batteries owing to its excellent charge–discharge cycle characteristics. However, sulfide-based solid electrolytes exhibit low chemical stability in air. This disadvantage affects process cost and thermal stability of all-solid-state cells. To resolve these issues, in this study, we focus on solid electrolytes, Li4SnS4 (LSS), that do not generate H2S gas in air. The thermal behavior and microstructure of LSS–NMC positive electrode composites before and after the initial charge–discharge cycle are investigated. The initially charged LSS–NMC composites exhibit several exothermal reactions above 250 °C. However, pristine and initially discharged samples do not show any considerable exothermal reactions. For LPS–NMC composites, by contrast, exothermal reactions are detected regardless of the charging and discharging state. To clarify the exothermic factors of initially charged LSS–NMC composites, we performed ex situ transmission electron microscopy observation and X-ray diffraction measurements. It is determined that SnS2, transition metal sulfides, and metal oxides are formed above 300 °C, which is attributable to LSS and NMC decomposition reactions. On the basis of the relation between thermal behavior and corresponding structural changes, exothermic factors and thermal stability of LSS–NMC composites are discussed in comparison with LPS–NMC composites.

    DOI: 10.1016/j.jpowsour.2020.228827

  • Preparation and Characterization of Cation-Substituted Na3SbS4 Solid Electrolytes Reviewed

    F. Tsuji, N. Masuzawa, A. Sakuda, M. Tatsumisago and A. Hayashi

    ACS Appl. Energy Mater. 雑誌   3   11706 - 11712   2020.12

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  • Effect of volume changes of active materials under different compressive pressures on the performance and microstructure of sulfide-based all-solid-state batteries

    山本真理, 寺内義洋, 作田敦, 加藤敦隆, 高橋雅也

    電池討論会PDF要旨集(CD-ROM)   61st   228595 - 228595   2020.10( ISSN:0378-7753

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    Compressive pressure applied during the operation of all-solid-state batteries that employ a sulfide solid electrolyte (SE) assists particle contact, thereby maintaining the ionic and electronic conduction network. The relationship between compressive pressure and volume variation in active materials is critical for designing practical full-cells with enhanced cell-based energy densities. However, studies into these aspects are rare. Here, we systematically investigate the effects of volume change of active materials [silicon, graphite, and LiNi1/3Mn1/3Co1/3O2 (NMC)] at different pressures (75 and 50 MPa) on electrochemical performance, cell internal resistance, and microstructure of full-cells with a thin SE layer (approximately 75-μm-thick). Pressurization at 75 MPa and use of graphite with lower expansion ratios improves capacity and capacity retentions. Increasing variation in the negative electrode volume increases charge-transfer resistance and crack formation in the NMC-composite layer. This indicates that the buffering effect via the elastic deformation of the thin SE layer is insufficient. Pressure facilitates plastic deformation of LixSi and SE, resulting in their improved contact, while perpendicular cracks appear throughout the Si-composite layer, effectively alleviating stress derived from variations in the volume of Si. This study provides important mechanistic insights into the design of advanced active materials and batteries required for industrial applications.

    DOI: 10.1016/j.jpowsour.2020.228595

    J-GLOBAL

  • First-Principles Calculation Study of Na<sup>+</sup>Superionic Conduction Mechanism in W- And Mo-Doped Na<inf>3</inf>SbS<inf>4</inf>Solid Electrolytes

    Randy Jalem, Akitoshi Hayashi, Fumika Tsuji, Atsushi Sakuda, Yoshitaka Tateyama

    Chemistry of Materials   32 ( 19 )   8373 - 8381   2020.10( ISSN:0897-4756

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    Publishing type:Research paper (scientific journal)  

    © 2020 American Chemical Society. The guiding principle for the design of inorganic compounds with high ionic conductivity has been extensively sought to realize next-generation all-solid-state batteries (ASSBs). Recently, a sulfide-type Na+ ion conductor, cubic Na3SbS4 with W doping (Na2.88Sb0.88W0.12S4), was reported with unprecedentedly high ionic conductivity of 3.2 × 10-2 S cm-1, making it now a champion solid electrolyte for Na-ASSB (A. Hayashi et al., Nat. Commun. 2019, 10, 5266). Herein, density functional theory molecular dynamics (DFT-MD) calculations were performed for pristine, W-doped, and Mo-doped Na3SbS4 to examine the ionic conduction mechanism (Boltzmann factor vs prefactor) and the aliovalent cation dopant effects in Na3SbS4. We showed that Na vacancies induced by cation doping play crucial roles in superionic conductivity, while the diffusion process is rather characterized by the concerted motion of Na+ ions. A comparison between the two dopants, Mo6+ and W6+, revealed that the conductivity enhancement can be primarily explained by a decrease of Na+ ion activation energy, which is found to be strongly correlated to the enlargement of Na Wyckoff site cages brought upon by the smaller WS4/MoS4 tetrahedral volume relative to the host SbS4 volume. This descriptor of the pathway free volume can suggest a general guiding principle for superionic conduction that can be applied to other cations, in addition to explaining the superior performance of W-doped Na3SbS4.

    DOI: 10.1021/acs.chemmater.0c02318

  • Synthesis of Sulfide Solid Electrolytes through the Liquid Phase: Optimization of the Preparation Conditions

    Kentaro Yamamoto, Masakuni Takahashi, Koji Ohara, Nguyen Huu Huy Phuc, Seunghoon Yang, Toshiki Watanabe, Tomoki Uchiyama, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago, Hiroyuki Muto, Atsunori Matsuda, Yoshiharu Uchimoto

    ACS Omega   5 ( 40 )   26287 - 26294   2020.10

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    Publishing type:Research paper (scientific journal)  

    All-solid-state lithium batteries using inorganic sulfide solid electrolytes have good safety properties and high rate capabilities as expected for a next-generation battery. Presently, conventional preparation methods such as mechanical milling and/or solid-phase synthesis need a long time to provide a small amount of the product, and they have difficult in supplying a sufficient amount to meet the demand. Hence, liquid-phase synthesis methods have been developed for large-scale synthesis. However, the ionic conductivity of sulfide solid electrolytes prepared via liquid-phase synthesis is typically lower than that prepared via solid-phase synthesis. In this study, we have controlled three factors: (1) shaking time, (2) annealing temperature, and (3) annealing time. The factors influencing lithium ionic conductivity of Li3PS4 prepared via liquid-phase synthesis were quantitatively evaluated using high-energy X-ray diffraction (XRD) measurement coupled with pair distribution function (PDF) analysis. It was revealed from PDF analysis that the amount of Li2S that cannot be detected by Raman spectroscopy or XRD decreased the ionic conductivity. Furthermore, it was revealed that the ionic conductivity of Li3PS4 is dominated by other parameters, such as remaining solvent in the sample and high crystallinity of the sample.

    DOI: 10.1021/acsomega.0c04307

  • Preparation of Sodium-Ion-Conductive Na3-xSbS4-xClx Solid Electrolytes Reviewed

    F. Tsuji, S. Yubuchi, A. Sakuda, M. Tatsumisago and A. Hayashi

    J. Ceram. Soc. Jpn. 雑誌   128 ( 9 )   641 - 647   2020.09

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    Kind of work:Joint Work  

  • Synthesis of Sulfide Solid Electrolytes through the Liquid Phase: Optimization of the Preparation Conditions Reviewed

    K. Yamamoto, M. Takahashi, K. Ohara, N. H. H. Phuc, S. H. Yang, T. Watanabe, T. Uchiyama, A. Sakuda, A. Hayashi, M. Tatsumisago, H. Muto, A. Matsuda and Y. Uchimoto

    ACS Omega 雑誌   5   26287 - 26294   2020.09

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    Kind of work:Joint Work  

  • First-Principles Calculation Study of Na+ Superionic Conduction Mechanism in W- and Mo-Doped Na3SbS4 Solid Electrolytes Reviewed

    R. Jalem, A. Hayashi, F. Tsuji, A. Sakuda and Y. Tateyama

    Chem. Mater. 雑誌   32   8373 - 8381   2020.09

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    Kind of work:Joint Work  

  • Preparation and Characterization of Composite Quasi-Solid Electrolytes Composed of 75Li2S・25P2S5 Glass and Phosphate Esters Reviewed

    K. Shimamoto, A. Sakuda, M. Tatsumisago and A. Hayashi

    J. Power Sources 雑誌   479 ( 228826 )   1 - 6   2020.09

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    Kind of work:Joint Work  

  • Characterization of Quasi-Solid Electrolytes Based on Li3PS4 Glass with Organic Carbonate Additives Reviewed

    K. Shimamoto, A. Sakuda, A. Hayashi and M. Tatsumisago

    J. Ceram. Soc. Jpn. 雑誌   128 ( 9 )   653 - 655   2020.09

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  • Characterization of quasi-solid electrolytes based on Li<inf>3</inf>PS<inf>4</inf>glass with organic carbonate additives

    Kei Shimamoto, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago

    Journal of the Ceramic Society of Japan   128 ( 9 )   653 - 655   2020.09( ISSN:1882-0743

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    Publishing type:Research paper (scientific journal)  

    ©2020 The Ceramic Society of Japan. All rights reserved. Composite quasi-solid electrolytes comprising Li3PS4 (LPS) glass and various organic carbonates were prepared, and the effects of these carbonates on the glass were investigated. Compared to LPS glass, the conductivity decreased for composites with highly dielectric cyclic carbonates and increased slightly for composites with a poorly dielectric linear carbonate. Scanning electron microscopy observations indicated that the addition of a poorly dielectric linear carbonate slightly improved the formability of LPS glass.

    DOI: 10.2109/jcersj2.20114

  • Preparation of sodium-ion-conductive Na<inf>3-x</inf>SbS<inf>4-x</inf>Cl<inf>x</inf>solid electrolytes

    Fumika Tsuji, So Yubuchi, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    Journal of the Ceramic Society of Japan   128 ( 9 )   641 - 647   2020.09( ISSN:1882-0743

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    Publishing type:Research paper (scientific journal)  

    © 2020 Ceramic Society of Japan. All rights reserved. Solid electrolytes have become important materials for improving the performance of next-generation all-solidstate sodium rechargeable batteries. Therefore, sodium vacancy doping for Na3SbS4electrolytes was performed by partially substituting Cl for S. Na3-xSbS4-xClxelectrolytes were prepared using a mechanochemical process and consecutive heat treatment. The structures, ionic conductivities, and air safety of the prepared Na3-x- SbS4-xCxl electrolytes were evaluated via X-ray diffraction and impedance, air stability, and electrochemical tests. The Na2.9375SbS3.9375Cl0.0625electrolyte showed a higher room-temperature ionic conductivity of 2.9 × 10-3Scm-1than that of the Na3SbS4electrolyte. An all-solid-state Na15Sn4/Na2.9375SbS3.9375Cl0.0625/TiS2cell showed a reversible capacity of approximately 100mAh g-1at room temperature. Thus, the Na2.9375SbS3.9375Cl0.0625solid electrolyte has the potential for application as a solid electrolyte in all-solid-state batteries.

    DOI: 10.2109/jcersj2.20089

  • Quasi-Solid Electrolytes Comprising Sulfide Electrolyte and Carboxylate Esters: Investigation of the Influence of the Carboxylate Ester Structure Reviewed

    K. Shimamoto, A. Sakuda, M. Tatsumisago and A. Hayashi

    J. Electrochem. Soc. 雑誌   167 ( 120521 )   1 - 6   2020.08

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  • Exothermal Behavior and Microstructure of a LiNi1/3Mn1/3Co1/3O2 Electrode Layer Using a Li4SnS4 Solid Electrolyte Reviewed

    H. Tsukasaki, M. Otoyama, T. Kimura, S. Mori, A. Sakuda, A. Hayashi and M. Tatsumisago

    J. Power Sources 雑誌   479 ( 228827 )   1 - 7   2020.08

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  • Sulfide Electrolyte Suppressing Side Reactions in Composite Positive Electrodes for All-Solid-State Lithium Batteries

    Misae Otoyama, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    ACS Applied Materials and Interfaces   12 ( 26 )   29228 - 29234   2020.07( ISSN:1944-8244

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    © 2020 American Chemical Society. Long-lasting all-solid-state batteries can be achieved by preventing side reactions in the composite electrodes comprising electrode active materials and solid electrolytes. Typically, the battery performance can be enhanced through the use of robust solid electrolytes that are resistant to oxidation and decomposition. In this study, the thermal stability of sulfide solid electrolytes Li3PS4 and Li4SnS4 toward oxide positive electrode active materials was estimated by investigating the occurrence of side reactions at the electrolyte-electrode interfaces when the composite electrodes are heated in an accelerated aging test: Li4SnS4 showed higher thermal stability because of the suppression of the substitution reaction between S and O. Moreover, thermally stable sulfide solid electrolytes are amenable to an improved cell construction process. The sintering (pelletizing and subsequent heating) of the composite electrodes with Li4SnS4 as the solid electrolyte allowed the manufacture of dense electrodes that exhibited increased ionic conductivity, thereby enhancing the battery performance.

    DOI: 10.1021/acsami.0c05050

    PubMed

  • Effects of Volume Variations under Different Compressive Pressures on the Performance and Microstructure of All-Solid-State Batteries Reviewed

    M. Yamamoto, Y. Terauchi, A. Sakuda, A. Kato and M. Takahashi

    J. Power Sources 雑誌   473 ( 228595 )   1 - 10   2020.07

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  • All-solid-state sodium-sulfur battery showing full capacity with activated carbon MSP20-sulfur-Na<inf>3</inf>SbS<inf>4</inf> composite

    Taka Ando, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    Electrochemistry Communications   116   2020.07( ISSN:1388-2481

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    © 2020 The Authors The need for an effective design of composite electrodes in all-solid-state Na-S batteries is warranted because of their slow charge–discharge reactions. By employing a composite of activated carbon MSP20, sulfur, and Na3SbS4 as the positive electrode material, we developed an effective all-solid-state Na-S battery that demonstrated the advantages of exhibiting a high capacity and good cyclability. Further, we discovered that filling the carbon micropores with sulfur and combining with highly conductive Na3SbS4, results in a reversible two-electron reaction between S and Na2S. This all-solid-state Na-S battery, operating at room temperature, demonstrates a high capacity of 1560 mAh per gram of sulfur (ca. 330 mAh per gram of positive electrode) and a capacity retention of 93% after 50 cycles. Decreasing the size of the S-MSP20 particles coated with Na3SbS4 in a liquid phase process was observed to reduce the volume change of the particles during charge and discharge cycles, which resulted in an excellent electrochemical performance.

    DOI: 10.1016/j.elecom.2020.106741

  • Elucidation of Capacity Degradation for Graphite in Sulfide-Based All-Solid-State Lithium Batteries: A Void Formation Mechanism

    Kentaro Kuratani, Atsushi Sakuda, Tomonari Takeuchi, Hironori Kobayashi

    ACS Applied Energy Materials   3 ( 6 )   5472 - 5478   2020.06

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    Capacity degradation mechanism of graphite in sulfide-based all-solid-state lithium batteries has been investigated by adopting three different press conditions for cell assembling. Reversible redox reaction and stage transition of graphite were recognized from cyclic voltammetry and X-ray diffraction measurement. Initial charge and discharge capacity of graphite in the thus obtained three cells were ca. 310 and 270 mAh g-1, respectively, indicating that the press conditions did not affect the initial charge and discharge capacity of graphite. After 50 cycles, the cell pressed at the highest pressure maintained over 95% of the capacity of that obtained at the 10th cycle. The capacity of the cell pressed at the lowest pressure, on the other hand, faded near 90%. The increase of resistance assigned to bulk solid electrolyte during cycling was detected by the impedance spectroscopy, and the cell pressed at the lowest pressure exhibited the largest resistance increase among all of the cells. Cross-sectional scanning electron microscope observation revealed formation of the voids in the bulk solid electrolyte, especially in the cell pressed at the lowest pressure, after 50 cycles, which resulted in the increase of the resistance for bulk solid electrolyte and capacity degradation of graphite.

    DOI: 10.1021/acsaem.0c00460

  • Reaction uniformity visualized by Raman imaging in the composite electrode layers of all-solid-state lithium batteries

    Misae Otoyama, Yusuke Ito, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    Physical Chemistry Chemical Physics   22 ( 23 )   13271 - 13276   2020.06( ISSN:1463-9076

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    © the Owner Societies. The reaction uniformity of LiCoO2 composite positive electrodes in all-solid-state cells was compared quantitatively by investigating the Raman band shifts corresponding to the state-of-charge (SOC) of LiCoO2. The quantitative SOC analysis was conducted using the Raman imaging data of composite electrodes with smaller or larger solid electrolytes. The electrodes exhibited different reaction uniformity although the cells showed similar initial charge capacities and average SOC. In the case of larger solid electrolytes, most LiCoO2 particles showed higher or lower SOC than the average SOC, and lower battery performance. The quantitative analysis of SOC in each LiCoO2 electrode demonstrated that a variable SOC outside the average SOC resulted in larger irreversible capacity and lower rate performance. The quantitative SOC analysis newly developed in the present study is a useful technique for designing composite electrodes showing higher battery performance.

