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Highly Selective Electrocatalytic Reduction of CO₂ into Methane on Cu–Bi Nanoalloys

Wang, Zhijiang and Yuan, Qi and Shan, Jingjing and Jiang, Zhaohua and Xu, Ping and Hu, Yongfeng and Zhou, Jigang and Wu, Lina and Niu, Zhuangzhuang and Sun, Jianmin and Cheng, Tao and Goddard, William A., III (2020) Highly Selective Electrocatalytic Reduction of CO₂ into Methane on Cu–Bi Nanoalloys. Journal of Physical Chemistry Letters, 11 (17). pp. 7261-7266. ISSN 1948-7185. https://resolver.caltech.edu/CaltechAUTHORS:20200723-122438908

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Abstract

Methane (CH₄), the main component of natural gas, is one of the most valuable products facilitating energy storage via electricity conversion. However, the poor selectivity and high overpotential for CH₄ formation with metallic Cu catalysts prevent realistic applications. Introducing a second element to tune the electronic state of Cu has been widely used as an effective method to improve catalytic performance, but achieving high selectivity and activity toward CH₄ remains challenging. Here, we successfully synthesized Cu–Bi NPs, which exhibit a CH₄ Faradaic efficiency (FE) as high as 70.6% at −1.2 V versus reversible hydrogen electrode (RHE). The FE of Cu–Bi NPs has increased by approximately 25-fold compared with that of Cu NPs. DFT calculations showed that alloying Cu with Bi significantly decreases the formation energy of *COH formation, the rate-determining step, which explains the improved performance. Further analysis showed that Cu that has been partially oxidized because of electron withdrawal by Bi is the most possible active site.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acs.jpclett.0c01261DOIArticle
ORCID:
AuthorORCID
Wang, Zhijiang0000-0001-9314-7922
Xu, Ping0000-0002-7984-776X
Zhou, Jigang0000-0001-6644-2862
Cheng, Tao0000-0003-4830-177X
Goddard, William A., III0000-0003-0097-5716
Alternate Title:Highly Selective Electrocatalytic Reduction of CO2 into Methane on Cu–Bi Nanoalloys
Additional Information:© 2020 American Chemical Society. Received: April 25, 2020; Accepted: July 23, 2020; Published: July 23, 2020. This work was supported by the National Natural Science Foundation of China (51572062, 81771903, and 21972034). This work was 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 No. DE-SC0004993. The computations used the Extreme Science and Engineering Discovery Environment (XSEDE) which is supported by National Science Foundation Grant Number ACI-1053575. This work is also a project supported by the Fund for Collaborative Innovation Center of Suzhou Nano Science & Technology, the Priority Academic Program Development of Jiangsu Higher Education Institutions. XAS analysis was performed at the Canadian Light Source, a national research facility of the University of Saskatchewan, which is supported by the Canada Foundation for Innovation (CFI), the Natural Sciences and Engineering Research Council (NSERC), the National Research Council (NRC), the Canadian Institutes of Health Research (CIHR), the Government of Saskatchewan, and the University of Saskatchewan. The authors declare no competing financial interest.
Group:JCAP
Funders:
Funding AgencyGrant Number
National Natural Science Foundation of China51572062
National Natural Science Foundation of China81771903
National Natural Science Foundation of China21972034
Department of Energy (DOE)DE-SC0004993
NSFACI-1053575
Suzhou Nano Science and TechnologyUNSPECIFIED
Priority Academic Program Development of Jiangsu Higher Education InstitutionsUNSPECIFIED
Canada Foundation for InnovationUNSPECIFIED
Natural Sciences and Engineering Research Council of Canada (NSERC)UNSPECIFIED
National Research Council of CanadaUNSPECIFIED
Canadian Institutes of Health Research (CIHR)UNSPECIFIED
Government of SaskatchewanUNSPECIFIED
University of SaskatchewanUNSPECIFIED
Subject Keywords:CO2 reduction reaction; Cu alloy; methane; DFT; faraday efficiency
Other Numbering System:
Other Numbering System NameOther Numbering System ID
WAG1387
Issue or Number:17
Record Number:CaltechAUTHORS:20200723-122438908
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20200723-122438908
Official Citation:Highly Selective Electrocatalytic Reduction of CO2 into Methane on Cu–Bi Nanoalloys. Zhijiang Wang, Qi Yuan, Jingjing Shan, Zhaohua Jiang, Ping Xu, Yongfeng Hu, Jigang Zhou, Lina Wu, Zhuangzhuang Niu, Jianmin Sun, Tao Cheng, and William A. Goddard. The Journal of Physical Chemistry Letters 2020 11 (17), 7261-7266; DOI: 10.1021/acs.jpclett.0c01261
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:104531
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:24 Jul 2020 14:32
Last Modified:08 Sep 2020 19:40

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