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

Wang, Zhijiang; Yuan, Qi; Shan, Jingjing; Jiang, Zhaohua; Xu, Ping; Hu, Yongfeng; Zhou, Jigang; Wu, Lina; Niu, Zhuangzhuang; Sun, Jianmin; Cheng, Tao; Goddard, William A.

doi:10.1021/acs.jpclett.0c01261

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

Journal Article · 22 July 2020 · Journal of Physical Chemistry Letters

DOI: https://doi.org/10.1021/acs.jpclett.0c01261 · OSTI ID:1801625

^[1]; Yuan, Qi ^[2]; Shan, Jingjing ^[3]; Jiang, Zhaohua ^[3];

^[3]; Hu, Yongfeng ^[4];

^[4];

^[5]; Niu, Zhuangzhuang ^[3];

^[3];

^[6];

^[7]

Harbin Institute of Technology (China); OSTI
Soochow University, Suzhou (China)
Harbin Institute of Technology (China)
Canadian Light Source (CLS), Saskatoon, SK (Canada)
Harbin Medical University (China)
Soochow University, Suzhou (China); California Institute of Technology (CalTech), Pasadena, CA (United States)
California Institute of Technology (CalTech), Pasadena, CA (United States)

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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Research Organization:: California Institute of Technology (CalTech), Pasadena, CA (United States)

Sponsoring Organization:: National Natural Science Foundation of China (NSFC); National Science Foundation (NSF); USDOE Office of Science (SC)

Grant/Contract Number:: SC0004993

OSTI ID:: 1801625

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 17 Vol. 11; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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

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