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Nano Research 2022, 15(9): 7896-7902 https://doi.org/10.1007/s12274-022-4441-0
Research Article | Issue | Published: 04 June 2022

Boosting faradaic efficiency of CO2 electroreduction to CO for Fe-N-C single-site catalysts by stabilizing Fe3+ sites via F-doping

Show Author's Information Yiqun Chen,  Guochang Li,  Yu Zeng,  Lijie Yan,  Xizhang Wang,  Lijun Yang( ),  Qiang Wu( ),  Zheng Hu( )
Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Lab for Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China
Keywords:
single-site catalysts, carbon dioxide electroreduction, iron-nitrogen-carbon, fluorine-doping, active site regulation
Topics:
Electrocatalysts
Cite this article:
Chen Y, Li G, Zeng Y, et al. Boosting faradaic efficiency of CO2 electroreduction to CO for Fe-N-C single-site catalysts by stabilizing Fe3+ sites via F-doping. Nano Research, 2022, 15(9): 7896-7902. https://doi.org/10.1007/s12274-022-4441-0
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Abstract Full text Electronic supplementary material About this article

The atomically dispersed Fe3+ sites of Fe-N-C single-site catalysts (SSCs) are demonstrated as the active sites for CO2 electroreduction (CO2RR) to CO but suffer from the reduction to Fe2+ at ~ −0.5 V, accompanied by the drop of CO faradaic efficiency (FECO) and deterioration of partial current (JCO). Herein, we report the construction of F-doped Fe-N-C SSCs and the electron-withdrawing character of fluorine could stabilize Fe3+ sites, which promotes the FECO from the volcano-like highest value (88.2%@−0.40 V) to the high plateau (> 88.5%@−0.40–−0.60 V), with a much-increasedJCO (from 3.24 to 11.23 mA·cm−2). The enhancement is ascribed to the thermodynamically facilitated CO2RR and suppressed competing hydrogen evolution reaction, as well as the kinetically increased electroactive surface area and improved charge transfer, due to the stabilized Fe3+ sites and enriched defects by fluorine doping. This finding provides an efficient strategy to enhance the CO2RR performance of Fe-N-C SSCs by stabilizing Fe3+.


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About this article

Boosting faradaic efficiency of CO2 electroreduction to CO for Fe-N-C single-site catalysts by stabilizing Fe3+ sites via F-doping

Show Author's information Yiqun Chen, Guochang Li, Yu Zeng, Lijie Yan, Xizhang Wang, Lijun Yang( ), Qiang Wu( ), Zheng Hu( )
Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Lab for Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China

Abstract

The atomically dispersed Fe3+ sites of Fe-N-C single-site catalysts (SSCs) are demonstrated as the active sites for CO2 electroreduction (CO2RR) to CO but suffer from the reduction to Fe2+ at ~ −0.5 V, accompanied by the drop of CO faradaic efficiency (FECO) and deterioration of partial current (JCO). Herein, we report the construction of F-doped Fe-N-C SSCs and the electron-withdrawing character of fluorine could stabilize Fe3+ sites, which promotes the FECO from the volcano-like highest value (88.2%@−0.40 V) to the high plateau (> 88.5%@−0.40–−0.60 V), with a much-increasedJCO (from 3.24 to 11.23 mA·cm−2). The enhancement is ascribed to the thermodynamically facilitated CO2RR and suppressed competing hydrogen evolution reaction, as well as the kinetically increased electroactive surface area and improved charge transfer, due to the stabilized Fe3+ sites and enriched defects by fluorine doping. This finding provides an efficient strategy to enhance the CO2RR performance of Fe-N-C SSCs by stabilizing Fe3+.

Keywords: single-site catalysts, carbon dioxide electroreduction, iron-nitrogen-carbon, fluorine-doping, active site regulation

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Publication history
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Acknowledgements

Publication history

Received: 10 March 2022
Revised: 06 April 2022
Accepted: 15 April 2022
Published: 04 June 2022
Issue date: September 2022

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was jointly supported by the National Key Research and Development Program of China (Nos. 2021YFA1500900, 2017YFA0206500, and 2018YFA0209103), the National Natural Science Foundation of China (Nos. 21832003, 21972061, and 52071174), the Natural Science Foundation of Jiangsu Province, Major Project (No. BK20212005), and Nanjing University Innovation Program for PhD candidate (No. CXYJ21-38).

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