Chemical Looping Conversion Of Ethane To Ethanol Via Photo-Assisted Nitration Of Ethane

CELL REPORTS PHYSICAL SCIENCE(2021)

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摘要
Ethane is an abundant and cheap hydrocarbon. Selective conversion of ethane to ethanol has economic value but is difficult to achieve due to overoxidation. Here, we report a chemical looping strategy established to selectively convert ethane (C2H6) to ethanol (C2H5OH) using molecular oxygen (O-2) as the end oxidant and nitrogen dioxide (NO2) as a relay oxidant. Visible light is used to excite NO2 to drive a radical reaction with C2H6 to produce ethyl nitrate (C2H5ONO2) at-10 degrees C with a selectivity of >80% and an ethane conversion of >90%. C2H5ONO2 is hydrolyzed to generate C2H5OH and nitric acid (HNO3), thus completing a chemical loop for the conversion of ethane to ethanol. DFT calculations show that the introduction of light overcomes the barrier of ethane activation at a relatively low temperature and thus avoids ethyl nitrate decomposition and overoxidation, leading to the high selectivity of ethyl nitrate.
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关键词
ethane nitration,NO2,photoactivation,chemical looping,ethanol formation
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