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Insight into the synergistic effect between plasma and oxygen vacancy in direct oxidation of CH4 to CH3OH by molecular O2 at mild condition

Journal 2024 · IF 4.7 · 发表于 2024 年 10 月 11 日
作者: Kai Li,Junqi Cai,Yue Tao,Yunhe Xing,Zuchao Zhu,Zhiqiang Lu,Xuming Zhang
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摘要

The direct conversion of methane into the value-added chemical methanol using molecular oxygen was investigated via plasma catalysis under mild condition. An efficient synergistic effect between plasma and catalyst was achieved using an oxygen vacancy-rich ZnO/Al 2 O 3 catalyst. A high methanol selectivity of 48.5 % and a high synergy factor of 2.1 could be achieved simultaneously over ZnO/Al 2 O 3 R300 catalyst. The presence of oxygen vacancies played a crucial role in methanol formation. A close relationship between oxygen vacancy content and methanol selectivity was established. In situ DRIFT and optical emission spectra were employed to identify key intermediates, and a plausible reaction mechanism was proposed. The CH 3 and CH 3 O species were the key intermediates on the catalyst surface. The oxygen vacancy could efficiently adsorb the O radicals and accelerate the formation of CH 3 O species. This work offers insights into the rational engineering of efficient catalyst for plasma catalysis process.

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