    DOI: 10.1039/d0cp00508h

    PubMed

  • Sulfide Electrolyte Suppressing Side Reactions in Composite Positive Electrodes for All-Solid-State Lithium Batteries Reviewed

    M. Otoyama, A. Sakuda, M. Tatsumisago and A. Hayashi

    ACS Appl. Mater. Interfaces 雑誌   12   29228 - 29234   2020.06

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  • A Reversible Oxygen Redox Reaction in Bulk-type All-Solid-State Batteries Reviewed

    K. Nagao, Y. Nagata, A. Sakuda, A. Hayashi, M. Deguchi, C. Hotehama, H. Tsukasaki, S. Mori, Y. Orikasa, K. Yamamoto, Y. Uchimoto and M. Tatsumisago

    Sci. Adv. 雑誌   6 ( (eaax7236) )   1 - 11   2020.06

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  • A reversible oxygen redox reaction in bulk-type all-solid-state batteries Reviewed

    Kenji Nagao, Yuka Nagata, Atsushi Sakuda, Akitoshi Hayashi, Minako Deguchi, Chie Hotehama, Hirofumi Tsukasaki, Shigeo Mori, Yuki Orikasa, Kentaro Yamamoto, Yoshiharu Uchimoto, Masahiro Tatsumisago

    Science Advances   6 ( 25 )   eaax7236 - eaax7236   2020.06

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    An all-solid-state lithium battery using inorganic solid electrolytes requires safety assurance and improved energy density, both of which are issues in large-scale applications of lithium-ion batteries. Utilization of high-capacity lithium-excess electrode materials is effective for the further increase in energy density. However, they have never been applied to all-solid-state batteries. Operational difficulty of all-solid-state batteries using them generally lies in the construction of the electrode-electrolyte interface. By the amorphization of Li<sub>2</sub>RuO<sub>3</sub> as a lithium-excess model material with Li<sub>2</sub>SO<sub>4</sub>, here, we have first demonstrated a reversible oxygen redox reaction in all-solid-state batteries. Amorphous nature of the Li<sub>2</sub>RuO<sub>3</sub>-Li<sub>2</sub>SO<sub>4</sub> matrix enables inclusion of active material with high conductivity and ductility for achieving favorable interfaces with charge transfer capabilities, leading to the stable operation of all-solid-state batteries.

    DOI: 10.1126/sciadv.aax7236

    PubMed

  • Reaction Uniformity Visualized by Raman Imaging in the Composite Electrode Layers of All-Solid-State Lithium Batteries Reviewed

    M. Otoyama, Y. Ito, A. Sakuda, M. Tatsumisago and A. Hayashi

    Phys. Chem. Chem. Phys. 雑誌   22   13271 - 13276   2020.05

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    Kind of work:Joint Work  

  • Elucidation of Capacity Degradation for Graphite in Sulfide-Based All-Solid-State Lithium Batteries: A Void Formation Mechanism Reviewed

    K. Kuratani, A. Sakuda, T. Takeuchi and H. Kobayashi

    ACS Appl. Energy Mater. 雑誌   3   5472 - 5478   2020.05

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  • All-Solid-State Sodium-Sulfur Battery Showing Full Capacity with Activated Carbon MSP20-Sulfur-Na3SbS4 Composite Reviewed

    T. Ando, A. Sakuda, M. Tatsumisago and A. Hayashi

    Electrochemistry Communications 雑誌   116 ( 106741 )   1 - 5   2020.05

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  • High-rate operation of sulfur/mesoporous activated carbon composite electrode for all-solid-state lithium-sulfur batteries

    Taka Ando, Yuta Sato, Takuya Matsuyama, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    Journal of the Ceramic Society of Japan   128 ( 5 )   233 - 237   2020.05( ISSN:1882-0743

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    Publishing type:Research paper (scientific journal)  

    ©2020 The Ceramic Society of Japan. All rights reserved. All-solid-state lithium-sulfur batteries are promising from the perspective of high safety, low cost, and high capability. Herein, composites of sulfur and microporous carbon (MSP20, MSC30) are prepared by a melt diffusion process, and their performance as electrode materials are compared with that of composites based on nanocarbons. In addition to the type of carbon, the degree of mixing with solid electrolytes is an important factor in the formation of ionic/electronic conduction pathways. The all-solid-state cell using S-MSC30-Li3PS4 shows a high initial discharge capacity of 1488 mAh per gram of sulfur at 25 °C at a current density of 1.3 mA cm12 and operates reversibly at a high current density of 12.7 mA cm12 (3C) at 100 °C. The amorphization of sulfur is effective for obtaining high capacity and sulfur impregnated into the meso- and micropores of carbon is more active than sulfur that forms nanocom osites with nanocarbon

    DOI: 10.2109/jcersj2.20003

  • High-Rate Operation of Sulfur/Mesoporous Activated Carbon Composite Electrode for All-Solid-State Lithium-Sulfur Batteries Reviewed

    T. Ando, Y. Sato, T. Matsuyama, A. Sakuda, M. Tatsumisago and A. Hayashi

    J. Ceram. Soc. Jpn. 雑誌   128 ( 5 )   233 - 237   2020.04

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  • How Certain Are the Reported Ionic Conductivities of Thiophosphate-Based Solid Electrolytes? An Interlaboratory Study

    Saneyuki Ohno, Tim Bernges, Johannes Buchheim, Marc Duchardt, Anna Katharina Hatz, Marvin A. Kraft, Hiram Kwak, Aggunda L. Santhosha, Zhantao Liu, Nicolò Minafra, Fumika Tsuji, Atsushi Sakuda, Roman Schlem, Shan Xiong, Zhenggang Zhang, Philipp Adelhelm, Hailong Chen, Akitoshi Hayashi, Yoon Seok Jung, Bettina V. Lotsch, Bernhard Roling, Nella M. Vargas-Barbosa, Wolfgang G. Zeier

    ACS Energy Letters   5 ( 3 )   910 - 915   2020.03

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  • Operando Confocal Microscopy for Dynamic Changes of Li<sup>+</sup> Ion Conduction Path in Graphite Electrode Layers of All-Solid-State Batteries

    Misae Otoyama, Hiroe Kowada, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    Journal of Physical Chemistry Letters   11 ( 3 )   900 - 904   2020.02

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    Copyright © 2020 American Chemical Society. The dynamic changes of ionic conduction path in the cross-sectional graphite composite electrodes of bulk-type all-solid-state lithium batteries have been monitored using operando confocal microscopic observations for color changes of graphite in response to their stage structures. The ionic conduction path decreased in the cross-sectional direction as cycle numbers increased, with simultaneous capacity degradation. The local reactivity of lithiation and delithiation was evaluated by image analysis considering state-of-charge (SOC) values. Electrode thickness changes were examined from the confocal microscope images obtained in the operando observations. The results revealed that voids and cracks were formed during cycle tests and that the thickness gradually increased. These cracks and voids were one of the main contributors to the limitation of ionic conduction paths in the depth direction. Operando microscopic observation and subsequent image analysis elucidated not only the morphological changes of active materials but also the differences in local SOC changes in the electrode.

    DOI: 10.1021/acs.jpclett.9b03456

    PubMed

  • Dry coating of active material particles with sulfide solid electrolytes for an all-solid-state lithium battery Reviewed

    Hideya Nakamura, Takashi Kawaguchi, Tomoyuki Masuyama, Atsushi Sakuda, Toshiya Saito, Kentaro Kuratani, Shuji Ohsaki, Satoru Watano

    Journal of Power Sources   448   2020.02( ISSN:0378-7753

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    © 2019 Elsevier B.V. In this study, we present a dry coating process to produce a core-shell composite particle for an all-solid-state lithium battery, where a single particle of the active material is coated with solid electrolytes. LiNi1/3Co1/3Mn1/3O2 (NCM) and Li3PS4 (LPS), which are typical cathode active material and sulfide solid electrolyte, were used. A dry impact-blending device was employed for the dry coating process. We demonstrated that a single particle of NCM was uniformly coated with a continuous layer of LPS by the dry coating process without any breakage or attrition of NCM, to produce an NCM@LPS core-shell particle. The charge-discharge cycling tests showed that the rate and cycle performances of an all-solid-state half-cell prepared with the NCM@LPS core-shell particles significantly improved. The three-dimensional internal structure of the composite cathode was subsequently analyzed using FIB-SEM with an image reconstruction technique. The results revealed that the composite cathode prepared with the NCM@LPS core-shell particles had a (i) high interfacial contact area between NCM and LPS and (ii) well-percolated ion transport pathway. In conclusion, the core-shell composite particle contributed to the structure of the composite cathode, thus resulting in improved cell performance.

    DOI: 10.1016/j.jpowsour.2019.227579

  • How Certain Are the Reported Ionic Conductivities of Thiophosphate-Based Solid Electrolytes? An Interlaboratory Study Reviewed

    S. Ohno, T. Bernges, J. Buchheim, M. Duchardt, A.-K. Hatz, M. A. Kraft, H. Kwak, A. L. Santhosha, Z. Liu, N. Minafra, F. Tsuji, A. Sakuda, R. Schlem, S. Xiong, Z. Zhang, P. Adelhelm, H. Chen, A. Hayashi, Y. S. Jung, B. V. Lotsch, B. Roling, N. M. Vergas-Barbosa, W. G. Zeier

    ACS Energy Lett. 雑誌   5   910 - 915   2020.02

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  • Aqueous Solution Synthesis of Na3SbS4-Na2WS4 Superionic Conductors Reviewed

    S. Yubuchi, A. Ito, N. Masuzawa, A. Sakuda, A. Hayashi and M. Tatsumisago

    J. Mater. Chem. A. 雑誌   8   1947 - 1954   2020.02

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  • Quasi-Solid Electrolytes Comprising Sulfide Electrolyte and Carboxylate Esters: Investigation of the Influence of the Carboxylate Ester Structure

    Kei Shimamoto, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi

    Journal of the Electrochemical Society   167 ( 12 )   2020.01( ISSN:0013-4651

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    © 2020 The Electrochemical Society ("ECS"). Published on behalf of ECS by IOP Publishing Limited. Composite quasi-solid electrolytes composed of Li3PS4 (LPS) glass and a carboxylate ester were prepared via planetary ball milling, and the influence of the molecular structure of the carboxylate esters on their ion-conduction was investigated. The results revealed that filling the voids in the solid electrolyte with a bulky carboxylate ester, which hardly reacted with the LPS glass, effectively maintains the high ionic conductivity of the LPS glass even when the relative density of LPS decreases. The use of this composite quasi-solid electrolyte is an effective approach to maintain the ion-conduction in not only an electrolyte separator layer but also a composite electrode layer in an all-solid-state battery.

    DOI: 10.1149/1945-7111/abacec

  • Operando Confocal Microscopy for Dynamic Changes of Li+ Ion Conduction Path in Graphite Electrode Layers of All-Solid-State Batteries Reviewed

    M. Otoyama, H. Kowada, A. Sakuda, M. Tatsumisago and A. Hayashi

    J. Phys. Chem. Lett. 雑誌   11   900 - 904   2020.01

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  • Dry Coating of Active Material Particles with Sulfide Solid Electrolytes for an All-Solid-State Lithium Battery Reviewed

    H. Nakamura, T. Kawaguchi, T. Masuyama, A. Sakuda, T. Saito, K. Kuratani, S. Ohsaki, S. Watano

    J. Power Sources 雑誌   448 ( 227579 )   1 - 10   2020.01

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  • Electrode performance of amorphous MoS<sub>3</sub> in all-solid-state sodium secondary batteries

    城田岳, 奈須滉, 出口三奈子, 作田敦, 辰巳砂昌弘, 林晃敏

    電池討論会PDF要旨集(CD-ROM)   61st   2020

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    All-solid-state Na–S secondary batteries that use sodium and sulfur, both available in abundance, are the most attractive next-generation batteries. In this study, two types of amorphous MoS3 (a-MoS3) were prepared as electrode active materials for use in all-solid-state sodium secondary batteries using the thermal decomposition (TD) of (NH4)2MoS4 and mechanochemical (MC) processes, denoted a-MoS3 (TD) and a-MoS3 (MC), respectively. X-ray diffraction, thermogravimetric-differential thermal analysis, and X-ray photoelectron spectroscopy (XPS) analyses revealed that a-MoS3 (TD) and a-MoS3 (MC) had different local structures. The a-MoS3 (TD) and a-MoS3 (MC) electrodes showed high reversible capacities of 310 mAh g−1 and 260 mAh g−1, respectively, for five cycles in all-solid-state sodium secondary batteries. XPS analysis of the discharge–charge products suggested that the dissociation and formation of disulfide bonds occurred during the discharge–charge reaction. The results show that a-MoS3 is a promising active electrode material for all-solid-state sodium batteries.

    DOI: 10.1016/j.powera.2021.100061

    J-GLOBAL

  • Preparation and characterization of sodium ion conductive Na<sub>3</sub>BS<sub>3</sub> glass electrolyte

    辻史香, 奈須滉, 作田敦, 辰巳砂昌弘, 林晃敏, 林晃敏

    電池討論会PDF要旨集(CD-ROM)   61st ( 5 )   1676 - 1682   2020

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    In order to find suitable solid electrolytes for all-solid-state sodium batteries, sulfide electrolytes composed of tetrahedral structural units such as PS4, SnS4 and SbS4 have been widely studied. In this paper, the ionic conductivities of Na3BS3ortho-thioborate electrolytes with triangular BS3 units are firstly reported. Na3BS3 glass was prepared via a mechanochemical process from crystalline Na3BS3 (monoclinic phase). The crystalline Na3BS3 was pre-synthesized from a mixture of Na2S, B, and S due to the instability of the B2S3 compound. A new metastable phase of trigonal Na3BS3 was precipitated as the primary phase by crystallization of the Na3BS3 glass. The prepared glass-ceramic electrolyte showed a higher ionic conductivity than the monoclinic Na3BS3 phase. The Na3BS3 glass showed the highest conductivity of 1.1 × 10-5 S cm-1, which was higher than that of conventional Na3PS4 glass. Futhermore, the Na3BS3 glass showed a superior formability and electrochemical stability to Na15Sn4 negative electrode. An all-solid-state cell with the Na3BS3 glass as an electrolyte successfully operated as a secondary battery at 60 °C. It is concluded that the Na3BS3 glass with triangular structural units has appropriate properties as a solid electrolyte for application to all-solid-state sodium batteries. The results of this study extend research on multi-component sulfide electrolytes with triangular BS3 structural units and contribute to the development of solid electrolytes for all-solid-state batteries. This journal is

    DOI: 10.1039/d0ma00777c

    J-GLOBAL

  • Aqueous solution synthesis of Na<inf>3</inf>SbS<inf>4</inf>-Na<inf>2</inf>WS<inf>4</inf> superionic conductors

    So Yubuchi, Akane Ito, Naoki Masuzawa, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago

    Journal of Materials Chemistry A   8 ( 4 )   1947 - 1954   2020( ISSN:2050-7488

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    © The Royal Society of Chemistry. We report a route for the synthesis of Na3SbS4-Na2WS4 superionic conductors from aqueous solution. Na3SbS4-Na2WS4 has the highest high sodium-ion conductivity (4.28 mS cm-1 at 25 °C) of reported sulfide-based solid electrolytes prepared via liquid-phase methods. The antimony in Na3SbS4 is replaced by tungsten in a higher valence state, which is charge-compensated by sodium vacancies in the form Na3-xSb1-xWxS4. Introducing sodium vacancies while maintaining the 3D conduction pathways increases the pre-exponential factor in the Arrhenius plots of ionic conduction. The development of a facile synthetic protocol, as well as the high ionic conductivity and excellent chemical stability of Na3SbS4-Na2WS4 in the presence of water, is a major step towards the realization of all-solid-state sodium batteries.

    DOI: 10.1039/c9ta02246e

  • A sodium-ion sulfide solid electrolyte with unprecedented conductivity at room temperature

    A. Hayashi, N. Masuzawa, S. Yubuchi, F. Tsuji, C. Hotehama, A. Sakuda, M. Tatsumisago

    Nature Communications   10 ( 1 )   2019.12

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    Solid electrolytes are key materials to enable solid-state rechargeable batteries, a promising technology that could address the safety and energy density issues. Here, we report a sulfide sodium-ion conductor, Na2.88Sb0.88W0.12S4, with conductivity superior to that of the benchmark electrolyte, Li10GeP2S12. Partial substitution of antimony in Na3SbS4 with tungsten introduces sodium vacancies and tetragonal to cubic phase transition, giving rise to the highest room-temperature conductivity of 32 mS cm−1 for a sintered body, Na2.88Sb0.88W0.12S4. Moreover, this sulfide possesses additional advantages including stability against humid atmosphere and densification at much lower sintering temperatures than those (>1000 °C) of typical oxide sodium-ion conductors. The discovery of the fast sodium-ion conductors boosts the ongoing research for solid-state rechargeable battery technology with high safety, cost-effectiveness, large energy and power densities.

