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Plasma-catalytic Direct Oxidation of Methane to Methanol over Cu-MOR: Revealing the Zeolite-confined Cu 2+ Active Sites
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  • Yanhui Yi,
  • Huan Lv,
  • Shengyan Meng,
  • Zhaolun Cui,
  • Shangkun Li,
  • Dongxing Li,
  • Xiaoxia Gao,
  • Hongchen Guo,
  • Annemie Bogaerts
Yanhui Yi
Dalian University of Technology State Key Laboratory of Fine Chemicals

Corresponding Author:yiyanhui@dlut.edu.cn

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Huan Lv
Dalian University of Technology State Key Laboratory of Fine Chemicals
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Shengyan Meng
Dalian University of Technology State Key Laboratory of Fine Chemicals
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Zhaolun Cui
South China University of Technology Department of Power Engineering
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Shangkun Li
Universiteit Van Antwerpen Onderzoeksgroep Toegepaste Taalkunde
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Dongxing Li
Dalian University of Technology State Key Laboratory of Fine Chemicals
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Xiaoxia Gao
Dalian University of Technology
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Hongchen Guo
Dalian University of Technology State Key Laboratory of Fine Chemicals
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Annemie Bogaerts
Universiteit Van Antwerpen Onderzoeksgroep Toegepaste Taalkunde
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Abstract

Efficient methane conversion to methanol remains a significant challenge in chemical industry. This study investigates the direct oxidation of methane to methanol under mild conditions, employing a synergy of non-thermal plasma and Cu-MOR (Copper-Mordenite) catalysts. Catalytic tests demonstrate that the Cu-MOR IE-3 catalyst (i.e., prepared by three cycles of ion exchange) exhibits superior catalytic performance (with 51% methanol selectivity and 7.9% methane conversion). Conversely, the Cu-MOR catalysts prepared via wetness impregnation tend to over-oxidize CH 4 to CO and CO 2. Through systematic catalyst characterizations (XRD, TPR, UV-Vis, HRTEM, XPS), we elucidate that ion exchange mainly leads to the formation of zeolite-confined Cu 2+ species, while wetness impregnation predominantly results in CuO particles. Based on the catalytic performance, catalyst characterizations and in-situ FTIR spectra, we conclude that zeolite-confined Cu 2+ species serve as the active sites for plasma-catalytic direct oxidation of methane to methanol.
22 Feb 2024Submitted to AIChE Journal
25 Feb 2024Submission Checks Completed
25 Feb 2024Assigned to Editor
25 Feb 2024Review(s) Completed, Editorial Evaluation Pending
02 Mar 2024Reviewer(s) Assigned