A CHA zeolite supported Ga-oxo cluster for partial oxidation of CH4 at room temperature

Yasumura, Shunsaku; Huang, Mengwen; Wu, Xiaopeng; Liu, Chong; Toyao, Takashi; Maeno, Zen; Shimizu, Ken-ichi

A CHA zeolite supported Ga-oxo cluster for partial oxidation of CH4 at room temperature

Yasumura, Shunsaku; Huang, Mengwen; Wu, Xiaopeng et al.

Catalysis today, 2020, 352, 118-126

Permalink : https://hdl.handle.net/2115/86490

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論文情報

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アクセス権	open access
URI	https://hdl.handle.net/2115/86490
タイトル	A CHA zeolite supported Ga-oxo cluster for partial oxidation of CH4 at room temperature
著者	Yasumura, Shunsaku ; Huang, Mengwen ; Wu, Xiaopeng ; Liu, Chong ; Toyao, Takashi ; Maeno, Zen ; Shimizu, Ken-ichi
著者名 Yasumura, Shunsaku
著者名 Huang, Mengwen
著者名 Wu, Xiaopeng
著者名 Liu, Chong
e-Rad_Researcher 80775388 著者名 Toyao, Takashi
e-Rad_Researcher 30721154 著者名 Maeno, Zen
e-Rad_Researcher 60324000 著者名 Shimizu, Ken-ichi
言語	英語
キーワード	CH4 activation
	Ga-exchanged zeolite
	Multinuclear Ga-oxo cluster
	In situ XAFS
	DFT calculation
発行日	2020-08-01
出版者	Elsevier
収録物名	Catalysis today
巻(号)	352
ページ	118-126
抄録	A catalytic system for activation of CH4 under mild conditions is in high demand. In this study, Ga-oxo clusters in CHA zeolites were prepared by reductive solid-state ion-exchange followed by O-2 treatment. Formation of the Ga-oxo clusters was demonstrated using X-ray absorption fine structure (XAFS) measurements. Plausible models of the cluster were developed by using an ab initio thermodynamic analysis. Importantly, the CHA zeolite-supported Ga-oxo clusters promote partial oxidation of CH4 to yield adsorbed formaldehyde and formic acid. The results of density functional theory (DFT) calculations, designed to gain information about the mechanism of the process, show that the Z(2)[Ga-2(O)(OH)(2)] is likely the most active cluster for C-H bond activation of CH4. Observations made in this experimental and theoretical effort demonstrate that main-group metal-oxo clusters have the potential of serving as active species for transformations of CH4.
資源タイプ	学術雑誌論文
出版タイプ	Accepted Manuscript
権利情報	Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International
権利情報	© 2020. This manuscript version is made available under the CC-BY-NC-ND 4.0 license https://creativecommons.org/licenses/by-nc-nd/4.0/
PISSN	0920-5861
関連情報 (isVersionOf)	出版社版DOI https://doi.org/10.1016/j.cattod.2019.10.035