TY - JOUR
T1 - Activation of light alkanes at room temperature and ambient pressure
AU - Zhang, Haochen
AU - Li, Chunsong
AU - Liu, Wenxuan
AU - Luo, Guangsheng
AU - Goddard, William A.
AU - Cheng, Mu Jeng
AU - Xu, Bingjun
AU - Lu, Qi
N1 - Publisher Copyright:
© 2023, The Author(s), under exclusive licence to Springer Nature Limited.
PY - 2023/8
Y1 - 2023/8
N2 - 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.]
AB - 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.]
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U2 - 10.1038/s41929-023-00990-9
DO - 10.1038/s41929-023-00990-9
M3 - Article
AN - SCOPUS:85165253032
SN - 2520-1158
VL - 6
SP - 666
EP - 675
JO - Nature Catalysis
JF - Nature Catalysis
IS - 8
ER -