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In-situ electrochemical restructuring of Cu2BiSx solid solution into Bi/CuxSy heterointerfaces enabling stabilization intermediates for high-performance CO2 electroreduction to formate

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Abstract

Bismuth-based materials are prevalent catalysts for CO2 electroreduction to formate, enduring high hydrogen evolution reactions and inadequate activity and stability. Herein, we reveal that in-situ electrochemical transformation of Cu2BiSx solid solution into Bi/CuxSy heterointerfaces, which can stabilize the intermediates and achieve highly selective and consistent CO2 electroreduction. It shows over 85% Faraday efficiency (FE) of formate with a potential window of −0.8 to −1.2 VRHE (RHE: reversible hydrogen electrode) and a stability above 90% over 27 h in H-type cell at −0.9 VRHE. It maintains more than 85% of FEformate at the current density of −25 to −200 mA·cm−2, and has stability of about 80% of FEformate at least 10 h at −150 mA·cm−2 in flow cell. In-situ Fourier transform infrared (FT-IR) spectroscopy measurement confirms that the preferred route of catalytic reaction is to generate *CO2− and *OCHO intermediates. The density functional theory (DFT) calculations illustrate that heterointerfaces facilitate the prior process of CO2 to HCOOH through *OCHO by additional Bi hybrid orbitals. This study is expected to open up a new idea for the design of CO2 electroreduction catalyst.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 21871005 and 22171005) and the University Synergy Innovation Program of Anhui Province (Nos. GXXT-2020-005, GXXT-2021-012, and GXXT-2021-013).

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Authors and Affiliations

  1. College of Chemistry and Materials Science, the Key Laboratory of Electrochemical Clean Energy of Anhui Higher Education Institutes, Anhui Provincial Engineering Laboratory for New-Energy Vehicle Battery Energy-Storage Materials, Anhui Normal University, Wuhu, 241002, China

    Xiaofeng Yang, Qinru Wang, Feiran Chen, Hu Zang, Changjiang Liu, Nan Yu & Baoyou Geng

  2. Institute of Energy, Hefei Comprehensive National Science Center, Hefei, 230031, China

    Baoyou Geng

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  1. Xiaofeng Yang
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Correspondence to Baoyou Geng.

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In-situ electrochemical restructuring of Cu2BiSx solid solution into Bi/CuxSy heterointerfaces enabling stabilization intermediates for high-performance CO2 electroreduction to formate

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Yang, X., Wang, Q., Chen, F. et al. In-situ electrochemical restructuring of Cu2BiSx solid solution into Bi/CuxSy heterointerfaces enabling stabilization intermediates for high-performance CO2 electroreduction to formate. Nano Res. 16, 7974–7981 (2023). https://doi.org/10.1007/s12274-022-5337-8

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