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Huang, M.*; 金城 哲弥*; 安村 駿作*; 鳥屋尾 隆*; 松村 大樹; 齋藤 寛之*; 清水 研一*; 並木 則和*; 前野 禅*
Catalysis Science & Technology, 13(23), p.6832 - 6838, 2023/12
被引用回数:0 パーセンタイル:0(Chemistry, Physical)Ga-exchanged zeolites are promising catalysts for dehydrogenative alkane transformations. Reduced Ga species, such as Ga hydrides and Ga cations, are possible active sites for alkane dehydrogenation based on in situ spectroscopic studies. However, most of the reported studies were conducted at lower temperatures compared with those encountered in actual operating conditions. In this study, the in situ Ga K-edge XANES analysis of Ga-exchanged MFI zeolite was performed under actual operating temperatures and different atmospheres (H, He, CO, vacuum, and CH). The absorption edge appeared at similarly lower energy values than that of GaO in all atmospheres, whereas the main absorption peak intensity differed depending on the presence or absence of a hydride source in the gas phase. Higher intensities were observed under H and CH atmospheres than under CO and vacuum atmospheres.
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:6 パーセンタイル:33.04(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.