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Computational and experimental demonstrations of one-pot tandem catalysis for electrochemical carbon dioxide reduction to methane

Zhang, Haochen and Chang, Xiaoxia and Chen, Jingguang G. and Goddard, William A., III and Xu, Bingjun and Cheng, Mu-Jeng and Lu, Qi (2019) Computational and experimental demonstrations of one-pot tandem catalysis for electrochemical carbon dioxide reduction to methane. Nature Communications, 10 . Art. No. 3340. ISSN 2041-1723. PMCID PMC6659690.

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Electroreduction of carbon dioxide to hydrocarbons and oxygenates on copper involves reduction to a carbon monoxide adsorbate followed by further transformation to hydrocarbons and oxygenates. Simultaneous improvement of these processes over a single reactive site is challenging due to the linear scaling relationship of the binding strength of key intermediates. Herein, we report improved electroreduction of carbon dioxide by exploiting a one-pot tandem catalysis mechanism based on computational and electrochemical investigations. By constructing a well-defined copper-modified silver surface, adsorbed carbon monoxide generated on the silver sites is proposed to migrate to surface copper sites for the subsequent reduction to methane, which is consistent with insights gained from operando attenuated total reflectance surface enhanced infrared absorption spectroscopic investigations. Our results provide a promising approach for designing carbon dioxide electroreduction catalysts to enable one-pot reduction of products beyond carbon monoxide and formate.

Item Type:Article
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URLURL TypeDescription CentralArticle
Zhang, Haochen0000-0002-2774-5868
Chang, Xiaoxia0000-0001-6598-6083
Chen, Jingguang G.0000-0002-9592-2635
Goddard, William A., III0000-0003-0097-5716
Xu, Bingjun0000-0002-2303-257X
Cheng, Mu-Jeng0000-0002-8121-0485
Lu, Qi0000-0002-0380-2629
Additional Information:© 2019 The Author(s). 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 16 December 2018; Accepted 30 June 2019; Published 26 July 2019. Data availability: The data that support the findings of this study are available from the corresponding author upon request. 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 numbers 21872079, 21606142). W.A.G. is supported by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award Number DE-SC0004993. X.C. and B.X. acknowledge the support of the National Science Foundation CAREER Program (Award No. CBET-1651625). 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. Author Contributions: H.Z., M.-J.C., and Q.L. conceived and designed both computational and electrochemical investigations and wrote the manuscript. H.Z. and M.-J.C. performed DFT calculations and analyzed the data. H.Z. and Q.L. carried out the electrocatalytic tests and analyzed the results. H.Z. and Q.L. performed electron microscopy studies, FIB, XPS, and analyzed these data. X.C. and B.X. performed ATR-SEIRAS experiments and analyzed the results. J.G.C., W.A.G., and B.X. contributed to data analysis and writing of this manuscript. The authors declare no competing interests.
Funding AgencyGrant Number
National Key Research and Development Program of China2017YFA0208200
National Natural Science Foundation of China21872079
National Natural Science Foundation of China21606142
Joint Center for Artificial Photosynthesis (JCAP)UNSPECIFIED
Department of Energy (DOE)DE-SC0004993
Ministry of Science and Technology (Taipei)107-2113-M-006-008-MY2
Subject Keywords:Electrocatalysis; Electrochemistry
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PubMed Central ID:PMC6659690
Record Number:CaltechAUTHORS:20190730-090851748
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:97511
Deposited By: Tony Diaz
Deposited On:30 Jul 2019 17:33
Last Modified:03 Oct 2019 21:32

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