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Experimental and theoretical study of multinuclear indium-oxo clusters in CHA zeolite for CH4 activation at room temperature

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Title: Experimental and theoretical study of multinuclear indium-oxo clusters in CHA zeolite for CH4 activation at room temperature
Authors: Maeno, Zen Browse this author →KAKEN DB
Yasumura, Shunsaku Browse this author
Liu, Chong Browse this author
Toyao, Takashi Browse this author →KAKEN DB
Kon, Kenichi Browse this author
Nakayama, Akira Browse this author
Hasegawa, Jun-ya Browse this author →KAKEN DB
Shimizu, Ken-ichi Browse this author →KAKEN DB
Issue Date: 7-Jul-2019
Publisher: Royal Society of Chemistry
Journal Title: Physical chemistry chemical physics
Volume: 21
Issue: 25
Start Page: 13415
End Page: 13427
Publisher DOI: 10.1039/c9cp01873e
Abstract: We have carried out an experimental and theoretical study of CHA-zeolite supported indium (In)-oxo clusters that promote CH4 activation at room temperature. X-ray absorption fine structure (XAFS) measurements indicate the formation of multinuclear In-oxo clusters by the O-2 activation of the In(I)-exchanged CHA zeolite prepared through reductive solid-state ion exchange (RSSIE). The structure of the In-oxo clusters and their locations were investigated in detail using ab initio thermodynamic analysis. The redox properties of the In species during RSSIE and the formation of the In-oxo clusters were also studied by temperature programmed reaction and in situ XAFS measurements. The reaction of CH4 on the O-2-activated In-CHA zeolite was monitored using IR spectroscopy where adsorbed formic acid was generated at room temperature. The adsorption and C-H activation of CH4 on our plausible model of the In-oxo clusters were theoretically investigated using density functional theory calculations. We found that CH4 is likely to adsorb and react more easily on dinuclear In-oxo ions than on monomeric In-oxo ions and that the C-H bond cleavage reaction occurs via a heterolytic pathway rather than a homolytic pathway. This study reveals the potential of multinuclear In-oxo clusters as active sites for the transformation of CH4 to oxygenates under mild reaction conditions.
Type: article (author version)
Appears in Collections:触媒科学研究所 (Institute for Catalysis) > 雑誌発表論文等 (Peer-reviewed Journal Articles, etc)

Submitter: 前野 禅

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