    DOI: 10.1038/s41467-019-13178-2

    PubMed

    Other URL: http://www.nature.com/articles/s41467-019-13178-2

  • Sulfur-Based Composite Electrode with Interconnected Mesoporous Carbon for All-Solid-State Lithium–Sulfur Batteries Reviewed

    Atsushi Sakuda, Yuta Sato, Akitoshi Hayashi, Masahiro Tatsumisago

    Energy Technology   7 ( 12 )   1 - 5   2019.12( ISSN:2194-4288

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    Authorship:Lead author   Publishing type:Research paper (scientific journal)  

    © 2019 WILEY-VCH Verlag GmbH &amp; Co. KGaA, Weinheim All-solid-state lithium–sulfur batteries have attracted much attention because of their large capacity and long life. However, their rate capability is not sufficiently high, prompting a great demand for improvement. Herein, a sulfur-based composite electrode is fabricated for the high-rate operation of all-solid-state lithium–sulfur batteries. The electrode is made of a carbon material having a large number of “interconnected mesopores” with a diameter of 5 nm. The highly mesoporous structure is conducive to electrode reactions and the formation of conduction pathways. Consequently, the rate capability of the composite electrode is drastically improved compared with that of an electrode made of conventional conducting nanocarbon. The all-solid-state lithium–sulfur battery with this composite electrode shows a high capacity of 1100 mA h g −1 per sulfur after 400 cycles at a high current density of 1.3 mA cm −2 at 25 °C. These findings are expected to contribute toward the development of practical all-solid-state lithium–sulfur batteries.

    DOI: 10.1002/ente.201900077

  • Microstructure and conductivity of Al-substituted Li<inf>7</inf>La<inf>3</inf>Zr<inf>2</inf>O<inf>12</inf> ceramics with different grain sizes Reviewed

    Yuma Matsuki, Kousuke Noi, K. Suzuki, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago

    Solid State Ionics   342   2019.12( ISSN:0167-2738

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    © 2019 Elsevier B.V. Al-doped Li7La3Zr2O12 (LLZ) sintered ceramics with two grain sizes were prepared to investigate the relationship between their microstructure and conducting properties. The X-ray diffraction patterns showed no difference in the peak shift and intensity between the two prepared LLZ ceramics, suggesting that their bulk conductivities were almost the same. Scanning electron microscopy and energy dispersive X-ray spectrometry were used to observe their microstructure. Neither of the ceramics had an obvious impurity phase along grain boundaries. One of LLZ (LLZ_LG) had a larger grain size of 5–20 μm and showed intergranular fracture. The other LLZ (LLZ_SG) had a smaller grain size of primarily &lt;1 μm and showed intragranular fracture. LLZ_LG showed a total conductivity of 3.6 × 10−4 S cm−1 and an activation energy, Ea, for conduction of 32 kJ mol−1, while LLZ_SG showed conductivity of 4.4 × 10−4 S cm−1 and Ea of 26 kJ mol−1. It is noteworthy that the grain boundary composed of small grains showed lower grain boundary resistance than that composed of large grains. As a result, it is clarified that LLZ ceramics with higher ion-conductivity and lower Ea can be prepared by suppressing grain growth.

    DOI: 10.1016/j.ssi.2019.115047

  • Microstructure and Conductivity of Al-Substituted Li7La3Zr2O12 Ceramics with Different Grain Sizes Reviewed

    Y. Matsuki, K. Noi, K. Suzuki, A. Sakuda, A. Hayashi and M. Tatsumisago

    Solid State Ionics 雑誌   342 ( 115047 )   1 - 6   2019.12

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  • Sulfur-Based Comosite Electrode with Interconnected Mesoporous Carbon for All-Solid-State Lithium-Sulfur Batteries Reviewed

    A. Sakuda, Y. Sato, A. Hayashi and M. Tatsumisago

    Energy Technol. 雑誌   7 ( 1900077 )   1 - 5   2019.12

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  • A Sodium-ion Sulfide Solid Electrolyte with Unprecedented Conductivity at Room Temperature Reviewed

    A. Hayashi, N. Masuzawa, S. Yubuchi, F. Tsuji, C. Hotehama, A. Sakuda and M. Tatsumisago

    Nat. Commun. 雑誌   10:5266   1 - 6   2019.11

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  • New lithium-conducting nitride glass Li<inf>3</inf>BN<inf>2</inf> Reviewed

    Manari Shigeno, Kenji Nagao, Minako Deguchi, Chie Hotehama, Hiroe Kowada, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago

    Solid State Ionics   339   2019.10( ISSN:0167-2738

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    © 2019 Elsevier B.V. Novel nitride glass electrolyte Li3BN2 was prepared from Li3N and BN via a mechanochemical process using planetary ball milling. Raman and X-ray photoelectron spectroscopies revealed that the glass was composed of Li+ and BN23− ions. The Li3BN2 glass exhibited good ductility, and the powder-compressed pellet showed a relative density of 84%. The hot-pressed pellet of the Li3BN2 glass showed a conductivity of 1.3 × 10−5 S cm−1 at 25 °C, which is much higher than that of oxide-based glass electrolytes such as Li3BO3 glass and LiPON thin films. Moreover, Young&#039;s modulus of the Li3BN2 glass was 51.1 GPa, which is an intermediate value between sulfides and oxides. The Li symmetric cell using the Li3BN2 glass electrolyte was cycled stably at 100 °C without short-circuiting. Nitride glassy materials are promising electrolytes for all-solid-state batteries because of their high conductivity, good mechanical properties, and electrochemical stability.

    DOI: 10.1016/j.ssi.2019.05.020

  • Mechanochemical Synthesis and Characterization of Amorphous Li2CN2 as a Lithium Ion Conductor Reviewed

    T. Kimura, C. Hotehama, A. Sakuda, A. Hayashi and M. Tatsumisago

    J. Ceram. Soc. Jpn 雑誌   127 ( 8 )   518 - 520   2019.08

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  • Mechanochemical Synthesis of Na-Sb Alloy Negative Electrodes and their Application to All-Solid-State Sodium Batteries Reviewed

    T. Ando, S. Yubuchi, A. Sakuda, A. Hayashi and M. Tatsumisago

    Electrochemistry 雑誌   87 ( 5 )   289 - 293   2019.08

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  • Metastable Materials for All-Solid-State Batteries Reviewed

    A. Sakuda, A. Hayashi and M. Tatsumisago

    Electrochemistry 雑誌   87 ( 5 )   247 - 250   2019.08

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  • Mechanochemical Synthesis of Cubic Rocksalt Na3TiS3 as Novel Active Materials for All-Solid-State Sodium Secondary Batteries Reviewed

    A. Nasu, M. Otoyama, A. Sakuda, A. Hayashi and M. Tatsumisago

    J. Ceram. Soc. Jpn 雑誌   127 ( 8 )   514 - 517   2019.08

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  • Mechanochemical synthesis and characterization of amorphous Li<inf>2</inf>CN<inf>2</inf> as a lithium ion conductor Reviewed

    Takuya Kimura, Chie Hotehama, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago

    Journal of the Ceramic Society of Japan   127 ( 8 )   518 - 520   2019.08( ISSN:1882-0743

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    Drastically higher conductivity was found in the amorphous lithium-ion conducting nitride relative to the crystal. The amorphous Li2CN2 prepared by a mechanochemical process has the conductivity of 1.1 © 1016 S cm11 at 25°C, which is more than 1000 times higher than that of the crystalline form. The nitride has a better deformability compared to Li3BO3 oxide glass.

    DOI: 10.2109/jcersj2.19077

  • Mechanochemical synthesis of cubic rocksalt Na<inf>2</inf>TiS<inf>3</inf> as novel active materials for all-solid-state sodium secondary batteries Reviewed

    Akira Nasu, Misae Otoyama, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago

    Journal of the Ceramic Society of Japan   127 ( 8 )   514 - 517   2019.08( ISSN:1882-0743

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    Mechanochemical (MC) process is one of the most effective methods to produce amorphous and cation disordered electrode active materials. We individually synthesized amorphous and cation disordered cubic rocksalt Na2TiS3 by controlling the preparation conditions of the MC process. Cubic rocksalt Na2TiS3 and ordered monoclinic Na2TiS3 were also obtained via the heat treatment of amorphous Na2TiS3. The all-solid-state cell with cubic rocksalt Na2TiS3 showed a high reversible capacity of 270 mAh g11, which corresponds to the theoretical capacity of Na2TiS3. The cell maintained the capacity for more than 30 cycles, indicating that the active materials can endure long operation life. The MC methods for transition metal sulfides and the search for ordered monoclinic polymorphs are necessary for the pursuit of novel electrode materials.

    DOI: 10.2109/jcersj2.19086

  • Suspension synthesis of Na<inf>3-x</inf>PS<inf>4-x</inf>Cl<inf>x</inf> solid electrolytes Reviewed

    Miwa Uematsu, So Yubuchi, Fumika Tsuji, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago

    Journal of Power Sources   428   131 - 135   2019.07( ISSN:0378-7753

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    © 2019 Elsevier B.V. All-solid-state sodium batteries with sulfide-based solid electrolytes are attracting attention as next-generation energy storage systems to replace Li-ion batteries, owing to their improved safety and the abundant sodium resources. Na 3 PS 4 -based materials, which have relatively high conductivities and favorable mechanical properties, make promising Na-ion solid electrolytes for realizing all-solid-state sodium batteries. However, it is essential to establish a further simple and effective protocol for manufacturing such solid electrolytes and composite electrodes. In this study, Na 3-x PS 4-x Cl x (x = 0, 0.0625) was prepared by a liquid-phase (suspension) process from Na 2 S, P 2 S 5 , and NaCl using 1,2-dimethoxyethane as a reaction media. Na 3 PS 4 heated at 400 °C and Na 2.9375 PS 3.9375 Cl 0.0625 heated at 480 °C exhibited Na-ion conductivities of 2.6 × 10 −4 and 4.3 × 10 −4 S cm −1 at 25 °C, respectively. A homogenous composite electrode was prepared with TiS 2 active material and Na 3 PS 4 solid electrolyte via the simple liquid-phase process, resulting in large contact areas between electrode and electrolyte particles. The electrode obtained by liquid-phase provided an all-solid-state cell with higher reversible capacity of 161 mAh g −1 than a conventional mechanically mixed electrode. Suspension syntheses of Na 3-x PS 4-x Cl x are useful for the simple production of solid electrolytes and are highly applicable to all-solid-state sodium batteries.

    DOI: 10.1016/j.jpowsour.2019.04.069

  • Formation of interfacial contact with ductile Li<inf>3</inf>BO<inf>3</inf>-based electrolytes for improving cyclability in all-solid-state batteries Reviewed

    Kenji Nagao, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago

    Journal of Power Sources   424   215 - 219   2019.06( ISSN:0378-7753

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    © 2019 Elsevier B.V. Highly safe all-solid-state batteries are constructed using oxide electrolytes because of their high chemical and electrochemical stabilities. Previously, we have developed various Li 3 BO 3 -based glass-ceramic electrolytes with high ductility and conductivity. In this study, we focus on the importance of electrode/electrolyte interfacial contacts in all-solid-state batteries. All-oxide solid-state cells (Li-In/LiNi 1/3 Mn 1/3 Co 1/3 O 2 ) with Li 3 BO 3 -based glass-ceramic electrolytes, are fabricated simply by pressing at room temperature. Furthermore, the effects of the ductility and ionic conductivity of glass-ceramic electrolytes on the charge-discharge properties of all-solid-state batteries are investigated. The 33Li 3 BO 3 ·33Li 2 SO 4 ·33Li 2 CO 3 (mol%) glass-ceramic electrolyte shows lower ionic conductivity and better ductility than the 90Li 3 BO 3 ·10Li 2 SO 4 electrolyte. The all-solid-state cells using these electrolytes operate as secondary batteries at 100 °C. However, better cycle performance is obtained with cells using the former electrolyte. Formation of well-contacted electrode/electrolyte interfaces when using highly ductile electrolytes leads to enhanced electrochemical performance of bulk-type all-solid-state batteries.

    DOI: 10.1016/j.jpowsour.2019.03.083

  • Ion-exchange Synthesis of Li2NaPS4 from Na3PS4 Reviewed

    J. Chen, S. Yubuchi, C. Hotehama, A. Sakuda, A. Hayashi and M. Tatsumisago

    Chem. Lett. 雑誌   48   863 - 865   2019.06

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  • Amorphous Ni-Rich Li(Ni1-x-yMnxCoy)O2-Li2SO4 Positive Electrode Materials for Bulk-Type All-Oxide Solid-State Batteries Reviewed

    K. Nagao, A. Sakuda, A. Hayashi, H. Tsukasaki, S. Mori and M. Tatsumisago

    Adv. Mater. Interfaces 雑誌   6 ( 1802016 )   1 - 10   2019.06

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  • Highly Stable Li/Li<inf>3</inf>BO<inf>3</inf>-Li<inf>2</inf>SO<inf>4</inf> Interface and Application to Bulk-Type All-Solid-State Lithium Metal Batteries Reviewed

    Kenji Nagao, Motoshi Suyama, Atsutaka Kato, Chie Hotehama, Minako Deguchi, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago

    ACS Applied Energy Materials   2 ( 5 )   3042 - 3048   2019.05( ISSN:2574-0962

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    © 2019 American Chemical Society. All-solid-state batteries (ASSBs) are potentially safe energy storage devices. The 90Li3BO3·10Li2SO4 (mol %) glass-ceramic is one of the promising oxide electrolytes due to its high ductility and ionic conductivity. Utilization of Li metal negative electrode enhances the energy density of ASSBs. Herein, the high electrochemical stability of the 90Li3BO3·10Li2SO4 electrolyte against Li metal negative electrode was demonstrated. The symmetric cells using a dense electrolyte body with relative density of 99% synthesized by the hot-pressing technique showed excellent cycle performance for the Li dissolution and deposition reactions. Finally, the all-solid-state (Li/80LiNi0.5Mn0.3Co0.2O2·20Li2SO4) full cell operated as a secondary battery at 100 °C.

    DOI: 10.1021/acsaem.9b00470

  • Preparation and characterization of lithium ion conductive Li <inf>3</inf> SbS <inf>4</inf> glass and glass-ceramic electrolytes Reviewed

    Takuya Kimura, Atsutaka Kato, Chie Hotehama, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago

    Solid State Ionics   333   45 - 49   2019.05( ISSN:0167-2738

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    © 2019 Elsevier B.V. Li 3 SbS 4 glass was prepared by a mechanochemical process and a glass-ceramic was prepared by heating the glass above the crystallization temperature. The glass-ceramic had a crystal structure similar to that of γ-Li 3 PS 4 . As indicated by the Raman spectra, both electrolytes contained an SbS 4 unit. The conductivity of the pelletized Li 3 SbS 4 glass was 1.5 × 10 −6 S·cm −1 at 25 °C, which was higher than that of its glass-ceramic. The amount of H 2 S generated from Li 3 SbS 4 glass in humid air was considerably lower than that from the Li 3 PS 4 glass.

