已核实 DOI 相关产品: 106

Activation of light alkanes at room temperature and ambient pressure

Journal 2023 · IF 37.8 · 6(8): 666-675 · 发表于 2023 年 7 月 20 日
作者: Zhang Haochen,Li Chunsong,Liu Wenxuan,Luo Guangsheng,Goddard William A.,Cheng Mu-Jeng,Xu Bingjun,Lu Qi
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摘要

Light alkane activation under mild conditions remains a substantial challenge. Here we report an aqueous reaction system capable of selectively converting light alkanes into corresponding olefins and oxygenates at room temperature and ambient pressure using Cu powder as the catalyst and O 2 as the oxidant. In ethane activation, we achieved a combined production of ethylene and acetic acid at a rate of 2.27 mmol g Cu −1  h −1 , with a combined selectivity up to 97%. Propane is converted to propylene with a selectivity up to 94% and a production rate up to 1.83 mmol g Cu −1  h −1 , while methane is converted mainly to carbon dioxide, methanol and acetic acid. On the basis of catalytic experiments, isotopic labelling experiments, spectroscopic insights and density functional theory calculations, we put forward mechanistic understandings in which the C–H bond is activated by the surface oxide species generated during the oxidation process, forming alkyl groups as key reaction intermediates.

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