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Single atom and defect engineering of CuO for efficient electrochemical reduction of CO 2 to C 2 H 4
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Chu, Senlin, Kang, Changwoo, Park, Woonghyeon, Han, Yu, Hong, Song, Hao, Leiduan, Zhang, Hao, Lo, Tsz Woon Benedict, Robertson, Alex W., Jung, Yousung, Han, Buxing and Sun, Zhenyu (2022) Single atom and defect engineering of CuO for efficient electrochemical reduction of CO 2 to C 2 H 4. SmartMat, 3 (1). pp. 194-205. doi:10.1002/smm2.1105 ISSN 2688-819X.
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Official URL: https://doi.org/10.1002/smm2.1105
Abstract
Electrochemical CO2 transformation to high‐value ethylene (C2H4) at high currents and efficiencies is desired and yet remains a grand challenge. We show for the first time that coupling single Sb atoms and oxygen vacancies of CuO enable synergistic electrocatalytic reduction of CO2 to C2H4 at low overpotentials. Highly dispersed Sb atoms occupying metal substitutional sites of CuO are synthesized under mild conditions. The overall CO2 reduction faradaic efficiency (FE) reaches 89.3 ± 1.1% with an FE toward C2H4 exceeding 58.4% at a high‐current density of 500 mA/cm2. Addition of the p‐block metal is found to induce transformation of CuO from flakes to nanoribbons rich in nanoholes and oxygen vacancies, greatly enhancing CO2 adsorption and activation while suppressing hydrogen evolution. Further density functional theory calculations with in situ X‐ray diffraction reveal that combining Sb sites and oxygen vacancies prominently lessen the dimerization energy of adsorbed CO intermediate, thus boosting the conversion of CO2 to produce C2H4. This study provides a new perspective for promoting selective C–C coupling for electrochemical CO2 reduction.
Item Type: | Journal Article | ||||||||||||
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Subjects: | Q Science > QD Chemistry T Technology > TP Chemical technology |
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Divisions: | Faculty of Science, Engineering and Medicine > Science > Physics | ||||||||||||
SWORD Depositor: | Library Publications Router | ||||||||||||
Library of Congress Subject Headings (LCSH): | Carbon dioxide -- Separation, Copper oxide , Electrocatalysis , Ethylene, Electrochemical analysis , Catalysts | ||||||||||||
Journal or Publication Title: | SmartMat | ||||||||||||
Publisher: | Wiley | ||||||||||||
ISSN: | 2688-819X | ||||||||||||
Official Date: | 30 March 2022 | ||||||||||||
Dates: |
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Volume: | 3 | ||||||||||||
Number: | 1 | ||||||||||||
Page Range: | pp. 194-205 | ||||||||||||
DOI: | 10.1002/smm2.1105 | ||||||||||||
Status: | Peer Reviewed | ||||||||||||
Publication Status: | Published | ||||||||||||
Access rights to Published version: | Open Access (Creative Commons) | ||||||||||||
Date of first compliant deposit: | 4 April 2022 | ||||||||||||
Date of first compliant Open Access: | 4 April 2022 | ||||||||||||
RIOXX Funder/Project Grant: |
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