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Chemical looping conversion of ethane to ethanol via photo-assisted nitration of ethane
Cell Reports Physical Science ( IF 7.9 ) Pub Date : 2021-06-28 , DOI: 10.1016/j.xcrp.2021.100481
Xuefeng He , Zhe Li , Huihui Hu , Jiawei Chen , Lingzhen Zeng , Jingzheng Zhang , Wenbin Lin , Cheng Wang

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 (O2) 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°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.



中文翻译:

通过乙烷的光辅助硝化将乙烷化学循环转化为乙醇

乙烷是一种丰富且廉价的碳氢化合物。乙烷选择性转化为乙醇具有经济价值,但由于过度氧化而难以实现。在这里,我们报告了一种化学循环策略,用于使用分子氧 (O 2 ) 作为最终氧化剂和二氧化氮 (NO 2 ) 作为中继氧化剂将乙烷 (C 2 H 6 )选择性转化为乙醇 (C 2 H 5 OH) . 可见光用于激发 NO 2以驱动与 C 2 H 6的自由基反应生成硝酸乙酯(C 2 H 5 ONO 2) 在 -10°C 下,选择性 >80%,乙烷转化率 >90%。C 2 H 5 ONO 2水解生成C 2 H 5 OH和硝酸(HNO 3 ),从而完成乙烷转化为乙醇的化学回路。DFT 计算表明,光的引入克服了乙烷在较低温度下活化的障碍,从而避免了硝酸乙酯的分解和过氧化,从而导致硝酸乙酯的高选择性。

更新日期:2021-07-21
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