    DOI: 10.1016/j.ssi.2019.01.017

  • Suspension Synthesis of Na3-xPS4-xClx Solid Electrolytes Reviewed

    M. Uematsu, S. Yubuchi, F. Tsuji, A. Sakuda, A. Hayashi and M. Tatsumisago

    J. Power Sources 雑誌   428   131 - 135   2019.05

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  • Highly Stable Li/Li3BO3-Li2SO4 Interface and Application to Bulk-Type All-Solid-State Lithium Metal Batteries Reviewed

    K. Nagao, M. Suyama, A. Kato, C. Hotehama, M. Deguchi, A. Sakuda, A. Hayashi and M. Tatsumisago

    ACS Appl. Energy Mater. 雑誌   2   3042 - 3048   2019.05

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  • New Lithium-Conducting Nitride Glass Li3BN2 Reviewed

    M. Shigeno, K. Nagao, M. Deguchi, C. Hotehama, H. Kowada, A. Sakuda, A. Hayashi and M. Tatsumisago

    Solid State Ionics 雑誌   339   2019.05

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  • Morphological Effect of Reaction Distribution Influenced by Binder Materials in Composite Electodes for Sheet-type All-Solid-State Lithium-Ion Batteries with the Sulfide-based Solid Electrolyte Reviewed

    K. Chen, S. Shinjo, A. Sakuda, K. Yamamoto, T. Uchiyama, K. Kuratani, T. Kakeuchi, Y. Orikasa, A. Hayashi, M. Tatsumisago, Y. Kimura, T. Nakamura, K. Amezawa and Y. Uchimoto

    J. Phys. Chem. C 雑誌   123   3292 - 3298   2019.05

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  • Quantitative Analysis of Crystallinity in an Argyrodite Sulfide-based Solid Electrolyte Synthesized Via Solution Processing Reviewed

    S. Yubuchi, H. Tsukasaki, A. Sakuda, S. Mori, A. Hayashi and M. Tatsumisago

    RSC Adv. 雑誌   9   14465 - 14471   2019.05

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  • Formation of Interfacial Contact with Ductile Li3BO3-based Electrolytes for Improving Cyclability in All-Solid-State Batteries Reviewed

    K. Nagao, A. Sakuda, A. Hayashi and M. Tatsumisago

    J. Power Sources 雑誌   424   215 - 219   2019.04

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  • Amorphous Ni-Rich Li(Ni <inf>1−</inf><inf>x</inf><inf>−</inf><inf>y</inf> Mn <inf>x</inf> Co <inf>y</inf> )O <inf>2</inf> –Li <inf>2</inf> SO <inf>4</inf> Positive Electrode Materials for Bulk-Type All-Oxide Solid-State Batteries Reviewed

    Kenji Nagao, Atsushi Sakuda, Akitoshi Hayashi, Hirofumi Tsukasaki, Shigeo Mori, Masahiro Tatsumisago

    Advanced Materials Interfaces   6 ( 8 )   2019.04( ISSN:2196-7350

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    © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim All-solid-state batteries attract significant attention owing to their potential to realize an energy storage system with high safety and energy density. In this paper, a mechanochemical synthesis of novel amorphous positive electrode materials of the Ni-rich LiNi 1−x−y Mn x Co y O 2 (NMC)–Li 2 SO 4 system suitable for oxide-type all-solid-state batteries is reported. Through the mechanochemical treatment with Li 2 SO 4 , excellent formabilities of the electrode materials as those of ductile solid electrolytes are obtained. Owing to the deformability of the active material, a good electrode/electrolyte interface is provided simply by pressing at room temperature. In all-oxide solid-state cells using 80NMCs·20Li 2 SO 4 (mol%) positive electrode materials, the cell capacity increases with the Ni content in the NMC. The all-solid-state cell using the 80NMC811·20Li 2 SO 4 positive electrode active material exhibits a high capacity larger than 250 mAh g −1 in a voltage range of 1.6–4.8 V versus Li at 100 °C. Furthermore, bulk-type all-oxide solid-state batteries (Li 4 Ti 5 O 12 /80NMC532·20Li 2 SO 4 (mol%)) successfully function as secondary batteries with excellent cycle performances.

    DOI: 10.1002/admi.201802016

  • All-solid-state cells with Li<inf>4</inf>Ti<inf>5</inf>O<inf>12</inf>/carbon nanotube composite electrodes prepared by infiltration with argyrodite sulfide-based solid electrolytes via liquid-phase processing Reviewed

    So Yubuchi, Wataru Nakamura, Thomas Bibienne, Steeve Rousselot, Lauren W. Taylor, Matteo Pasquali, Mickaël Dollé, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago

    Journal of Power Sources   417   125 - 131   2019.03( ISSN:0378-7753

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    © 2019 Elsevier B.V. All-solid-state cells are safe, and have high energy densities and power densities. Sulfide-based solid electrolytes (SEs) exhibit high ionic conductivities and favorable mechanical properties allowing for the facile preparation of all-solid-state cells via simple mixing and cold-pressing processes. For practical applications, it is necessary to produce SEs and all-solid-state cells more efficiently. Herein, a novel fabrication process for homogeneous composite electrodes used in all-solid-state cells was successfully demonstrated using an infiltration technique. The Li 4 Ti 5 O 12 and carbon nanotube (LTO@CNT) porous electrode was infiltrated with a precursor solution containing an argyrodite Li 6 PS 5 Br SE, and the solvent was removed by drying at 150 °C under vacuum to prepare an infiltrated SE-LTO@CNT electrode. The process without conventional mixing formed an electrochemically active interface with a large contact area and favorable conduction pathways. The all-solid-state cell with the SE-LTO@CNT electrode showed an improved capacity of 163 mAh g −1 compared to those prepared with the dry-mixed electrodes at 25 °C, and the high capacity was maintained for 500 cycles. Moreover, the cell with the SE-LTO@CNT electrode showed a reversible capacity of 100 mAh g −1 or more at 4 C-rate and 100 °C. Thus, the infiltration process is effective for the practical fabrication and application of all-solid-state cells.

    DOI: 10.1016/j.jpowsour.2019.01.070

  • Fast Cationic and Anionic Redox Reactions in Li<inf>2</inf>RuO<inf>3</inf>-Li<inf>2</inf>SO<inf>4</inf> Positive Electrode Materials Reviewed

    Kenji Nagao, Atsushi Sakuda, Wataru Nakamura, Akitoshi Hayashi, Masahiro Tatsumisago

    ACS Applied Energy Materials   2 ( 3 )   1594 - 1599   2019.03( ISSN:2574-0962

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    © 2019 American Chemical Society. For the application of lithium-ion batteries (LiBs) to a large-scale power source for electric vehicles, positive electrode materials with high energy and power densities should be developed. Although Li-excess materials are regarded as high-capacity positive electrodes, there are several issues in the anionic redox reactions, such as oxygen gas evolution and large resistance, which lead to capacity fading and limitation of high-current operation. Here, we report the high-current operation of an electrochemical cell using the Li 2 RuO 3 -Li 2 SO 4 positive electrode in LiBs. The cell using Li 2 Ru 0.8 S 0.2 O 3.2 showed a high capacity of 350 mAh g -1 with an average discharge voltage of 2.9 V vs Li at 25 °C. By introducing an amorphous matrix based on Li 2 SO 4 , a high diffusion coefficient was maintained during the whole charge-discharge process, and low charge-transfer resistance was maintained even at a high oxidation state up to 4.2 V vs Li. As a result, extremely high current operation, such as 40 C rate, was achieved.

    DOI: 10.1021/acsaem.8b02163

  • Liquid-phase syntheses of sulfide electrolytes for all-solid-state lithium battery Reviewed

    Akira Miura, Nataly Carolina Rosero-Navarro, Atsushi Sakuda, Kiyoharu Tadanaga, Nguyen H.H. Phuc, Atsunori Matsuda, Nobuya Machida, Akitoshi Hayashi, Masahiro Tatsumisago

    Nature Reviews Chemistry   3 ( 3 )   189 - 198   2019.03( ISSN:2397-3358

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    © 2019, Springer Nature Limited. Solid sulfide electrolytes are key materials in all-solid-state lithium batteries because of their high lithium-ion conductivity and deformability, which enable the lithium-ion path to be connected between the material’s grain boundaries under pressure near room temperature. However, sulfur species are moisture-sensitive and exhibit high vapour pressures; therefore, syntheses of sulfide electrolytes need to be carefully designed. Liquid-phase reactions can be performed at low temperatures in controlled atmospheres, opening up the prospect of scalable processes for the preparation of sulfide electrolytes. Here, we review liquid-phase syntheses for the preparation of sulfide-based solid electrolytes and composites of electrolytes and electrodes, and we compare the charge–discharge performances of the all-solid-state lithium batteries using these components.

    DOI: 10.1038/s41570-019-0078-2

  • Morphological Effect on Reaction Distribution Influenced by Binder Materials in Composite Electrodes for Sheet-type All-Solid-State Lithium-Ion Batteries with the Sulfide-based Solid Electrolyte Reviewed

    Kezheng Chen, Sae Shinjo, Atsushi Sakuda, Kentaro Yamamoto, Tomoki Uchiyama, Kentaro Kuratani, Tomonari Takeuchi, Yuki Orikasa, Akitoshi Hayashi, Masahiro Tatsumisago, Yuta Kimura, Takashi Nakamura, Koji Amezawa, Yoshiharu Uchimoto

    Journal of Physical Chemistry C   123 ( 6 )   3292 - 3298   2019.02( ISSN:1932-7447

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    © 2019 American Chemical Society. In sheet-type all-solid-state lithium-ion batteries with the sulfide-based solid electrolyte, composite electrodes consist of active material, solid electrolyte, conductive additive material, and binder. Thus, they form a three-dimensional ionic and electronic conduction pass. In composite electrodes, the reaction inhomogeneity derived from their morphology exerts a remarkable effect on battery performance. In this study, we prepared sheet-type composite electrodes for all-solid-state lithium-ion batteries with the sulfide-based solid electrolyte using different binder materials with different solvents and investigated the reaction distribution within the electrodes using the 2D-imaging X-ray absorption spectroscopy. Thus, we demonstrated that the dominant factor of the reaction distribution formation is the ionic conduction, depending on the structure of the composite electrode, and that the structure is influenced by the combination between the binder and the solvent used in the preparation of the sheet-type composite electrode.

    DOI: 10.1021/acs.jpcc.8b09569

  • Liquid-Phase Syntheses of Sulfide Electrolytes for All-Solid-State Lithium Battery Reviewed

    A. Miura, N.C. Rosero-Navarro, A. Sakuda, K. Tadanaga, N.H.H. Phuc, A. Matsuda, N. Machida, A. Hayashi and M. Tatsumisago

    Nature Reviews Chemistry 雑誌   doi: 10.1038/s41570 - 019   2019.02

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  • Fast Cationic and Anionic Redox Reactions in Li2RuO3-Li2SO4 Positive Electrode Materials Reviewed

    K. Nagao, A. Sakuda, W. Nakamura, A. Hayashi and M. Tatsumisago

    ACS Appl. Energy Mater. 雑誌   2   1594 - 1599   2019.02

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  • Amorphous Na2TiS3 as an Active Material for All-Solid-State Sodium Batteries Reviewed

    A. Nasu, M. Otoyama, A. Sakuda, A. Hayashi and M. Tatsumisago

    Chem. Lett. 雑誌   48   288 - 290   2019.02

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  • Amorphous Na <inf>2</inf> TiS <inf>3</inf> as an active material for all-solid-state sodium batteries Reviewed

    Akira Nasu, Misae Otoyama, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago

    Chemistry Letters   48 ( 3 )   288 - 290   2019.01( ISSN:0366-7022

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    © 2019 The Chemical Society of Japan. Amorphous transition metal polysulfides are promising high capacity electrode active materials for sodium secondary batteries. Here we report the superior electrode performance of amorphous Na 2 TiS 3 . Crystalline (c-) and amorphous (a-) Na 2 TiS 3 were prepared by solid phase reaction with heat treatment and mechanochemical reaction, respectively. a-Na 2 TiS 3 showed 10 fold higher ionic conductivity (1.5 © 10 16 S cm 11 ) than that of c-Na 2 TiS 3 . The all-solid-state cells using c-Na 2 TiS 3 and a-Na 2 TiS 3 showed reversible capacities of 110 mAh g 11 and 250 mAh g 11 , respectively. Amorphization of Na 2 TiS 3 is a powerful way to improve electrode performance in all-solid-state sodium secondary batteries.

    DOI: 10.1246/cl.180895

  • Development of Next Generation Battery Materials by Mechanochemical Process Invited Reviewed

    作田敦, 林晃敏, 辰巳砂昌弘

    粉体工学会誌   56 ( 8 )   452 - 458   2019.01( ISSN:0386-6157

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    Copyright © The Japan Institute of Electronics Packaging Mechanochemistry is a study that deals with the interaction between mechanical energy and chemical energy. Mechanochemical reaction is a chemical reaction by mechanical energy. We have synthesized various next-generation battery materials using the mechanochemical method and evaluated their unique properties. In this paper, we review our recent researches on mechanochemical syntheses of sulfide materials as next-generation battery materials.

    DOI: 10.4164/sptj.56.452

    J-GLOBAL

  • Lithium dissolution/deposition behavior of Al-doped Li<inf>7</inf>La<inf>3</inf>Zr<inf>2</inf>O<inf>12</inf> ceramics with different grain sizes Reviewed

    Yuma Matsuki, Kousuke Noi, Minako Deguchi, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago

    Journal of the Electrochemical Society   166 ( 3 )   A5470 - A5473   2019.01( ISSN:0013-4651

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    © The Author(s) 2019. Published by ECS. Lithium dissolution/deposition behavior of Al-doped Li7La3Zr2O12 (LLZ) was investigated in terms of grain size of LLZ-sintered bodies. One LLZ had smaller grain sizes of primarily less than 1 μm (LLZ_SG), and the other one had larger grain sizes of 5-20 μm (LLZ_LG). The total resistance of a Li symmetric cell using LLZ_SG was smaller than that using LLZ_LG at 100◦C. The cell using LLZ_SG was stably cycled at 100◦C without short-circuiting at a high current density of 1.3 mA cm−2, while the cell using LLZ_LG was stably cycled at current densities below 0.26 mA cm−2. Stronger bonding at grain boundaries for LLZ_SG was expected to contribute to the improvement of cyclability.

    DOI: 10.1149/2.0661903jes

  • Ion-exchange synthesis of Li<inf>2</inf>NaPS<inf>4</inf> from Na<inf>3</inf>PS<inf>4</inf> Reviewed

    Jin Chen, So Yubuchi, Chie Hotehama, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago

    Chemistry Letters   48 ( 8 )   863 - 865   2019.01( ISSN:0366-7022

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    Publishing type:Research paper (scientific journal)  

    © 2019 The Chemical Society of Japan. A novel Li2NaPS4 crystal was successfully prepared from tetragonal Na3PS4 via Na+/Li+ ion-exchange in an acetonitrile solution of lithium bis(fluorosulfonyl)amide at room temperature. Its crystal structure was analyzed by powder X-ray diffraction. The Li2NaPS4 crystal maintained the basic anion framework of tetragonal Na3PS4 (P421c). The chemical environment of PS43- units in the ion-exchanged product was similar to that in the Li3PS4 crystal. Ion-exchange synthesis is a promising approach to develop novel sulfide-based materials.

    DOI: 10.1246/cl.190135

  • An argyrodite sulfide-based superionic conductor synthesized by a liquid-phase technique with tetrahydrofuran and ethanol Reviewed

    So Yubuchi, Miwa Uematsu, Chie Hotehama, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago

    Journal of Materials Chemistry A   7 ( 2 )   558 - 566   2019.01( ISSN:2050-7488

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    Publishing type:Research paper (scientific journal)  

    © 2018 The Royal Society of Chemistry. Sulfide-based solid electrolytes with halide elements are essential components of advanced all-solid-state batteries. Argyrodite crystals are viable candidates as solid electrolytes for realizing all-solid-state batteries. However, a simple and effective route for the synthesis of these solid electrolytes is required. Herein, argyrodite Li 6 PS 5 Br superionic conductors were synthesized from a homogeneous solution by a liquid-phase technique. The Li 6 PS 5 Br solid electrolyte was prepared in a shorter synthesis time of one day using tetrahydrofuran and ethanol as compared with the solid-phase method. More importantly, of all the sulfide-based solid electrolytes prepared by liquid-phase techniques, Li 6 PS 5 Br showed the highest ionic conductivity of 3.1 mS cm -1 at 25 °C. The obtained particle size of 1 μm is suitable for application in all-solid-state cells. Moreover, coating electrode active materials with the solid electrolyte using the precursor solution led to a large contact area between the electrode and electrolyte and improved the cell performance. In addition, infiltrating a porous electrode with the precursor solution of the solid electrolyte is suitable for forming homogeneous composite electrodes to improve the cell performance. The all-solid-state cell using the Li 6 PS 5 Br fine powder with a high conductivity of 1 mS cm -1 or more exhibited a reversible capacity of 150 mA h g -1 . This technique is effective for the industrial production of solid electrolytes and is applicable to all-solid-state batteries.

    DOI: 10.1039/c8ta09477b

  • Mechanochemical Synthesis of Na-Sb Alloy Negative Electrodes and Their Application to All-solid-state Sodium Batteries Reviewed

    Taka Ando, So Yubuchi, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago

    Electrochemistry   87 ( 5 )   289 - 293   2019.01( ISSN:1344-3542

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    Publishing type:Research paper (scientific journal)  

    © The Electrochemical Society of Japan, All rights reserved. Na-Sb alloy was synthesized as an advanced negative electrode material for all-solid-state sodium batteries by a mechanochemical process. An all-solid-state symmetric cell using a composite of an Na-Sb alloy and Na3PS4 solid electrolyte operated reversibly with a high reversible capacity of 370 mAh g−1 at room temperature under a current density of 0.064 mA cm−2. The composite electrode showed an effective ionic conductivity of 3.4 × 10−5 S cm−1. The cell also operated at 60°C under the same current density with low polarization compared to room temperature operation. The sodiation process from NaSb to Na3Sb was examined by ex situ X-ray diffraction (XRD) measurements. An all-solid-state half-cell using a TiS2 composite electrode and a Na3Sb composite electrode showed a high reversible capacity of 200 mAh g−1 at room temperature under a constant current density of 0.064 mA cm−2. Na-Sb alloys are a suitable negative electrode material for all-solid-state sodium batteries.

