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Highly active and stable stepped Cu surface for enhanced electrochemical CO₂ reduction to C₂H₄

Choi, Chungseok and Kwon, Soonho and Cheng, Tao and Xu, Mingjie and Tieu, Peter and Lee, Changsoo and Cai, Jin and Lee, Hyuck Mo and Pan, Xiaoqing and Duan, Xiangfeng and Goddard, William A., III and Huang, Yu (2020) Highly active and stable stepped Cu surface for enhanced electrochemical CO₂ reduction to C₂H₄. Nature Catalysis, 3 (10). pp. 804-812. ISSN 2520-1158. https://resolver.caltech.edu/CaltechAUTHORS:20200723-121126169

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Abstract

Electrochemical CO₂ reduction to value-added chemical feedstocks is of considerable interest for renewable energy storage and renewable source generation while mitigating CO₂ emissions from human activity. Copper represents an effective catalyst in reducing CO₂ to hydrocarbons or oxygenates, but it is often plagued by a low product selectivity and limited long-term stability. Here we report that copper nanowires with rich surface steps exhibit a remarkably high Faradaic efficiency for C₂H₄ that can be maintained for over 200 hours. Computational studies reveal that these steps are thermodynamically favoured compared with Cu(100) surface under the operating conditions and the stepped surface favours C₂ products by suppressing the C₁ pathway and hydrogen production.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1038/s41929-020-00504-xDOIArticle
https://rdcu.be/b6WbjPublisherFree ReadCube access
ORCID:
AuthorORCID
Choi, Chungseok0000-0001-9169-1393
Kwon, Soonho0000-0002-9225-3018
Cheng, Tao0000-0003-4830-177X
Tieu, Peter0000-0001-8727-2313
Lee, Hyuck Mo0000-0003-4556-6692
Pan, Xiaoqing0000-0002-0965-8568
Duan, Xiangfeng0000-0002-4321-6288
Goddard, William A., III0000-0003-0097-5716
Huang, Yu0000-0003-1793-0741
Alternate Title:Highly Active and Stable Stepped Cu Surface for Enhanced Electrochemical CO2 Reduction to C2H4
Additional Information:© 2020 Nature Publishing Group. Received 08 July 2019; Accepted 30 July 2020; Published 07 September 2020. The TEM work was conducted using the facilities in the Electron Imaging Center at the California NanoSystems Institute at the University of California Los Angles and the Irvine Materials Research Institute at the University of California Irvine. C.C., J.C., X.D. and Y.H. acknowledge support from the Office of Naval Research (ONR) under grant no. N000141712608. S.K., T.C. and W.A.G. were supported by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the US Department of Energy under Award no. DE-SC0004993. C.L., S.K. and H.M.L. used the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation grant no. ACI-1548562. C.L. and H.M.L. were also supported by a National Research Foundation (NRF) of Korea grant funded by the Korean Government (no. NRF-2017R1E1A1A03071049). The work done at the University of California Irvine was supported by the Irvine Materials Research Institute and ExxonMobil. Data availability: The data that support the findings of this study are available from the corresponding authors upon reasonable request. Author Contributions: C.C. designed and conducted most of the experiments, analysed all the data and prepared the manuscript. S.K., T.C. and W.A.G. performed the density theoretical calculations and prepared the manuscript. M.X., P.T. and X.P. took SEI and bright-field scanning transmission electron microscopy images. J.C., C.L., H.M.L and X.D. assisted in the experiments and the preparation of the manuscript. Y.H. initiated the study, oversaw the project and wrote the manuscript. All the authors discussed the results and contributed to the manuscript. The authors declare no competing interests.
Group:JCAP
Funders:
Funding AgencyGrant Number
Office of Naval Research (ONR)N000141712608
Joint Center for Artificial Photosynthesis (JCAP)UNSPECIFIED
Department of Energy (DOE)DE-SC0004993
NSFACI-1548562
National Research Foundation of KoreaNRF-2017R1E1A1A03071049
Irvine Materials Research InstituteUNSPECIFIED
ExxonMobilUNSPECIFIED
Subject Keywords:Electrocatalysis; Heterogeneous catalysis
Other Numbering System:
Other Numbering System NameOther Numbering System ID
WAG1391
Issue or Number:10
Record Number:CaltechAUTHORS:20200723-121126169
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20200723-121126169
Official Citation:Choi, C., Kwon, S., Cheng, T. et al. Highly active and stable stepped Cu surface for enhanced electrochemical CO2 reduction to C2H4. Nat Catal 3, 804–812 (2020). https://doi.org/10.1038/s41929-020-00504-x
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:104529
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:08 Sep 2020 19:36
Last Modified:27 Nov 2020 18:29

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