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Plasma-catalytic direct oxidation of methane to methanol over Cu-MOR: Revealing the zeolite-confined Cu2+ active sites

Journal 2024 · IF 13.3 · 发表于 2024 年 8 月 2 日
作者: Huan Lv,Shengyan Meng,Zhaolun Cui,Shangkun Li,Dongxing Li,Xiaoxia Gao,Hongchen Guo,Annemie Bogaerts,Yanhui Yi
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摘要

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.