    DOI: 10.5796/electrochemistry.19-00014

  • Metastable materials for all-solid-state batteries Reviewed

    Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago

    Electrochemistry   87 ( 5 )   247 - 250   2019.01( ISSN:1344-3542

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    Publishing type:Research paper (scientific journal)  

    © The Electrochemical Society of Japan, All rights reserved. Materials with metastable structures often exhibit high stability up to a certain temperature, despite not being thermodynamically stable. Therefore, it is important to use the excellent physical properties generated by metastable structure. Secondary batteries are an energy device that stores chemical energy by producing thermodynamically metastable materials. Metastable materials can also be directly utilized as the electrode active materials and the solid electrolytes. The rapid quenching and mechanochemical processes are useful to obtain room temperature metastable materials. This review provides an overview of our research progress on glassy and metastable crystalline materials for all-solid-state batteries.

    DOI: 10.5796/electrochemistry.19-H0002

  • An Argyrodite Sulfide-based Superionic Conductor Synthesized by a Liquid-phase Technique with Tetrahydrofuran and Ethanol Reviewed

    S. Yubuchi, M. Uematsu, C. Hotehama, A. Sakuda, A. Hayashi and M. Tatsumisago

    J. Mater. Chem. A 雑誌   7   558 - 566   2019.01

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    Kind of work:Joint Work  

  • Preparation and Characterization of Lithium Ion Conductive Li3SbS4 Glass and Glass-Ceramic Electrolytes Reviewed

    T. Kimura, A. Kato, C. Hotehama, A. Sakuda, A. Hayashi and M. Tatsumisago

    Solid State Ionics 雑誌   333   45 - 49   2019.01

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    Kind of work:Joint Work  

  • All-Solid-State Cells with Li4Ti5O12/Carbon Nanotube Composite Electrodes Prepared by Infiltration with Argyrodite Sulfide-based Solid Electrolytes via Liquid-phase Processing Reviewed

    S. Yubuchi, W. Nakamura, T. Bibienne, S. Rousselot, L. W. Taylor, M. Pasquali, M. Dollé, A. Sakuda, A. Hayashi and M. Tatsumisago

    J. Power Sources 雑誌   417   125 - 131   2019.01

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    Kind of work:Joint Work  

  • Lithium Dissolution/Deposition Behavior of Al-Doped Li7La3Zr2O12 Ceramics with Different Grain Sizes Reviewed

    Y. Matsuki, K. Noi, M. Deguchi, A. Sakuda, A. Hayashi and M. Tatsumisago

    J. Electrochem. Soc. 雑誌   166 ( 3 )   A5470 - A5473   2019.01

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    Kind of work:Joint Work  

  • Characterization of composite quasi-solid electrolytes composed of 75Li<sub>2</sub>S・25P<sub>2</sub>S<sub>5</sub> glass and phosphate esters

    島本圭, 島本圭, 作田敦, 林晃敏, 辰巳砂昌弘

    電池討論会PDF要旨集(CD-ROM)   60th   2019( ISSN:0378-7753

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    © 2020 Elsevier B.V. Mechanical properties and ionic conductivities of solid electrolytes are important factors influencing the performance of all-solid-state batteries. This study investigates composite quasi-solid electrolytes composed of Li2S–P2S5 glass and a phosphate ester, prepared via planetary ball milling, and the relative densities of the powder-compressed pellets, formed using the composite quasi-solid electrolytes. Dense pellets of the Li2S–P2S5 glass electrolyte are obtained via addition of phosphate esters; the relative densities increase from 90.6% to 93.1%, without the ionic conductivities decreasing, upon addition of a small quantity of tris (2, 2, 2-trifluoroethyl) phosphate to the Li3PS4 glass. The addition of small quantities of phosphate esters to sulfide solid electrolytes is effective in improving the formability of these solid electrolytes.

    DOI: 10.1016/j.jpowsour.2020.228826

    J-GLOBAL

  • 全固体における界面形成とキャラクタリゼーション

    林 晃敏, 作田 敦, 辰巳砂 昌弘

    セラミックス   54   250 - 253   2019

  • Quantitative analysis of crystallinity in an argyrodite sulfide-based solid electrolyte synthesized via solution processing Reviewed

    So Yubuchi, Hirofumi Tsukasaki, Atsushi Sakuda, Shigeo Mori, Akitoshi Hayashi, Masahiro Tatsumisago

    RSC Advances   9 ( 25 )   14465 - 14471   2019( ISSN:2046-2069

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    Publishing type:Research paper (scientific journal)  

    © 2019 The Royal Society of Chemistry. Liquid-phase synthesis is a useful technique for preparing argyrodite sulfide-based solid electrolytes, and the synthesis conditions such as heat treatment strongly affect the conductivity. Because the understanding of structural changes reveals crucial information about their properties, it is necessary to evaluate this change during heat treatment to determine the factors that affect the conductivity. In this study, X-ray diffraction measurements and transmission electron microscope observations reveal the effects of heat treatment on the crystallinities and ionic conductivities in the synthesis process of argyrodite electrolytes with tetrahydrofuran and ethanol. The amorphous material is in the main phase when heated at low temperatures below 200 °C and exhibits relatively low conductivities of ca. 2 × 10-4 S cm-1 despite precipitation of the argyrodite crystals. As the heat treatment temperature increases, the ratio of argyrodite crystals increases, involving nucleation and grain growth, leading to high conductivities of over 10-3 S cm-1. It is critical to control the ratio of the amorphous and crystal phases to achieve high conductivities in the synthesis of argyrodite electrolytes via liquid-phase processing.

    DOI: 10.1039/c9ra00949c

  • Amorphization of Sodium Cobalt Oxide Active Materials for High-Capacity All-Solid-State Sodium Batteries Reviewed

    Y. Nagata, K. Nagao, M. Deguchi, A. Sakuda, A. Hayashi, H. Tsukasaki, S. Mori and M. Tatsumisago

    Chem. Mater. 雑誌   30 ( 20 )   6998 - 7004   2018.11

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    Kind of work:Joint Work  

  • Analysis of the Discharge/Charge Mechanism in VS4 Positive Electrode Material Reviewed

    K. Koganei, A. Sakuda, T. Takeuchi, H. Sakaebe, H. Kobayashi, H. Kageyama, T. Kawaguchi, H. Kiuchi, K. Nakanishi, M Yoshimura T. Ohta, T. Fukunaga, E. Matsubara

    Solid State Ionics 雑誌   323   32 - 36   2018.10

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  • A Reversible Rocksalt to Amorphous Phase Transition Involving Anion Redox Reviewed

    A. Sakuda, K. Ohara, T. Kawaguchi, K. Fukuda, K. Nakanishi, H. Arai, Y. Uchimoto, T. Ohta, E. Matsubara, Z. Ogumi, K. Kuratani, H. Kobayashi, M. Shikano, T. Takeuchi and H. Sakaebe

    Sci. Rep. 雑誌   8 ( 1 )   1 - 6   2018.10

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  • Slurry Mixing for Fabricating Silicon-Composite Electrodes in All-Solid-State Batteries with High Areal Capacity and Cycling Stability Reviewed

    M. Yamamoto, Y. Terauchi, A. Sakuda and M. Takahashi

    J. Power Sources 雑誌   402   506 - 512   2018.10

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    Kind of work:Joint Work  

  • Lithium Dissolution/Deposition Behavior with Li3PS4-LiI Electrolyte for All-Solid-State Batteries Operating at High Temperatures Reviewed

    M. Suyama, A. Kato, A. Sakuda, A. Hayashi and M. Tatsumisago

    Electrochim. Acta 雑誌   286   158 - 162   2018.10

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    Kind of work:Joint Work  

  • Optical Microscopic Observation of Graphite Composite Negative Electrodes in All-Solid-State Lithium Batteries Reviewed

    M. Otoyama, A. Sakuda, A. Hayashi and M. Tatsumisago

    Solid State Ionics 雑誌   323   123 - 129   2018.10

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    Kind of work:Joint Work  

  • Favorable Composite Electrodes for All-Solid-State Batteries Reviewed

    A. Sakuda

    J. Ceram. Soc. Jpn. 雑誌   126 ( 9 )   675 - 683   2018.09

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    Kind of work:Single Work  

  • Mechanical Properties of Sulfide Glasses in All-Solid-State Batteries Reviewed

    A. Kato, M. Nose, M. Yamamoto, A. Sakuda, A. Hayashi and M. Tatsumisago

    J. Ceram. Soc. Jpn. 雑誌   126 ( 9 )   719 - 727   2018.09

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    Kind of work:Joint Work  

  • Mechanochemical Synthesis and Characterization of Metastable Hexagonal Li4SnS4 Solid Electrolyte Reviewed

    K. Kanazawa, S. Yubuchi, C. Hotehama, M. Otoyama, S. Shimono, H. Ishibashi, Y. Kubota, A. Sakuda, A. Hayashi and M. Tatsumisago

    Inorg. Chem. 雑誌   57 ( 16 )   9925 - 9930   2018.08

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    Kind of work:Joint Work  

  • Structure Analyses of Fe-substituted Li2S-based Positive Electrode Materials for Li-S Batteries Reviewed

    T. Takeuchi, H. Kageyama, N. Taguchi, K. Nakanishi, T. Kawaguchi, K. Ohara, K. Fukuda, A. Sakuda, T. Ohta, T. Fukunaga, H. Sakaebe, H. Kobayashi and E. Matsubara

    Solid State Ionics 雑誌   320   387 - 391   2018.07

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    Kind of work:Joint Work  

  • High-Temperature Performance of All-Solid-State Lithium-Metal Batteries Having Li/Li3PS4 Interfaces Modified with Au Thin Films Reviewed

    A. Kato, M. Suyama, C. Hotehama, H. Kowada, A. Sakuda, A. Hayashi and M. Tatsumisago

    J. Electrochem. Soc. 雑誌   165 ( 9 )   A1950 - A1954   2018.06

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    Kind of work:Joint Work  

  • Electrochemical Properties of All-Solid-State Lithium Batteries with Amorphous FeSx-based Composite Positive Electrodes Prepared via Mechanochemistry Reviewed

    M. Pan, T. Hakari, A. Sakuda, A. Hayashi, Y. Suginaka, S. Mori and M. Tatsumisago

    Electrochemistry 雑誌   86 ( 4 )   175 - 178   2018.06

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  • Mechanochemically Prepared Li2S-P2S5-LiBH4 Solid Electrolytes with an Argyrodite Structure Reviewed

    A. Sakuda, A. Yamauchi, S. Yubuchi, N. Kitamura, Y. Idemoto, A. Hayashi and M. Tatsumisago

    ACS Omega 雑誌   3 ( 5 )   5453 - 5458   2018.05

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    Kind of work:Joint Work  

  • Preparation of an Amorphous 80LiCoO2・20Li2SO4 Thin Film Electrode by Pulsed Laser Deposition Reviewed

    M. Nishimura, K. Nagao, Y. Ito, M. Deguchi, A. Sakuda, A. Hayashi and M. Tatsumisago

    Electrochemistry 雑誌   86 ( 5 )   246 - 249   2018.05

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    Kind of work:Joint Work  

  • Oxide-Based Composite Electrolytes Using Na3Zr2Si2PO12/Na3PS4 Interfacial Ion Transfer Reviewed

    K. Noi, Y. Nagata, T. Hakari, K. Suzuki, S. Yubuchi, Y. Ito, A. Sakuda, A. Hayashi and M. Tatsumisago

    ACS Appl. Mater. Interfaces 雑誌   10 ( 23 )   19605 - 19614   2018.05

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    Kind of work:Joint Work  

  • Mechanical Properties of Li2S-P2S5 Glasses with Lithium Halides and Application in All-Solid-State Batteries Reviewed

    A. Kato, M. Yamamoto, A. Sakuda, A. Hayashi and M. Tatsumisago

    ACS Appl. Energy Mater. 雑誌   1   1002 - 1007   2018.04

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  • Amorphous LiCoO2-based Positive Electrode Active Materials with Good Formability for All-Solid-State Rechargeable Batteris Reviewed

    K. Nagao, Y. Nagata, A. Sakuda, A. Hayashi and M. Tatsumisago

    MRS Advances 雑誌   3 ( 23 )   1319 - 1327   2018.03

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  • Structure Analyses of Fe-substituted Li2S-based Positive Electrode Materials for Li-S Batteries Reviewed

    T. Takeuchi, H. Kageyama, N. Taguchi, K. Nakanishi, T. Kawaguchi, K. Ohara, K. Fukuda, A. Sakuda, T. Ohta, T. Fukunaga, H. Sakaebe, H. Kobayashi and E. Matsubara

    Solid State Ionics 雑誌   320   387 - 391   2018.03

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    Kind of work:Joint Work  

  • Preparation of Na3PS4 Electrolyte by Liquid-phase Process Using Ether Reviewed

    M. Uematsu, S. Yubuchi, K. Noi, A. Sakuda, A. Hayashi and M. Tatsumisago

    Solid State Ionics 雑誌   320   33 - 37   2018.02

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    Kind of work:Joint Work  

  • Binder-free Sheet-type All-Solid-State Batteries with Enhanced Rate Capabilities and High Energy Densities Reviewed

    M. Yamamoto, Y. Terauchi, A. Sakuda and M. Takahashi

    Scientific Reports 雑誌   8 ( 1212 )   1 - 10   2018.01

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    Kind of work:Joint Work  

  • Preparation of Sodium Ion Conductive Na10GeP2S12 Glass-Ceramic Electrolytes Reviewed

    F. Tsuji, N. Tanibata, A. Sakuda, A. Hayashi and M. Tatsumisago

    Chem. Lett. 雑誌   2018 ( 47 )   13 - 15   2018.01

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    Kind of work:Joint Work  

  • Electronic and Ionic Conductivities of LiNi1/3Mn1/3Co1/3O2-Li3PS4 Positive Composite Electrodes for All-Solid-State Lithium Batteries Reviewed

    T. Asano, S. Yubuchi, A. Sakuda, A. Hayashi and M. Tatsumisago

    J. Electrochem Soc. 雑誌   164 ( 14 )   A3960 - A3963   2017.12

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    Kind of work:Joint Work  

  • Recent Progress on Interface Formation in All-Solid-State Batteries Reviewed

    A. Sakuda, A. Hayashi and M. Tatsumisago

    Curr. Opin. Electrochem. 雑誌   6   108 - 114   2017.12

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    Kind of work:Joint Work  

  • All-Solid-State Battery Electrode Sheets Prepared by a Slurry Coating Process Reviewed

    A. Sakuda, K. Kuratani, M. Yamamoto, M. Takahashi, T. Takeuchi and H. Kobayashi

    J. Electrochem Soc. 雑誌   164 ( 12 )   A2474 - A2478   2017.12

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    Kind of work:Joint Work  

  • Cubic Rocksalt Li2SnS3 and a Solid Solution with Li3NbS4 Prepared by Mechanochemical Synthesis Reviewed

    A. Sakuda, K. Kuratani, T. Takeuchi, H. Kiuchi, T. Kawaguchi, M. Shikano, H. Sakaebe and H. Kobayashi

    Electrochemistry 雑誌   85 ( 9 )   580 - 584   2017.09

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    Kind of work:Joint Work  

  • Amorphous Metal Polysulfides: Electrode Materials with Unique Insertion / Extraction Reactions Reviewed

    A. Sakuda, K. Ohara, K. Fukuda, K. Nakanishi, T. Kawaguchi, H. Arai, Y. Uchimoto, T. Ohta, E. Matsubara, Z. Ogumi, T. Okumura, H. Kobayashi, H. Kageyama, M. Shikano, H. Sakaebe and T. Takeuchi

    J. Am. Chem. Soc. 雑誌   139   8796 - 8799   2017.07

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  • Electrical and Mechanical Properties of Glass and Glass-Ceramic Electrolytes in the System Li3BO3-Li2SO4 Reviewed

    M. Tatsumisago, R. Takano, M. Nose, K. Nagao, A. Kato, A. Sakuda, K. Tadanaga and A. Hayashi

    J. Ceram. Soc. Jpn. 雑誌   125 ( 6 )   433 - 437   2017.06

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    Kind of work:Joint Work  

  • Fabrication of Composite Positive Electrode Sheet with High Active Material Content and Effect of Fabrication Pressure for All-Solid-State Battery Reviewed

