4.8 Article

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

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 44, Pages 19649-19653

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202004846

Keywords

CO2 reduction; copper catalysts; in situ spectroscopy; Raman; XAFS

Funding

  1. Australian Research Council (ARC) [FL170100154, DP160104866, DP170104464]
  2. Australian Government

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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.

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