Boosting Direct Oxidation of Methane with Molecular Oxygen at Low Temperature over Rh/ZSM-5 Catalyst
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作者
Yu, Xing; Mao, Jianing; Wu, Bo; Wei, Yao; Sun, Yuhan; Zhong, Liangshu
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刊物名称
CHEMCATCHEM
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年、卷、文献号
2023, , 1867-3899
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关键词
Yu, Xing; Mao, Jianing; Wu, Bo; Wei, Yao; Sun, Yuhan; Zhong, Liangshu
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摘要
As a clean fossil energy and chemical feedstock, development of breakthrough strategies for direct conversion of methane (CH4) into various chemicals under mild reaction conditions is highly desired. Herein, Rh/ZSM-5 catalyst was reported to convert CH4 to oxygenates with molecular oxygen (O-2) in the presence of CO at low temperature with promising catalytic performance. The oxygenates productivity reached as high as 5638.0 mu mol g(cat.)(-1) h(-1). Structure characterization confirmed the existence of highly dispersed Rh2O3 nanoparticles with an average diameter of 2.4 nm in the Rh/ZSM-5 catalyst. Based on control experiments and mechanism study, it was suggested that CO plays a pivotal role over the Rh/ZSM-5 catalyst to boost direct oxidation of methane. CO participates in water-gas-shift reaction to produce in-situ H species, which enables to form *OH, *OOH and H2O2 active species by reacting with O-2. The as-obtained *OH, *OOH and H2O2 species will thus render high activity for methane oxidation.