    M. Yamamoto, M. Takahashi, Y. Terauchi, Y. Kobayashi, S. Ikeda and A. Sakuda

    J. Ceram. Soc. Jpn. 雑誌   125 ( 5 )   391 - 395   2017.05

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    Kind of work:Joint Work  

  • Preparation and Characterization of Glass Solid Electrolytes in the Pseudoternary System Li3BO3-Li2SO4-Li2CO3 Reviewed

    K. Nagao, M. Nose, A. Kato, A. Sakuda, A. Hayashi and M. Tatsumisago

    Solid State Ionics 雑誌   308   68 - 76   2017.05

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    Kind of work:Joint Work  

  • Development of Li2TiS3-Li3NbS4 by a Mechanochemical Process Reviewed

    A. Sakuda, T. Takeuchi, M. Shikano, K. Ohara, K. Fukuda, Y. Uchimoto, Z. Ogumi, H. Kobayashi and H. Sakaebe

    J. Ceram. Soc. Jpn. 雑誌   125 ( 4 )   268 - 271   2017.04

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Books and Other Publications

  • モビリティ用電池の化学 -リチウムイオン二次電池から燃料電池まで- (CSJ Current Review 44 Chemistry of Batteries for Mobilities)

    林 晃敏, 作田 敦, 辰巳砂昌弘( Role: Joint author ,  全固体電池)

    化学同人  2022.03 

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    Responsible for pages:50-56  

  • Next Generation Batteries – Realization of High Energy Density Rechargeable Batteries-

    A. Sakuda( Role: Joint author)

    Springer Nature Singapore  2021.12 

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    Responsible for pages:119-123  

  • Next Generation Batteries – Realization of High Energy Density Rechargeable Batteries-

    M. Tatsumisago and A. Sakuda( Role: Joint author ,  Solution Process)

    Springer Nature Singapore  2021.12 

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    Responsible for pages:77-83  

  • 車載用リチウムイオン電池の開発最前線

    林 晃敏・作田 敦・辰巳砂昌弘( Role: Joint author)

    シーエムシー出版  2020.11 

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    Responsible for pages:188-194  

  • Encyclopedia of Materials: Technical Ceramics and Glasses

    K. Ohara, A. Sakuda, A. Hayashi( Role: Joint author)

    Elsevier   2020.06 

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    Responsible for pages:1-11  

  • 全固体リチウム電池の開発動向と応用展望

    作田 敦( Role: Joint author)

    シーエムシー出版  2019.06 

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    Responsible for pages:137-144  

  • リチウムイオン電池&全固体電池製造技術 -微粒子&スラリー調整および評価を中心に-

    加藤敦隆・作田 敦・林 晃敏・辰巳砂昌弘( Role: Joint author)

    シーエムシー・リサーチ  2019.06 

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    Responsible for pages:235-244  

  • 最近の化学工学67 進化する燃料電池・二次電池 -反応・構造・製造技術の基礎と未来社会を支える電池技術-

    林 晃敏・作田 敦・辰巳砂昌弘( Role: Joint author)

    化学工学会  2019.02 

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    Responsible for pages:193-206  

  • 全固体電池開発の現状と産業化へのアプローチ ~製造プロセス、部材作成、高容量化、評価手法~

    辰巳砂昌弘・作田 敦・林 晃敏( Role: Joint author)

    情報機構  2018.11 

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    Responsible for pages:72-83  

  • 全固体電池の基礎理論と開発最前線

    林 晃敏・作田 敦・辰巳砂昌弘( Role: Joint author)

    シーエムシー・リサーチ  2018.07 

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    Responsible for pages:57-71  

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MISC

  • Mechanochemical synthesis of electrode-electrolyte bifunctional material in the system Li<sub>2</sub>SV<sub>2</sub>S<sub>3</sub>-LiI

    作田敦, 重冨竜輝, 藤田侑志, 本橋宏大, 辰巳砂昌弘, 林晃敏

    日本化学会春季年会講演予稿集(Web)   102nd   2022

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  • The effect of stack pressure on Li stripping and plating performance in all-solid-state Li symmetric cell using sulfide electrolyte

    林晃敏, 朝倉大智, 稲岡嵩晃, 本橋宏大, 作田敦, 辰巳砂昌弘

    日本化学会春季年会講演予稿集(Web)   102nd   2022

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  • Cross-sectional SEM observation for Si composite electrode of all-solid-state battery with sulfide electrolyte

    作田敦, 栗岡英司, 奈須滉, 本橋宏大, 林晃敏

    日本化学会春季年会講演予稿集(Web)   102nd   2022

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  • SEM Observation for SnB<sub>2</sub>O<sub>4</sub> Glass Composite Electrode in All-Solid-State Batteries with Sulfide Electrolyte

    林晃敏, 林侑希, 木村拓哉, 本橋宏大, 作田敦

    日本化学会春季年会講演予稿集(Web)   102nd   2022

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  • 遷移金属硫化物ガラス正極材料の充放電メカニズム

    作田敦

    日本放射光学会年会・放射光科学合同シンポジウム(Web)   35th   2022

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  • Synthesis and characterization of Na<sub>2</sub>S-In<sub>2</sub>S<sub>3</sub> electrolytes with Na ion conductivity

    本橋宏大, 奈須滉, 保手浜千絵, 作田敦, 辰巳砂昌弘, 林晃敏

    電気化学会大会講演要旨集(CD-ROM)   89th   2022

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  • Development of all-solid-state battery with inorganic amorphous material

    林晃敏, 作田敦, 辰巳砂昌弘

    日本化学会春季年会講演予稿集(Web)   102nd   2022

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  • 次世代二次電池開発の最新動向と展望 解説 硫化物電解質を用いた全固体リチウム-硫黄電池の研究開発

    林晃敏, 作田敦, 本橋宏大, 辰巳砂昌弘

    工業材料   70 ( 3 )   2022( ISSN:0452-2834

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  • Synthesis of Na<sub>3</sub>BS<sub>3</sub> glass electrolyte through sodium polysulfide

    作田敦, 音野智哉, 城田岳, 奈須滉, 本橋宏大, 林晃敏

    日本化学会春季年会講演予稿集(Web)   102nd   2022

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  • Expectations for Ion-conducting Glasses and the Future

    大幸裕介, 作田敦, 本間剛, 林晃敏

    セラミックス   57 ( 3 )   137 - 140   2022( ISSN:0009-031X

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  • Development of Sulfide-Based Solid Electrolytes for Application to All-Solid-State Batteries

    木村拓哉, 作田敦, 辰巳砂昌弘, 林晃敏

    月刊ファインケミカル   51 ( 7 )   2022( ISSN:0913-6150

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  • Progress of glass electrolyte for all-solid-state battery

    林晃敏, 作田敦, 辰巳砂昌弘

    日本化学会春季年会講演予稿集(Web)   102nd   2022

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  • All-Solid-State Battery

    林晃敏, 作田敦, 辰巳砂昌弘

    CSJ Current Review   ( 44 )   2022

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  • Microstructural analysis by TEM of SnB<sub>2</sub>O<sub>4</sub> glassy electrode composites for all-solid-state lithium batteries

    坂本圭悟, 塚崎裕文, 林侑希, 木村拓哉, 作田敦, 林晃敏, 森茂生

    日本セラミックス協会秋季シンポジウム講演予稿集(Web)   35th   2022

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  • Preparation of All-Solid-State Lithium Battery Using TiO<sub>2</sub> Anode and Oxide Electrolyte

    伊崎真一郎, 伊崎真一郎, 薄井洋行, 薄井洋行, 道見康弘, 道見康弘, 奈須滉, 作田敦, 林晃敏, 坂口裕樹, 坂口裕樹

    電気化学秋季大会講演要旨集(CD-ROM)   2021   2021

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  • Preparation of All-Solid-State Lithium Battery Using TiO<sub>2</sub> Anode and Oxide Electrolyte

    伊崎真一郎, 伊崎真一郎, 薄井洋行, 薄井洋行, 道見康弘, 道見康弘, 奈須滉, 作田敦, 林晃敏, 坂口裕樹, 坂口裕樹

    電池討論会PDF要旨集(CD-ROM)   62nd   2021

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  • Ex situ TEM Observation of Deterioration Process of Sulfide-based Solid Electrolytes during Exposure to Humidity-Controlled Air

    塚崎裕文, 佐野光, 木村拓哉, 作田敦, 林晃敏, 森茂生

    電池討論会PDF要旨集(CD-ROM)   62nd   2021

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  • Role of sodium vacancy and aliovalent substitution in superionic Na<sub>3-x</sub>Sb<sub>1-x</sub>W<sub>x</sub>S<sub>4</sub>

    西村真一, 西村真一, 作田敦, 林晃敏, 林晃敏, 山田淳夫, 山田淳夫

    電池討論会PDF要旨集(CD-ROM)   62nd   2021

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  • In situ TEM observation and Microstructures in Na<sub>3</sub>PS<sub>4</sub> electrolytes

    中島宏, 塚崎裕文, DING Jiong, 木村拓哉, 中野匠, 作田敦, 林晃敏, 森茂生

    電池討論会PDF要旨集(CD-ROM)   62nd   2021

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  • Preparation of LiCoO<sub>2</sub>-Li<sub>2</sub>SO<sub>4</sub> nanocrystalline/amorphous composite electrodes and their application in all-solid-state batteries

    計賢, 作田敦, 出口三奈子, 辰巳砂昌弘, 林晃敏

    電池討論会PDF要旨集(CD-ROM)   62nd   2021

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  • LiCoO<sub>2</sub>-Li<sub>2</sub>MnO<sub>3</sub>-Li<sub>2</sub>SO<sub>4</sub> nanocrystalline/amorphous composite electrodes: Preparation and application in all-solid-state batteries

    作田敦, 計賢, 田中啓之, 荒井美穂, 辰巳砂昌弘, 林晃敏

    電池討論会PDF要旨集(CD-ROM)   62nd   2021

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  • Ionic Conductivity of Li<sub>3</sub>BS<sub>3</sub> Glass Electrolytes Prepared via Mechanochemistry

    木村拓哉, 井上文音, 長尾賢治, 作田敦, 辰巳砂昌弘, 林晃敏

    電気化学秋季大会講演要旨集(CD-ROM)   2021   2021

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  • Surface Degradation of Sulfide-Based Li-P-S-I Glass Ceramic Electrolyte by Exposure to Small Amount of Water and Recovery by Heat Treatment (2)

    森野裕介, 佐野光, 川本浩二, 樋口弘幸, 山本徳行, 福井賢一, 松田厚範, 作田敦, 林晃敏

    電池討論会PDF要旨集(CD-ROM)   62nd   2021

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  • Surface Degradation of Sulfide-Based Li-P-S-I Glass Ceramic Electrolyte by Exposure to Small Amount of Water and Recovery by Heat Treatment (1)

    佐野光, 森野裕介, 松村安行, 川本浩二, 樋口弘幸, 山本徳行, 松田厚範, 塚崎裕文, 森茂生, 作田敦, 林晃敏

    電池討論会PDF要旨集(CD-ROM)   62nd   2021

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  • Deterioration of Li-P-S-I Glass Ceramic Electrolyte under Manufacturing Environment and Its Recovery by Heat Treatment

    佐野光, 森野裕介, 川本浩二, 樋口弘幸, 山本徳行, 作田敦, 林晃敏

    電気化学秋季大会講演要旨集(CD-ROM)   2021   2021

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  • Preparation of amorphous MoS<sub>3</sub> by thermal decomposition and application to electrochemical catalyst for hydrogen evolution reaction

    作田敦, 長谷川優樹, 川崎友輔, 城田岳, 出口三奈子, 林晃敏

    日本化学会春季年会講演予稿集(Web)   101st   2021

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  • Correlation between charge density distribution and ionic conduction in sulfide glasses

    尾原幸治, 作田敦, 池田一貴, 中田謙吾, 廣井慧, 中野匠, 木村拓哉, 森茂生, 林晃敏

    日本物理学会講演概要集(CD-ROM)   76 ( 2 )   2021( ISSN:2189-079X

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  • Ionic conductivity and microstructural analysis of sulfide-based solid electrolyte Na<sub>3</sub>PS<sub>4</sub>

    DING Jiong, 中島宏, 塚崎裕文, 木村拓哉, 中野匠, 森茂生, 作田敦, 辰巳砂昌弘, 林晃敏

    日本セラミックス協会年会講演予稿集(Web)   2021   2021

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  • Conductivity Degradation of Sulfide-Based Solid Electrolyte under Low-Humidity Environment and Its Recovery by Heat Treatment

    佐野光, 森野裕介, 松村安行, 阿部武志, 石黒恭生, 作田敦, 佐藤大輝, 今西哲士, 福井賢一, 高橋司, 平野武広, 堀智, 菅野了次

    電気化学会大会講演要旨集(CD-ROM)   88th   2021

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  • Mechanochemical synthesis of Na<sub>3</sub>BO<sub>3</sub> glass electrolytes with various sodium salts

    林晃敏, 奥島千尋, 日下部史也, 奈須滉, 木村拓哉, 作田敦, 辰巳砂昌弘

    日本化学会春季年会講演予稿集(Web)   101st   2021

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  • All-solid-state sodium batteries using sulfide electrolytes with reduction stability and hard carbon negative electrode

    吉田航, 奈須滉, 作田敦, 辰巳砂昌弘, 林晃敏

    電池討論会PDF要旨集(CD-ROM)   62nd   2021

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  • Characterization of Na<sub>3</sub>BS<sub>3</sub> glass as solid electrolyte with reduction stability and application to all-solid-state sodium metal cells

    奈須滉, 稲岡嵩晃, 作田敦, 辰巳砂昌弘, 林晃敏

    電池討論会PDF要旨集(CD-ROM)   62nd   2021

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  • Preparation of fluorine-doped Li<sub>6</sub>PS<sub>5</sub>Cl electrolytes and their electrochemical performance for Li dissolution/deposition

    林晃敏, 井澤遼, 梅田智仁, 保手浜千絵, 作田敦, 辰巳砂昌弘

    日本化学会春季年会講演予稿集(Web)   101st   2021

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  • Development of Sulfide Solid Electrolyte with Superior Sodium-ion Conductivity

    林晃敏, 林晃敏, 作田敦

    セラミックス   56 ( 9 )   2021( ISSN:0009-031X

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  • Elucidation of reaction mechanism of Li<sub>2</sub>S-V<sub>2</sub>S<sub>3</sub>-LiI binary functional cathode for all-solid-state batteries

    渡邊稔樹, XIAO Yao, 山本健太郎, PAN Wenli, 内山智貴, 上杉健太朗, 竹内晃久, 作田敦, 林晃敏, 辰巳砂昌弘, 高見剛, 松永利之, 内本喜晴

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  • The evaluation of the compressed Li<sub>3</sub>PS<sub>4</sub> glass electrolyte using the AC impedance method

    作田敦, 鳥居真人, 遠地智大, 辰巳砂昌弘, 林晃敏

    日本化学会春季年会講演予稿集(Web)   101st   2021

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  • Characterization of lithium ion conductive Li<sub>3</sub>BX<sub>y</sub> (X = N, O, S) glass electrolytes

    木村拓哉, 茂野真成, 井上文音, 長尾賢治, 作田敦, 辰巳砂昌弘, 林晃敏

    ガラスおよびフォトニクス材料討論会講演要旨集   62nd   2021

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  • Preparation and characterization of Li<sub>3-x</sub>YCl<sub>6-x</sub> solid electrolytes by the mechanochemical method

    林晃敏, 岡田侑也, 米田陽平, 木村拓哉, 作田敦

    日本化学会春季年会講演予稿集(Web)   101st   2021

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  • Mechanochemical synthesis of Li<sub>2</sub>O based solid electrolytes

    藤田侑志, 川崎友輔, 稲岡嵩晃, 中野匠, 木村拓哉, 作田敦, 辰巳砂昌弘, 林晃敏

    電気化学会大会講演要旨集(CD-ROM)   88th   2021

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  • Liquid-phase synthesis using ethylenediamine for Li<sub>3</sub>PS<sub>4</sub> solid electrolytes

    伊藤茜, 木村拓哉, 保手浜千絵, 作田敦, 辰巳砂昌弘, 林晃敏

    電気化学会大会講演要旨集(CD-ROM)   87th   2020

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  • Effect of annealing conditions to the local structure and the lithium ion conductivity of Li<sub>2</sub>S-P<sub>2</sub>S<sub>5</sub>-based electrolytes synthesized by using ethyl propionate

    高橋勝國, YANG Seunghoon, 山本健太郎, 尾原幸治, 渡邊稔樹, 内山智貴, 作田敦, 林晃敏, 辰巳砂昌弘, 引間和浩, 武藤浩行, 松田厚範, 内本喜晴

    電池討論会PDF要旨集(CD-ROM)   61st   2020

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  • Preparation of Li<sub>2</sub>S activated by Cu substitution and its application to all-solid-state batteries

