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Selective electroreduction of CO2 and CO to C2H4 by synergistically tuning nanocavities and the surface charge of copper oxide
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Li, Xin, Li, Lifen, Xia, Qineng, Hong, Song, Hao, Leiduan, Robertson, Alex W., Zhang, Hao, Benedict Lo, Tsz Woon and Sun, Zhenyu (2022) Selective electroreduction of CO2 and CO to C2H4 by synergistically tuning nanocavities and the surface charge of copper oxide. ACS Sustainable Chemistry & Engineering, 10 (19). pp. 6466-6475. doi:10.1021/acssuschemeng.2c01600 ISSN 2168-0485.
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WRAP-Selective-electroreduction-CO2-CO- C2H4-synergistically-tuning-copper-oxide-2022.pdf - Accepted Version - Requires a PDF viewer. Download (1542Kb) | Preview |
Official URL: https://doi.org/10.1021/acssuschemeng.2c01600
Abstract
Electroreduction of CO2 and CO to high-value chemicals and fuels continues to be a grand challenge. Here, we report synergistic electrolysis of CO2 and CO to C2H4 by concurrently tuning nanocavities and the interface of CuO with a hydrogen evolution inactive metal oxide (ZrO2). The designed CuO@ZrO2 delivers a faradaic efficiency (FE) as high as 54.7 ± 1.1% toward C2H4 formation and a remarkable overall CO2 reduction FE exceeding 84.0% at 250 mA cm–2, significantly outperforming pristine CuO and many recently demonstrated Cu-based catalysts. The composite also exhibits a markedly enhanced FE of converting CO to C2H4, approximately three-fold that of pure CuO. Operando Raman spectroscopy as well as postmortem X-ray photoelectron spectroscopy measurements verify that Cu+ species are well retained in the presence of ZrO2 during CO2 reduction, in stark contrast to the rapid transformation of Cu+ to Cu0 in the catalyst without the metal oxide. Experiments in combination with theoretical calculations further show that the incorporation of ZrO2 substantially decreases the dimerization barriers of adsorbed CO intermediates, thus boosting C–C coupling to produce C2H4.
| Item Type: | Journal Article | ||||||||||||
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| Subjects: | Q Science > QD Chemistry T Technology > TD Environmental technology. Sanitary engineering |
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| Divisions: | Faculty of Science, Engineering and Medicine > Science > Physics | ||||||||||||
| Library of Congress Subject Headings (LCSH): | Electrolytic reduction, Electrocatalysis, Carbon dioxide mitigation, Carbon monoxide | ||||||||||||
| Journal or Publication Title: | ACS Sustainable Chemistry & Engineering | ||||||||||||
| Publisher: | American Chemical Society | ||||||||||||
| ISSN: | 2168-0485 | ||||||||||||
| Official Date: | 16 May 2022 | ||||||||||||
| Dates: |
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| Volume: | 10 | ||||||||||||
| Number: | 19 | ||||||||||||
| Page Range: | pp. 6466-6475 | ||||||||||||
| DOI: | 10.1021/acssuschemeng.2c01600 | ||||||||||||
| Status: | Peer Reviewed | ||||||||||||
| Publication Status: | Published | ||||||||||||
| Reuse Statement (publisher, data, author rights): | This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Sustainable Chemistry & Engineering, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://dx.doi.org/10.1021/acssuschemeng.2c01600.” | ||||||||||||
| Access rights to Published version: | Restricted or Subscription Access | ||||||||||||
| Copyright Holders: | American Chemical Society | ||||||||||||
| Date of first compliant deposit: | 8 June 2022 | ||||||||||||
| Date of first compliant Open Access: | 4 May 2023 | ||||||||||||
| RIOXX Funder/Project Grant: |
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