掲載種別：研究論文（学術雑誌）  

DOI： 10.1021/acsami.5c00484

掲載種別：研究論文（学術雑誌）  

Understanding how support materials influence the properties of Pt nanoparticles is crucial for advancing catalyst development. Using density functional theory calculations, we examine the effects of graphene, MgO(100), α-Al2O3(0001), and SnO2(110) supports on O atom adsorption and the stability, electronic, and geometric properties of Pt33 nanoparticles. Our findings reveal that all supports significantly enhance O atom adsorption at the Pt33/support interface, with varying implications for Pt atom detachment and nanoparticle stability. The strength of Pt–support interactions follows the order: graphene < MgO(100) < α-Al2O3(0001) < SnO2(110). Bond order analysis indicates that supports stabilize the Pt–Pt interactions in the supported Pt33 and their outer shell atoms. Electronic equilibrium between Pt33 and the support induces electron transfer from graphene, MgO(100), and α-Al2O3(0001) to Pt33, and from Pt33 to SnO2(110), shifting the d-band center and influencing catalytic properties. Strain analysis reveals compressive and tensile effects on Pt–Pt distances, correlating with the Pt33 adsorption energies and indicating a link between geometric changes and nanoparticle stability. These insights elucidate the role of supports in O atom adsorption mechanisms and the tuning of Pt nanoparticle properties, providing valuable guidance for designing advanced catalysts with enhanced efficiency and stability for applications in fuel cells, sensors, and environmental remediation.

DOI： 10.1016/j.susc.2024.122686

掲載種別：研究論文（学術雑誌）  

Abstract

The applicability of multicomponent quantum mechanical (MC_QM) approach was assessed by calculating the H/D isotope effect on the electronic absorption spectra of small molecules. The calculated excitation energy of the water molecule increased upon H/D substitution, a trend consistent with the experimentally observed peak shift in the absorption cross-section. This increase in excitation energy was primarily attributed to changes in the highest occupied molecular orbital, driven by a reduction in nuclear quantum fluctuations due to isotope substitution. Similar trends were observed in the absorption spectra of ethylene, hexatriene, and biphenyl, reinforcing the generality of these findings. These results suggest that MC_QM is an efficient method for evaluating H/D isotope effects on ultraviolet–visible spectra without requiring vibrational analysis. Furthermore, the approach provides a clear connection between spectral changes and alterations in molecular orbitals induced by isotope substitution.

DOI： 10.1093/chemle/upaf031

その他URL： https://academic.oup.com/chemlett/article-pdf/54/2/upaf031/61900318/upaf031.pdf

掲載種別：研究論文（学術雑誌）  

Direct CO2 conversion to liquid hydrocarbons (HCs) in a single process was achieved using cobalt (Co) catalysts supported on lanthanum ion (La3+)‐doped cerium oxide (CeO2) under a gas stream of H2/CO2/N2 = 3/1/1. The yield of liquid HCs was the highest for 30 mol% of La3+‐doped CeO2, which was because extrinsic oxygen vacancy formed by doping La3+ could act as an effective reaction site for reverse water gas shift reaction. However, the excess La3+ addition afforded surface covering lanthanum carbonates, resulting in depression of the catalytic performance. On the other hand, bare CeO2 lead to an increase in the selectivity of undesirable methane, which arose from reduction of CO2 to CO proceeding by intrinsic oxygen vacancy generated by only Ce3+, and weaker CO2 capture ability of intrinsic oxygen vacancy than extrinsic one, resulting in the proceeding of Sabatier reaction on Co catalyst. The rational design of reaction sites presented in this study will contribute to sustainability.

DOI： 10.1002/cctc.202400261

掲載種別：研究論文（学術雑誌）  

DOI： 10.1016/j.mtcomm.2024.108379