    川崎友輔, 出口三奈子, 塚崎裕文, 森茂生, 作田敦, 辰巳砂昌弘, 林晃敏

    電池討論会PDF要旨集(CD-ROM)   61st   2020

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  • Structural Analysis of 80Li<sub>2</sub>S・20LiI Solid Solution Positive Electrode for All-solid-state Batteries

    作田敦, 藤田侑志, 安藤鷹, 岸拓馬, 計賢, 出口三奈子, 辰巳砂昌弘, 林晃敏

    日本化学会春季年会講演予稿集(CD-ROM)   100th   2020

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  • Characterization of amorphous MoS<sub>3</sub> electrode for all-solid-state sodium secondary batteries

    城田岳, 奈須滉, 出口三奈子, 作田敦, 辰巳砂昌弘, 林晃敏

    日本セラミックス協会秋季シンポジウム講演予稿集(CD-ROM)   33rd   2020

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  • Charge discharge performance of all-solid-state batteries with lithium sulfide-lithium salt composites as a positive electrode

    計賢, 出口三奈子, 作田敦, 辰巳砂昌弘, 林晃敏

    日本セラミックス協会年会講演予稿集(CD-ROM)   2020   2020

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  • Development of Ion Exchange Process for Sulfide Polyanion Materials

    作田敦, 林晃敏, 辰巳砂昌弘

    村田学術振興財団年報   ( 34 )   2020( ISSN:0919-3383

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  • Degradation of Sulfide-based Solid Electrolytes in Dry-Room-Simulated Environment

    佐野光, 森野裕介, 佐藤信平, 板山直彦, 作田敦, 林晃敏, 高橋司, 宮下徳彦, 岩崎正博, 竹原雅裕, 阿部武志, 石黒恭生

    電池討論会PDF要旨集(CD-ROM)   61st   2020

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  • Towards Superior All-Solid-State Lithium and Sodium Secondary Batteries Using Sulfur-based Active Materials

    作田敦, 安藤鷹, 佐藤優太, 金澤健人, 黒松亜紀, 林晃敏, 辰巳砂昌弘

    電池討論会PDF要旨集(CD-ROM)   61st   2020

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  • Thermal stability and microstructure of the LiNi<sub>1/3</sub>Mn<sub>1/3</sub>Co<sub>1/3</sub>O<sub>2</sub> electrode layer using air-stable Li<sub>4</sub>SnS<sub>4</sub> solid electrolyte

    塚崎裕文, 乙山美紗恵, 木村拓哉, 森茂生, 作田敦, 林晃敏, 辰巳砂昌弘

    日本セラミックス協会秋季シンポジウム講演予稿集(CD-ROM)   33rd   2020

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  • In situ TEM observation of air-exposure degradation process of sulfide-based solid electrolytes

    塚崎裕文, 五十嵐啓介, 和久井亜希子, 矢口紀恵, 木村拓哉, 作田敦, 林晃敏, 辰巳砂昌弘, 森茂生

    電池討論会PDF要旨集(CD-ROM)   61st   2020

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  • Synthesis and characterization of amorphous MoS<sub>3</sub> electrode for all-solid-state sodium secondary battery.

    作田敦, 城田岳, 奈須滉, 辰巳砂昌弘, 林晃敏

    日本化学会春季年会講演予稿集(CD-ROM)   100th   2020

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  • Oxide-Based All-Solid-State Lithium Battery

    林晃敏, 作田敦, 辰巳砂昌弘

    機能材料   40 ( 5 )   2020( ISSN:0286-4835

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  • Examination of feeding technique of silage mixing feed rice and tofu cake in pigs.

    鈴木菜月, 吉岡圭輔, 前田育子, 佐々木将武, 戸田尚美, 作田敦

    茨城県畜産センター研究報告   ( 51 )   2020( ISSN:1346-6488

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  • エネルギー・環境問題を解決する新材料・新技術 ガラス材料を用いた全固体電池の電極-電解質界面構築

    作田敦, 辰巳砂昌弘, 林晃敏

    金属   90 ( 10 )   2020( ISSN:0368-6337

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  • Effect of properties of solvents used for liquid phase synthesis to lithium ion conductivity

    高橋勝國, 高橋勝國, YANG Seunghoon, 山本健太郎, 尾原幸治, 渡邊稔樹, 内山智貴, 作田敦, 林晃敏, 辰巳砂昌弘, 引間和浩, 武藤浩行, 松田厚範, 内本喜晴

    固体イオニクス討論会講演要旨集   46th (CD-ROM)   2020

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  • Increasing capacity of all-solid-state Na-S batteries using liquid-phase synthesized Na<sub>3</sub>SbS<sub>4</sub> solid electrolyte

    安藤鷹, 作田敦, 辰巳砂昌弘, 林晃敏

    電気化学会大会講演要旨集(CD-ROM)   87th   2020

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  • Solvent effect on local structure and lithium ion conductivity of liquid phase synthesized Li<sub>2</sub>S-P<sub>2</sub>S<sub>5</sub>-based electrolytes

    山本健太郎, YANG Seunghoon, 高橋勝國, 尾原幸治, 渡邊俊樹, 内山智貴, 作田敦, 林晃敏, 辰巳砂昌弘, 引間和浩, 武藤浩行, 松田厚範, 内本喜晴

    電池討論会PDF要旨集(CD-ROM)   61st   2020

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  • 未来を拓く最新電池技術 実用化が見えてきた全固体リチウム二次電池

    作田敦, 林晃敏, 辰巳砂昌弘

    KEC情報   ( 252 )   2020

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  • Powder Process Technology to Enrich the Daily Life: Basics and Research Trends of Bulk-Type All-Solid-State Batteries

    作田敦, 林晃敏, 辰巳砂昌弘

    粉砕   ( 64 )   2020( ISSN:0429-9051

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  • In-situ X-ray diffraction for Na<sub>3</sub>PS<sub>4</sub> solid electrolytes exposed to air flow

    林晃敏, 中野匠, 木村拓哉, 作田敦, 辰巳砂昌弘

    日本化学会春季年会講演予稿集(CD-ROM)   100th   2020

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  • Amorphous state investigation of the Li<sub>2</sub>S-P<sub>2</sub>S glass via in situ TEM observation

    塚崎裕文, 五十嵐啓介, 和久井亜希子, 矢口紀恵, 乙山美紗恵, 作田敦, 林晃敏, 辰巳砂昌弘, 森茂生

    日本セラミックス協会年会講演予稿集(CD-ROM)   2020   2020

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  • Electrochemical Structural Changes of Na<sub>2</sub>FeS<sub>2</sub> as Iron Based Active Materials for All-Solid-State Batteries

    奈須滉, 作田敦, 土本晃久, 大久保將史, 山田淳夫, 辰巳砂昌弘, 林晃敏

    固体イオニクス討論会講演要旨集   46th (CD-ROM)   2020

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  • Electrochemical Property of Na<sub>2</sub>FeS<sub>2</sub> Active Material for All-Solid-State Sodium Batteries

    奈須滉, 作田敦, 土本晃久, 大久保將史, 山田淳夫, 辰巳砂昌弘, 林晃敏

    日本セラミックス協会秋季シンポジウム講演予稿集(CD-ROM)   33rd   2020

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  • Li<sub>2</sub>S based positive electrodes for all-solid-state Li/S batteries with high energy densities

    計賢, 藤田侑志, 出口三奈子, 川崎友輔, 乙山美紗恵, 米田陽平, 作田敦, 辰巳砂昌弘, 林晃敏

    電池討論会PDF要旨集(CD-ROM)   61st   2020

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  • Reaction mechanism of Li<sub>2</sub>S-LiI positive electrode for all-solid-state Li/S batteries

    藤田侑志, 計賢, 出口三奈子, 塚崎裕文, 作田敦, 森茂生, 辰巳砂昌弘, 林晃敏

    電池討論会PDF要旨集(CD-ROM)   61st   2020

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  • Evaluation of Insertion of Zinc Thin Film into the Interface between Lithium Metal Negative Electrode and Li<sub>3</sub>PS<sub>4</sub> Glass Electrolyte

    林晃敏, 稲岡嵩晃, 乙山美紗恵, 作田敦, 辰巳砂昌弘

    日本化学会春季年会講演予稿集(CD-ROM)   100th   2020

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  • Short-circuit suppression by insertion of Sn thin film into Li metal-Li<sub>3</sub>PS<sub>4</sub> glass electrolyte interfaces

    稲岡嵩晃, 乙山美紗恵, 作田敦, 辰巳砂昌弘, 林晃敏

    電池討論会PDF要旨集(CD-ROM)   61st   2020

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  • Mechanochemical synthesis and characterization of sodium ion conductive Na<sub>3</sub>SbS<sub>4-x</sub>O<sub>x</sub> solid electrolytes

    林晃敏, 林晃敏, 高柳拓真, 辻史香, 作田敦, 辰巳砂昌弘

    日本化学会春季年会講演予稿集(CD-ROM)   100th   2020

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  • Mechanochemical Synthesis and Crystal Structure Analysis of Argyrodite-type Li<sub>6</sub>SbS<sub>5</sub>I Electrolytes

    木村拓哉, 保手浜千絵, 藤井孝太郎, 八島正知, 作田敦, 辰巳砂昌弘, 林晃敏

    日本セラミックス協会秋季シンポジウム講演予稿集(CD-ROM)   33rd   2020

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  • Mechanochemical Synthesis and Characterization of Li<sub>5</sub>GaS<sub>4</sub> Solid Electrolytes

    木村拓哉, 保手浜千絵, 作田敦, 辰巳砂昌弘, 林晃敏

    日本セラミックス協会年会講演予稿集(CD-ROM)   2020   2020

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  • Mechanochemical synthesis and structural analysis by using solid-state NMR of Li-B-Si-P-O based glassy electrolytes

    林晃敏, 中野祐輔, 井上文音, 作田敦, 辰巳砂昌弘

    日本化学会春季年会講演予稿集(CD-ROM)   100th   2020

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  • Local Structure of Li<sub>4+2x</sub>P<sub>2-2x</sub>Si<sub>2x</sub>S<sub>7</sub> Glass Electrolytes Prepared via Mechanochemical Process.

    作田敦, 山口穂多瑠, 矢野綾子, 辰巳砂昌弘, 林晃敏

    日本化学会春季年会講演予稿集(CD-ROM)   100th   2020

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  • インジウムやアンチモン置換によるLi<sub>4</sub>SnS<sub>4</sub>の電極活性の向上

    川崎友輔, 岸拓馬, 作田敦, 辰巳砂昌弘, 林晃敏

    化学電池材料研究会ミーティング講演要旨集   21st   2019

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  • アルジロダイト型Li<sub>7-x</sub>PS<sub>6-x</sub>Cl<sub>x</sub>結晶の作製とLi溶解析出特性

    林晃敏, 梅田智仁, 須山元嗣, 由淵想, 作田敦, 辰巳砂昌弘

    日本化学会春季年会講演予稿集(CD-ROM)   99th   2019

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  • Mechanochemical synthesis and characterization of an argyrodite-type Li<sub>6</sub>SbS<sub>5</sub>I electrolyte

    木村拓哉, 保手浜千絵, 作田敦, 辰巳砂昌弘, 林晃敏

    電池討論会PDF要旨集(CD-ROM)   60th   2019

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  • アルジロダイト型Li<sub>6-x</sub>SbS<sub>5-x</sub>I<sub>1+x</sub>の結晶構造解析とイオン伝導度

    木村拓哉, 保手浜千絵, 作田敦, 辰巳砂昌弘, 林晃敏

    固体イオニクス討論会講演要旨集   45th   2019

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  • アセトニトリルを用いたNa<sub>3-x</sub>PS<sub>4-x</sub>Cl<sub>x</sub>固体電解質の液相合成と特性評価

    林晃敏, 伊藤茜, 増澤直貴, 由淵想, 作田敦, 辰巳砂昌弘

    日本化学会春季年会講演予稿集(CD-ROM)   99th   2019

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  • PDF解析を用いた液相合成Li<sub>2</sub>S-P<sub>2</sub>S<sub>5</sub>系固体電解質の局所構造とリチウムイオン伝導度の相関関係の解明

    高橋勝國, 高橋勝國, YANG Seunghoon, 山本健太郎, PHUC Nguyen Huu Huy, 尾原幸治, 内山智貴, 作田敦, 林晃敏, 辰巳砂昌弘, 武藤浩行, 松田厚範, 松永利之, 内本喜晴

    固体イオニクス討論会講演要旨集   45th   2019

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  • Relationship between the local structure and lithium ionic conductivity of Li<sub>2</sub>S-P<sub>2</sub>S<sub>5</sub> solid electrolyte by pair distribution function analysis

    高橋勝國, YANG Seunghoon, 山本健太郎, PHUC Nguyen Huu Huy, 尾原幸治, 内山智貴, 作田敦, 林晃敏, 辰巳砂昌弘, 武藤浩行, 松田厚範, 松永利之, 内本喜晴

    電池討論会PDF要旨集(CD-ROM)   60th   2019

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  • Direct observation of Li metal dendrite growth in all-solid-state batteries by operando CT measurement

    MU Zhiwei, 高橋勝國, XIAO Yao, 鈴木宏睦, 山本健太郎, 内山智貴, 上杉健太朗, 竹内晃久, 作田敦, 林晃敏, 辰巳砂昌弘, 松永利之, 内本喜晴

    電池討論会PDF要旨集(CD-ROM)   60th   2019

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  • Sodium Ion Conductivity of Composite Electrolytes with Na<sub>3</sub>Zr<sub>2</sub>Si<sub>2</sub>PO<sub>12</sub> and Na<sub>3</sub>SbS<sub>4</sub>

    矢野綾子, 由淵想, 長尾賢治, 作田敦, 辰巳砂昌弘, 林晃敏

    電池討論会PDF要旨集(CD-ROM)   60th   2019

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  • Na<sub>2</sub>FeS<sub>2</sub>正極活物質の全固体電池における電極特性評価

    奈須滉, 作田敦, 辰巳砂昌弘, 林晃敏

    固体イオニクス討論会講演要旨集   45th   2019

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  • Suppression of Li metal dendrite growth by interfacial modification between Li metal anode/solid electrolyte

    MU Zhiwei, 高橋勝國, XIAO Yao, 鈴木宏睦, 山本健太郎, 内山智貴, 上杉健太朗, 竹内晃久, 作田敦, 林晃敏, 辰巳砂昌弘, 松永利之, 内本喜晴

    電池討論会PDF要旨集(CD-ROM)   60th   2019

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  • Li<sub>7</sub>P<sub>3</sub>S<sub>11</sub>ベース硫窒化物系固体電解質の作製と評価

    木村拓哉, 福嶋晃弘, 作田敦, 林晃敏, 辰巳砂昌弘

    日本セラミックス協会年会講演予稿集(CD-ROM)   2019   2019

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  • Li<sub>4-x</sub>Sn<sub>1-x</sub>Sb<sub>x</sub>S<sub>4</sub>固溶体の作製と電極活物質としての評価

    作田敦, 川崎友輔, 岸拓馬, 林晃敏, 辰巳砂昌弘

    日本化学会春季年会講演予稿集(CD-ROM)   99th   2019

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  • Ionic conductivity and crystallization process in Li<sub>2</sub>S-P<sub>2</sub>S<sub>5</sub> glass electrolyte

    森茂生, 五十嵐啓介, 塚崎裕文, 和久井亜希子, 矢口紀恵, 乙山美紗恵, 保手浜千絵, 小和田弘枝, 作田敦, 林晃敏, 辰巳砂昌弘

    電池討論会PDF要旨集(CD-ROM)   60th   2019

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  • Li<sub>2</sub>S-P<sub>2</sub>S<sub>5</sub>系ガラス電解質の結晶化プロセスとその場TEM観察

    森茂生, 五十嵐啓介, 塚崎裕文, 和久井亜希子, 矢口紀恵, 乙山美紗恵, 保手浜千絵, 小和田弘枝, 作田敦, 林晃敏, 辰巳砂昌弘

    固体イオニクス討論会講演要旨集   45th   2019

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  • LGPS結晶/Li<sub>3</sub>PS<sub>4</sub>-LiIガラスを用いた固体電解質複合成形体の導電率および機械的特性の評価

    作田敦, 遠地智大, 西村政輝, 林晃敏, 辰巳砂昌弘

    日本化学会春季年会講演予稿集(CD-ROM)   99th   2019

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  • In-situ observation of Li<sub>2</sub>S-P<sub>2</sub>S<sub>5</sub> glass electrolyte crystallization process by hollow cone dark field TEM

    五十嵐啓介, 塚崎裕文, 和久井亜希子, 矢口紀恵, 乙山美紗恵, 作田敦, 林晃敏, 辰巳砂昌弘, 森茂生

    電池討論会PDF要旨集(CD-ROM)   60th   2019

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  • Fe-Li<sub>2</sub>SO<sub>4</sub>系アモルファス電極活物質の作製と酸化物型全固体電池への応用

