Highly Selective Electrocatalytic Reduction of CO₂ into Methane on Cu–Bi Nanoalloys
Creators
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1.
Harbin Institute of Technology
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2.
Soochow University
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3.
Canadian Light Source (Canada)
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4.
Harbin Medical University
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5.
California Institute of Technology
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.
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.Attached Files
Supplemental Material - jz0c01261_si_001.pdf
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Additional details
Additional titles
- Alternative title
- Highly Selective Electrocatalytic Reduction of CO2 into Methane on Cu–Bi Nanoalloys
Identifiers
- Eprint ID
- 104531
- DOI
- 10.1021/acs.jpclett.0c01261
- Resolver ID
- CaltechAUTHORS:20200723-122438908
Related works
- Describes
- 10.1021/acs.jpclett.0c01261 (DOI)
Funding
- National Natural Science Foundation of China
- 51572062
- National Natural Science Foundation of China
- 81771903
- National Natural Science Foundation of China
- 21972034
- Department of Energy (DOE)
- DE-SC0004993
- NSF
- ACI-1053575
- Suzhou Nano Science and Technology
- Priority Academic Program Development of Jiangsu Higher Education Institutions
- Canada Foundation for Innovation
- Natural Sciences and Engineering Research Council of Canada (NSERC)
- National Research Council of Canada
- Canadian Institutes of Health Research (CIHR)
- Government of Saskatchewan
- University of Saskatchewan
Dates
- Created
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2020-07-24Created from EPrint's datestamp field
- Updated
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2021-11-16Created from EPrint's last_modified field