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Nano Research 2023, 16(5): 7974-7981 https://doi.org/10.1007/s12274-022-5337-8
Research Article | Issue | Published: 13 February 2023

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

Show Author's Information Xiaofeng Yang1,  Qinru Wang1,  Feiran Chen1,  Hu Zang1,  Changjiang Liu1,  Nan Yu1,  Baoyou Geng1,2( )
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
Institute of Energy, Hefei Comprehensive National Science Center, Hefei 230031, China
Keywords:
CO2 electroreduction, formate, in-situ electrochemical restructuring, heterointerfaces, current density
Topics:
ElectrodesNanorodsNanostructured materialsSulfur compounds
Cite this article:
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 Research, 2023, 16(5): 7974-7981. https://doi.org/10.1007/s12274-022-5337-8
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Abstract Full text Electronic supplementary material About this article

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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About this article

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

Show Author's information Xiaofeng Yang1, Qinru Wang1, Feiran Chen1, Hu Zang1, Changjiang Liu1, Nan Yu1, Baoyou Geng1,2( )
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
Institute of Energy, Hefei Comprehensive National Science Center, Hefei 230031, China

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.

Keywords: CO2 electroreduction, formate, in-situ electrochemical restructuring, heterointerfaces, current density

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Publication history
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Acknowledgements

Publication history

Received: 30 October 2022
Revised: 15 November 2022
Accepted: 15 November 2022
Published: 13 February 2023
Issue date: May 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

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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