Electrochemical Reduction of CO2 to Ethane through Stabilization of an Ethoxy Intermediate

被引:151
作者
Vasileff, Anthony [1 ]
Zhu, Yanping [2 ]
Zhi, Xing [1 ]
Zhao, Yongqiang [1 ]
Ge, Lei [3 ]
Chen, Hao Ming [2 ]
Zheng, Yao [1 ]
Qiao, Shi-Zhang [1 ]
机构
[1] Univ Adelaide, Sch Chem Engn & Adv Mat, Adelaide, SA 5005, Australia
[2] Natl Taiwan Univ, Dept Chem, Taipei 106, Taiwan
[3] Univ Southern Queensland, Ctr Future Mat, Springfield Cent, Qld 4300, Australia
基金
澳大利亚研究理事会;
关键词
CO2; reduction; copper catalysts; in situ spectroscopy; Raman; XAFS; CARBON-DIOXIDE; CU; COPPER; ELECTROREDUCTION; SELECTIVITY; SURFACE; RAMAN; SPECTROSCOPY; EVOLUTION; ETHYLENE;
D O I
10.1002/anie.202004846
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Electrochemical conversion of CO2 into ethane is seldom observed because of the generally higher selectivity towards methane, ethylene, and ethanol. Consequently, little experimental evidence for its reaction mechanism exists and thus remains largely unknown. Now, by combining electrochemistry with in situ X-ray absorption fine-structure and in situ Raman techniques, iodide-derived copper (ID-Cu) and oxide-derived copper (OD-Cu) systems were studied to obtain a deeper understanding of the CO2 to ethane mechanism. With trace iodine species on the surface and positively charged Cu species, production of ethane is significantly more favored on ID-Cu compared to OD-Cu, with higher selectivity and faster kinetics. For the first time, it is experimentally found that the formation of ethane follows the same pathway to ethylene and ethanol, and better stabilization of the late stage ethoxy intermediate can steer the reaction to ethane over ethanol.
引用
收藏
页码:19649 / 19653
页数:5
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