Activation of light alkanes at room temperature and ambient pressure

Haochen Zhang, Chunsong Li, Wenxuan Liu, Guangsheng Luo, William A. Goddard, Mu Jeng Cheng, Bingjun Xu, Qi Lu

研究成果: Article同行評審

4 引文 斯高帕斯(Scopus)

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 O2 as the oxidant. In ethane activation, we achieved a combined production of ethylene and acetic acid at a rate of 2.27 mmol gCu−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 gCu−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. [Figure not available: see fulltext.]

原文English
頁(從 - 到)666-675
頁數10
期刊Nature Catalysis
6
發行號8
DOIs
出版狀態Published - 2023 8月

All Science Journal Classification (ASJC) codes

  • 催化
  • 生物工程
  • 生物化學
  • 製程化學與技術

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