    作田敦, 徳永晋也, 永田佑佳, 長尾賢治, 林晃敏, 辰巳砂昌弘

    日本化学会春季年会講演予稿集(CD-ROM)   99th   2019

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  • 究極に安全な電池への挑戦 期待広がる全固体リチウムイオン二次電池の実用化

    小林弘典, 倉谷健太郎, 奥村豊旗, 作田敦

    産総研LINK(Web)   ( 22 )   2019( ISSN:2189-6097

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  • 立方晶岩塩型構造を有するNa<sub>2</sub>TiS<sub>3</sub>の構造解析と電極特性の評価

    奈須滉, 乙山美紗恵, 作田敦, 辰巳砂昌弘, 林晃敏

    化学電池材料研究会ミーティング講演要旨集   21st   2019

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  • 耐湿性を有する窒素含有Li<sub>7</sub>P<sub>3</sub>S<sub>11</sub>ベース電解質の開発

    木村拓哉, 福嶋晃弘, 作田敦, 辰巳砂昌弘, 林晃敏

    化学電池材料研究会ミーティング講演要旨集   21st   2019

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  • 金属多硫化物系電極活物質の創製及び常温加圧焼結による次世代電池研究の新展開

    作田敦

    電気化学会大会講演要旨集(CD-ROM)   86th   2019

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  • 非晶質イオニクス材料を用いた全固体電池の開発

    林晃敏, 作田敦, 辰巳砂昌弘

    セラミックス基礎科学討論会講演要旨集   57th   2019

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  • Development of sulfide solid electrolytes prepared by crystallization of mother glasses

    林晃敏, 作田敦, 辰巳砂昌弘

    日本結晶成長学会誌(CD-ROM)   46 ( 1 )   2019( ISSN:2188-7268

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  • 液相場で合成したLi<sub>2</sub>S-P<sub>2</sub>S<sub>5</sub>系固体電解質の構造とイオン伝導度との関係

    高橋勝國, 山本健太郎, PHUC Nguyen Huu Huy, 尾原幸治, 内山智貴, 作田敦, 林晃敏, 辰巳砂昌弘, 武藤浩行, 松田厚範, 内本喜晴

    電気化学会大会講演要旨集(CD-ROM)   86th   2019

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  • 活性炭-硫黄複合体を正極に用いた高容量全固体ナトリウム硫黄電池の作製

    安藤鷹, 由淵想, 作田敦, 林晃敏, 辰巳砂昌弘

    電気化学会大会講演要旨集(CD-ROM)   86th   2019

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  • 多成分系ガラスの結晶化によるSrAl<sub>2</sub>O<sub>4</sub>:Eu<sup>2+</sup>,Dy<sup>3+</sup>長残光性蛍光体の作製

    日下部史也, 松木祐磨, 作田敦, 上田純平, 田部勢津久, 辰巳砂昌弘, 林晃敏

    ガラスおよびフォトニクス材料討論会講演要旨集   60th   2019

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  • Synthesis and characterization of amorphous molybdenum polysulfides as large-capacity electrode active materials with high chemical stability

    作田敦, 古川奉寛, 倉谷健太郎, 竹内友成, 栄部比夏里, 林晃敏, 辰巳砂昌弘

    電池討論会PDF要旨集(CD-ROM)   60th   2019

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  • 全固体電池の革新を目指した新規な固体電解質及び電極活物質の開発

    作田敦, 林晃敏, 辰巳砂昌弘

    日本化学会春季年会講演予稿集(CD-ROM)   99th   2019

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  • 全固体電池とその課題:高イオン伝導固体電解質の開発~固固界面の制御と解析 全固体電池における界面形成とキャラクタリゼーション

    林晃敏, 作田敦, 辰巳砂昌弘

    セラミックス   54 ( 4 )   2019( ISSN:0009-031X

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  • 全固体リチウム電池におけるLi<sub>4</sub>SnS<sub>4</sub>固体電解質を用いた正極複合体の熱安定性評価

    乙山美紗恵, 由淵想, 作田敦, 林晃敏, 辰巳砂昌弘

    電気化学会大会講演要旨集(CD-ROM)   86th   2019

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  • 全固体ナトリウム硫黄電池の開発にむけた硫黄-活性炭複合正極の検討

    安藤鷹, 作田敦, 辰巳砂昌弘, 林晃敏

    化学電池材料研究会ミーティング講演要旨集   21st   2019

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  • 全固体Li金属電池の耐短絡性向上にむけたLi<sub>2</sub>S-P<sub>2</sub>S<sub>5</sub>系ベース固体電解質の探索

    須山元嗣, 作田敦, 林晃敏, 辰巳砂昌弘

    電気化学会大会講演要旨集(CD-ROM)   86th   2019

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  • Development of Li<sub>2</sub>S-V<sub>2</sub>S<sub>3</sub>-LiI as electrode active materials with high ionic and electronic conductivities for all-solid-state Li-S batteries

    作田敦, 岸拓馬, 計賢, 出口三奈子, 林晃敏, 辰巳砂昌弘

    電池討論会PDF要旨集(CD-ROM)   60th   2019

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  • 体積変化率の異なる活物質および正・負極の組み合わせによるレート・サイクル特性への影響

    山本真理, 寺内義洋, 作田敦, 加藤敦隆, 高橋雅也

    日本セラミックス協会年会講演予稿集(CD-ROM)   2019   2019

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  • Diagnosis for All-Solid-State Lithium Metal Cells by X-ray CT

    乙山美紗恵, 須山元嗣, 保手浜千絵, 小和田弘枝, 武田佳彦, 伊藤幸一郎, 作田敦, 辰巳砂昌弘, 林晃敏

    電池討論会PDF要旨集(CD-ROM)   60th   2019

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  • リチウムイオン伝導性Li<sub>4</sub>GeO<sub>4</sub>-Li<sub>2</sub>WO<sub>4</sub>系電解質の作製と評価

    米田陽平, 茂野真成, 長尾賢治, 作田敦, 辰巳砂昌弘, 林晃敏

    化学電池材料研究会ミーティング講演要旨集   21st   2019

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  • リチウムイオン伝導性Li<sub>3</sub>PS<sub>4</sub>-Li<sub>3</sub>SbS<sub>4</sub>ガラス系固体電解質の作製と評価

    木村拓哉, 作田敦, 林晃敏, 辰巳砂昌弘

    電気化学会大会講演要旨集(CD-ROM)   86th   2019

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  • メカノケミカル法を用いたナトリウムイオン伝導性Na<sub>10+x</sub>Sn<sub>1+x</sub>P<sub>2-x</sub>S<sub>12</sub>固体電解質の作製

    辻史香, HOH Kah Loong, MARTIN Steve W., 林晃敏, 林晃敏, 作田敦, 辰巳砂昌弘

    日本セラミックス協会年会講演予稿集(CD-ROM)   2019   2019

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  • Mechanochemical synthesis and characterization of Li<sub>4</sub>SiO<sub>4</sub>-Li<sub>2</sub>SO<sub>4</sub> glass-ceramic electrolytes

    米田陽平, 茂野真成, 長尾賢治, 作田敦, 辰巳砂昌弘, 林晃敏

    電池討論会PDF要旨集(CD-ROM)   60th   2019

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  • メカノケミカル法による立方晶岩塩型Na<sub>2</sub>TiS<sub>3</sub>正極活物質の作製

    奈須滉, 乙山美紗恵, 作田敦, 林晃敏, 辰巳砂昌弘

    電気化学会大会講演要旨集(CD-ROM)   86th   2019

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  • メカノケミカル法によるLi<sub>2</sub>WO<sub>4</sub>ベース酸化物ガラス電解質の作製と評価

    林晃敏, 米田陽平, 茂野真成, 長尾賢治, 作田敦, 辰巳砂昌弘

    日本化学会春季年会講演予稿集(CD-ROM)   99th   2019

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  • メカノケミカル法によるLi<sub>2</sub>S-B<sub>2</sub>S<sub>2</sub>系ガラス電解質の作製とキャラクタリゼーション

    井上文音, 長尾賢治, 作田敦, 辰巳砂昌弘, 林晃敏

    ガラスおよびフォトニクス材料討論会講演要旨集   60th   2019

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  • メカノケミカル法によるEu<sup>2+</sup>,Dy<sup>3+</sup>添加SrAl<sub>2</sub>O<sub>4</sub>ベース長残光蛍光体の作製

    林晃敏, 日下部史也, 松木祐磨, 作田敦, 辰巳砂昌弘

    日本化学会春季年会講演予稿集(CD-ROM)   99th   2019

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  • メカニカルミリングにより複合化したNa<sub>3</sub>Zr<sub>2</sub>Si<sub>2</sub>PO<sub>12</sub>-Na<sub>3</sub>SbS<sub>4</sub>電解質のイオン伝導性

    矢野綾子, 由淵想, 長尾賢治, 作田敦, 林晃敏, 辰巳砂昌弘

    電気化学会大会講演要旨集(CD-ROM)   86th   2019

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  • バルク型全固体電池におけるLi<sub>4</sub>SnS<sub>4</sub>固体電解質を用いた正極複合体の熱安定性と電池特性

    乙山美紗恵, 作田敦, 辰巳砂昌弘, 林晃敏

    化学電池材料研究会ミーティング講演要旨集   21st   2019

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  • Development of Solid Electrolytes for All-Solid-State Batteries

    林晃敏, 作田敦, 辰巳砂昌弘

    日本ゴム協会誌   92 ( 11 )   2019( ISSN:0029-022X

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  • Synthesis and characterization of metastable sodium titanium sulfides as electrode active materials

    奈須滉, 乙山美紗恵, 作田敦, 辰巳砂昌弘, 林晃敏

    電池討論会PDF要旨集(CD-ROM)   60th   2019

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  • Capacity fading mechanism of TiS<sub>4</sub> positive electrode toward the improvement of cycle properties

    倉谷健太郎, 作田敦, 光原圭, 片山真祥, 稲田康宏, 木内久雄, 小林弘典, 竹内友成, 栄部比夏里

    電池討論会PDF要旨集(CD-ROM)   60th   2019

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  • ガラス系電解質を用いた固体界面構築と全固体エネルギー貯蔵デバイスへの応用

    林晃敏, 作田敦, 辰巳砂昌弘

    電気化学会大会講演要旨集(CD-ROM)   86th   2019

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Industrial Property Rights

  • 電極触媒複合体、電極及びこれらの製造方法

    作田 敦, 長谷川 優樹, 林 晃敏

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    Application no:特願2021-032789 

    Announcement no:特開2022-133863 

    J-GLOBAL

  • アルカリ金属電池用の電極活物質、それを含む電極及びアルカリ金属電池

    作田 敦、辰巳砂 昌弘、林 晃敏

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    property_type:Patent 

    Patent/Registration no:PCT/JP2020/38342 

  • 全固体ナトリウム電池用の固体電解質とその製造方法及び全固体ナトリウム電池

    林 晃敏, 辰巳砂 昌弘, 作田 敦

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    property_type:Patent 

    Application no:JP2019028881 

    Publication no:WO2020-022342 

    J-GLOBAL

  • 固体電解質組成物、それを用いた成形体、及び全固体二次電池

    島本 圭, 辰巳砂 昌弘, 林 晃敏, 作田 敦

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    property_type:Patent 

    Application no:特願2019-065062 

    Announcement no:特開2020-166994 

    J-GLOBAL

  • 全固体ナトリウム電池用の固体電解質及び全固体ナトリウム電池

    林 晃敏、辰巳砂 昌弘、作田 敦

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    property_type:Patent 

    Patent/Registration no:特願2019-552777、US 16/762752 

  • 全固体ナトリウム電池用の固体電解質及び全固体ナトリウム電池

    林 晃敏, 辰巳砂 昌弘, 作田 敦

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    property_type:Patent 

    Application no:JP2018041013 

    Publication no:WO2019-093273 

    J-GLOBAL

  • 全固体ナトリウム電池用の固体電解質とその製造方法及び全固体ナトリウム電池

    林 晃敏、辰巳砂 昌弘、作田 敦

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    property_type:Patent 

    Patent/Registration no:PCT/JP2019/ 028881 

  • 低結晶性バナジウム硫化物

    小金井 寿人, 作田 敦, 竹内 友成, 栄部 比夏里, 小林 弘典

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    property_type:Patent 

    Application no:JP2018013204 

    Publication no:WO2018-181698 

    Patent/Registration no:特許第6867713号 

    J-GLOBAL

  • 全固体ナトリウム電池用固体電解質及び全固体ナトリウム電池

    林 晃敏, 辰巳砂 昌弘, 作田 敦

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    property_type:Patent 

    Patent/Registration no:PCT/JP2018/ 041013 

  • リチウムスズ硫化物

    作田 敦, 竹内 友成, 倉谷 健太郎, 栄部 比夏里, 鹿野 昌弘, 小林 弘典

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    property_type:Patent 

    Application no:特願2017-071979 

    Announcement no:特開2018-172244 

    Patent/Registration no:特許第6721912号 

    J-GLOBAL

  • リチウムスズ硫化物

    作田 敦, 倉谷 健太郎, 小林 弘典, 竹内 友成

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    property_type:Patent 

    Application no:特願2017-001810 

    Announcement no:特開2018-111616 

    Patent/Registration no:特許第6950916号 

    J-GLOBAL

  • リチウム-鉄-リン-硫黄-炭素複合体及びその製造方法

    竹内 友成, 蔭山 博之, 作田 敦, 栄部 比夏里

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    property_type:Patent 

    Application no:特願2016-560265 

    Patent/Registration no:特許第6501272号 

    J-GLOBAL

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Collaborative research (seeds) keywords

  • 全固体電池

Outline of collaborative research (seeds)

  • 全固体電池

Grant-in-Aid for Scientific Research

  • ナトリウム二次電池用金属硫化物系電極活物質の開拓

    Grant-in-Aid for Scientific Research(C)  2022.04

  • ホロコーン照射を用いた蓄電固体材料のヘテロ/ホモ界面状態の2次元/3次元構造解析

    Grant-in-Aid for Scientific Research(A)  2022.04

  • 全固体イオニクスデバイスにおける電極複合体ダイナミクスの研究基盤確立

    Grant-in-Aid for Scientific Research(S)  2022.04

  • ナトリウム二次電池用金属硫化物系電極活物質の開拓

    2021

  • ナトリウム二次電池用金属硫化物系電極活物質の開拓

    2020

  • ナトリウム二次電池用金属硫化物系電極活物質の開拓

    2020

  • 非晶質を介する新奇充放電機構を有するナトリウム二次電池用金属硫化物材料の創製

    2019

  • 非晶質を介する新奇充放電機構を有するナトリウム二次電池用金属硫化物材料の創製

    2018

  • 非晶質を介する新奇充放電機構を有するナトリウム二次電池用金属硫化物材料の創製

    2017

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Charge of on-campus class subject

  • 無機材料化学

    2022   Weekly class   Undergraduate

  • 物理化学演習IIA

    2022   Weekly class   Undergraduate

  • 応用化学実験I

    2022   Weekly class   Undergraduate

  • 初年次ゼミナール

    2022   Weekly class   Undergraduate

  • 物質化学生命系特別演習

    2022   Intensive lecture   Graduate school

  • 物質化学生命系特別演習第1

    2022   Intensive lecture   Graduate school

  • 応用化学特論3 (応用化学分野)

    2022   Weekly class   Graduate school

  • 無機材料化学特論 (応用化学分野)

    2022   Weekly class   Graduate school

  • 応用化学実験III

    2022   Weekly class   Undergraduate

  • 物質化学生命系特別研究 (応用化学分野)

    2022   Intensive lecture   Graduate school

  • 物質化学生命系特別演習第2 (応用化学分野)

    2022   Intensive lecture   Graduate school

  • 応用化学実験II

    2022   Weekly class   Undergraduate

  • 応用化学実験IV

    2022   Weekly class   Undergraduate

  • 応用化学実験V

    2022   Weekly class   Undergraduate

  • Advanced Applied Chemistry III

    2021    

  • Laboratory Exercises for Applied Chemistry II

    2021   Practical Training  

  • Laboratory Exercises for Applied Chemistry I

    2021   Practical Training  

  • Laboratory Exercises for Applied Chemistry V

    2021   Practical Training  

  • Laboratory Exercises for Applied Chemistry III

    2021   Practical Training  

  • Inorganic Materials Chemistry

    2021    

  • Exercises in Physical Chemistry IIA

    2021    

  • Laboratory Exercises for Applied Chemistry IV

    2021   Practical Training  

  • Advanced Inorganic Materials Chemistry

    2021    

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Charge of off-campus class subject

  • 応用化学の最前線

    2023.01
    Institution:Tokyo Institute of Technology

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    Level:Postgraduate