Electrochemical reduction of CO2 to ethane through stabilization of an ethoxy intermediate

Vasileff, Anthony and Zhu, Yanping and Zhi, Xing and Zhao, Yongqiang and Ge, Lei ORCID: https://orcid.org/0000-0003-2989-0329 and Chen, Hao Ming and Zheng, Yao and Qiao, Shi-Zhang (2020) Electrochemical reduction of CO2 to ethane through stabilization of an ethoxy intermediate. Angewandte Chemie - International Edition, 59 (4). pp. 19649-19653. ISSN 1433-7851


Abstract

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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Item Type: Article (Commonwealth Reporting Category C)
Refereed: Yes
Item Status: Live Archive
Additional Information: Permanent restricted access to Published version, in accordance with the copyright policy of the publisher.
Faculty/School / Institute/Centre: Current - Institute for Advanced Engineering and Space Sciences - Centre for Future Materials (1 Jan 2017 -)
Faculty/School / Institute/Centre: Current - Institute for Advanced Engineering and Space Sciences - Centre for Future Materials (1 Jan 2017 -)
Date Deposited: 14 Dec 2020 06:11
Last Modified: 27 Jan 2021 23:49
Uncontrolled Keywords: CO2 reduction; copper catalysts; in situ spectroscopy; Raman; XAFS
Fields of Research (2008): 03 Chemical Sciences > 0306 Physical Chemistry (incl. Structural) > 030601 Catalysis and Mechanisms of Reactions
09 Engineering > 0904 Chemical Engineering > 090402 Catalytic Process Engineering
Fields of Research (2020): 40 ENGINEERING > 4004 Chemical engineering > 400404 Electrochemical energy storage and conversion
34 CHEMICAL SCIENCES > 3406 Physical chemistry > 340601 Catalysis and mechanisms of reactions
Socio-Economic Objectives (2020): 19 ENVIRONMENTAL POLICY, CLIMATE CHANGE AND NATURAL HAZARDS > 1903 Mitigation of climate change > 190301 Climate change mitigation strategies
17 ENERGY > 1703 Energy storage, distribution and supply > 170304 Energy storage (excl. hydrogen and batteries)
Identification Number or DOI: https://doi.org/10.1002/anie.202004846
URI: http://eprints.usq.edu.au/id/eprint/40367

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