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Oxygen induced promotion of electrochemical reduction of CO₂ via co-electrolysis

He, Ming and Li, Chunsong and Zhang, Haochen and Chang, Xiaoxia and Chen, Jingguang G. and Goddard, William A., III and Cheng, Mu-jeng and Xu, Bingjun and Lu, Qi (2020) Oxygen induced promotion of electrochemical reduction of CO₂ via co-electrolysis. Nature Communications, 11 . Art. No. 3844. ISSN 2041-1723. PMCID PMC7395777.

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Harnessing renewable electricity to drive the electrochemical reduction of CO₂ is being intensely studied for sustainable fuel production and as a means for energy storage. Copper is the only monometallic electrocatalyst capable of converting CO₂ to value-added products, e.g., hydrocarbons and oxygenates, but suffers from poor selectivity and mediocre activity. Multiple oxidative treatments have shown improvements in the performance of copper catalysts. However, the fundamental underpinning for such enhancement remains controversial. Here, we combine reactivity, in-situ surface-enhanced Raman spectroscopy, and computational investigations to demonstrate that the presence of surface hydroxyl species by co-electrolysis of CO₂ with low concentrations of O₂ can dramatically enhance the activity of copper catalyzed CO2 electroreduction. Our results indicate that co-electrolysis of CO₂ with an oxidant is a promising strategy to introduce catalytically active species in electrocatalysis.

Item Type:Article
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URLURL TypeDescription CentralArticle
He, Ming0000-0001-5392-503X
Li, Chunsong0000-0002-8016-1896
Zhang, Haochen0000-0002-2774-5868
Chen, Jingguang G.0000-0002-9592-2635
Goddard, William A., III0000-0003-0097-5716
Cheng, Mu-jeng0000-0002-8121-0485
Xu, Bingjun0000-0002-2303-257X
Additional Information:© The Author(s) 2020. This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit Received 31 March 2020; Accepted 14 July 2020; Published 31 July 2020. This work is supported by the National Key Research and Development Program of China (Grant Number 2017YFA0208200) and the National Natural Science Foundation of China (Grant Number 21872079). X.C. and B.X. acknowledge the support of the National Science Foundation CAREER Program (Award No. CBET-1651625). W.A.G. is supported by the US National Science Foundation (CBET-1805022). M.-j.C. acknowledges financial support from the Ministry of Science and Technology of the Republic of China under Grant No. MOST 107-2113-M-006-008-MY2. Data availability: The data that support the findings of this study are available from the corresponding author upon request. Author Contributions: These authors contributed equally: Ming He, Chunsong Li. Q.L. conceived and designed the project. M.H. and C.L. carried out the electrocatalytic tests and physical characterizations. X.C. and B.X. performed in situ SERS experiments. H.Z. and M.-j.C. performed DFT calculations. J.G.C. and W.A.G. contributed to data analysis and writing of this manuscript. These authors contributed equally: M.H. and C.L. The authors declare no competing interests.
Funding AgencyGrant Number
National Key Research and Development Program of China2017YFA0208200
National Natural Science Foundation of China21872079
Ministry of Science and Technology (China)MOST 107-2113-M-006-008-MY2
Subject Keywords:Catalytic mechanisms; Electrocatalysis
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PubMed Central ID:PMC7395777
Record Number:CaltechAUTHORS:20200803-093757604
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Official Citation:He, M., Li, C., Zhang, H. et al. Oxygen induced promotion of electrochemical reduction of CO2 via co-electrolysis. Nat Commun 11, 3844 (2020).
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:104697
Deposited By: Tony Diaz
Deposited On:03 Aug 2020 17:05
Last Modified:01 Sep 2020 22:28

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