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Universal electrochemical quantification of active site density in transition metal nitrogen carbon electrocatalysts

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  • Guang Li

    (Xiamen University, State Key Laboratory of Physical Chemistry of Solid Surfaces, Engineering Research Center of Electrochemical Technologies of Ministry of Education, College of Chemistry and Chemical Engineering)

  • Shu-Hu Yin

    (Nantong University, School of Microelectronics and Integrated Circuits (Jiangsu Key Laboratory of Semi. Dev. & IC Design, Package and Test))

  • Li-Fei Ji

    (Xiamen University, State Key Laboratory of Physical Chemistry of Solid Surfaces, Engineering Research Center of Electrochemical Technologies of Ministry of Education, College of Chemistry and Chemical Engineering)

  • Xu-Yuan Nie

    (Chongqing University, Center of Advanced Electrochemical Energy, Institute of Advanced Interdisciplinary Studies; School of Chemistry and Chemical Engineering)

  • Ting Zhu

    (Nantong University, School of Microelectronics and Integrated Circuits (Jiangsu Key Laboratory of Semi. Dev. & IC Design, Package and Test))

  • Xiao-Yang Cheng

    (Xiamen University, State Key Laboratory of Physical Chemistry of Solid Surfaces, Engineering Research Center of Electrochemical Technologies of Ministry of Education, College of Chemistry and Chemical Engineering)

  • Jun Xu

    (Nantong University, School of Microelectronics and Integrated Circuits (Jiangsu Key Laboratory of Semi. Dev. & IC Design, Package and Test))

  • Rui Huang

    (Xiamen University, State Key Laboratory of Physical Chemistry of Solid Surfaces, Engineering Research Center of Electrochemical Technologies of Ministry of Education, College of Chemistry and Chemical Engineering)

  • Yan-Xia Jiang

    (Xiamen University, State Key Laboratory of Physical Chemistry of Solid Surfaces, Engineering Research Center of Electrochemical Technologies of Ministry of Education, College of Chemistry and Chemical Engineering)

  • Bin-Wei Zhang

    (Chongqing University, Center of Advanced Electrochemical Energy, Institute of Advanced Interdisciplinary Studies; School of Chemistry and Chemical Engineering)

  • Shi-Gang Sun

    (Xiamen University, State Key Laboratory of Physical Chemistry of Solid Surfaces, Engineering Research Center of Electrochemical Technologies of Ministry of Education, College of Chemistry and Chemical Engineering
    Chongqing University, Center of Advanced Electrochemical Energy, Institute of Advanced Interdisciplinary Studies; School of Chemistry and Chemical Engineering)

Abstract

In-situ electrochemical nitrite reduction is an established method to quantify site density (SD) of platinum-group-metal-free catalysts for PEM fuel cells. However, its poisoning mechanism remains unclear, often yielding underestimated values. Crucially, we identify a unique configuration where single metal centers adsorb two NO molecules, which challenges conventional electrochemical quantification. To resolve this, we developed an in-situ acid-assisted nitrite poisoning method (AANPM) coupled with graphene-based attenuated total reflection Fourier transform infrared spectroscopy (graphene-based in-situ ATR-FTIR). This approach quantifies SD and elucidates active site structures in transition metal-nitrogen-carbon (MNC) electrocatalysts. By incorporating the average electron transfer number for NO electroreduction (NOR), we achieve accurate SD calculations. Validated across iron/cobalt phthalocyanine molecular catalysts and pyrolyzed FeNC/CoNC materials, this method can be used to stablish structure-activity relations.

Suggested Citation

  • Guang Li & Shu-Hu Yin & Li-Fei Ji & Xu-Yuan Nie & Ting Zhu & Xiao-Yang Cheng & Jun Xu & Rui Huang & Yan-Xia Jiang & Bin-Wei Zhang & Shi-Gang Sun, 2025. "Universal electrochemical quantification of active site density in transition metal nitrogen carbon electrocatalysts," Nature Communications, Nature, vol. 16(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-65614-1
    DOI: 10.1038/s41467-025-65614-1
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