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吉田 寿雄*; 山本 旭*; 細川 三郎*; 山添 誠司*; 吉川 聡一*; 原 賢二*; 中村 充孝; 蒲沢 和也*; 田中 庸裕*
Topics in Catalysis, 64(9-12), p.660 - 671, 2021/08
被引用回数:2 パーセンタイル:12.08(Chemistry, Applied)Inelastic neutron scattering (INS) enables direct and selective observation of H species due to the extremely large incoherent neutron scattering cross section of a hydrogen atom. In the present study, the adsorbed H species on some heterogeneous precious metal catalysts supported by alumina and carbon black were investigated by in situ INS spectroscopy with a newly designed sample cell. Three alumina-supported metal catalysts having Pt, Pd, and Rh metal nanoparticles with different particle sizes exhibited different INS spectra in intensities and band distribution. Observation of the H species on the metal nanoparticles and the alumina surface revealed their properties. In addition, the H atoms stored in Pd nanoparticles were observed as palladium hydride. In contrast, the H species on a Pt catalyst supported by carbon black were found to be strongly adsorbed on the carbon support.
山添 誠司*; 山本 旭*; 細川 三郎*; 福田 良一*; 原 賢二*; 中村 充孝; 蒲沢 和也*; 佃 達哉*; 吉田 寿雄*; 田中 庸裕*
Catalysis Science & Technology, 11(1), p.116 - 123, 2021/01
被引用回数:5 パーセンタイル:35.71(Chemistry, Physical)Hydrogen (H) species adsorbed on catalyst surfaces are key intermediates in catalytic hydrogenation reactions over supported metal catalysts. However, individual identification of H species on the metal catalysts has not been established to date. Here, we elucidated the H species on Pt/AlO by the combination of inelastic neutron scattering (INS) and density functional theory (DFT). Several H species in the presence of H were successfully identified at different sites on the Pt surface and AlO support. The INS and FT-IR measurements revealed that the hydride/atop Pt-H, bridged perimeter/terrace Pt-H-Pt, and threefold Pt-H are active intermediates in the CH hydrogenation reaction, whereas the edge Pt-H-Pt is a rather inert species. In addition, the measurements indicate that the AlO itself acts as hydrogen storage material by mediating AlO-H and Al-H-Al species, which serve H species in the CH hydrogenation reaction.