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論文

Observation of adsorbed hydrogen species on supported metal catalysts by inelastic neutron scattering

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.

論文

Identification of hydrogen species on Pt/Al$$_{2}$$O$$_{3}$$ by ${it in situ}$ inelastic neutron scattering and their reactivity with ethylene

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/Al$$_{2}$$O$$_{3}$$ by the combination of ${it in situ}$ inelastic neutron scattering (INS) and density functional theory (DFT). Several H species in the presence of H$$_{2}$$ were successfully identified at different sites on the Pt surface and Al$$_{2}$$O$$_{3}$$ support. The ${it in situ}$ INS and FT-IR measurements revealed that the hydride/atop Pt-H, bridged perimeter/terrace Pt-H-Pt, and threefold Pt$$_{3}$$-H are active intermediates in the C$$_{2}$$H$$_{4}$$ hydrogenation reaction, whereas the edge Pt-H-Pt is a rather inert species. In addition, the ${it in situ}$ measurements indicate that the Al$$_{2}$$O$$_{3}$$ itself acts as hydrogen storage material by mediating AlO-H and Al-H-Al species, which serve H species in the C$$_{2}$$H$$_{4}$$ hydrogenation reaction.

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