Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 11, Issue 17, Pages 7261-7266Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.0c01261
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Funding
- National Natural Science Foundation of China [51572062, 81771903, 21972034]
- Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub - Office of Science of the U.S. Department of Energy [DE-SC0004993]
- National Science Foundation [ACI-1053575]
- Fund for Collaborative Innovation Center of Suzhou Nano Science Technology
- Canada Foundation for Innovation (CFI)
- Natural Sciences and Engineering Research Council (NSERC)
- National Research Council (NRC)
- Canadian Institutes of Health Research (CIHR)
- Government of Saskatchewan
- University of Saskatchewan
- the Priority Academic Program Development of Jiangsu Higher Education Institutions
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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.
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