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A CHA zeolite supported Ga-oxo cluster for partial oxidation of CH4 at room temperature
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| Title: | A CHA zeolite supported Ga-oxo cluster for partial oxidation of CH4 at room temperature |
| Authors: | Yasumura, Shunsaku Browse this author | | Huang, Mengwen Browse this author | | Wu, Xiaopeng Browse this author | | Liu, Chong Browse this author | | Toyao, Takashi Browse this author →KAKEN DB | | Maeno, Zen Browse this author →KAKEN DB | | Shimizu, Ken-ichi Browse this author →KAKEN DB |
| Keywords: | CH4 activation | | Ga-exchanged zeolite | | Multinuclear Ga-oxo cluster | | In situ XAFS | | DFT calculation |
| Issue Date: | 1-Aug-2020 |
| Publisher: | Elsevier |
| Journal Title: | Catalysis today |
| Volume: | 352 |
| Start Page: | 118 |
| End Page: | 126 |
| Publisher DOI: | 10.1016/j.cattod.2019.10.035 |
| Abstract: | 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. |
| Rights: | © 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/ | | https://creativecommons.org/licenses/by-nc-nd/4.0/ |
| Type: | article (author version) |
| URI: | http://hdl.handle.net/2115/86490 |
| 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)
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Submitter: 前野 禅
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