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Quantifying the density and utilization of active sites in non-precious metal oxygen electroreduction catalysts

Author

Listed:
  • Nastaran Ranjbar Sahraie

    (The Electrochemical Energy, Catalysis and Material Science Laboratory, Technical University Berlin)

  • Ulrike I. Kramm

    (Technical University Darmstadt
    Technical University Darmstadt)

  • Julian Steinberg

    (The Electrochemical Energy, Catalysis and Material Science Laboratory, Technical University Berlin)

  • Yuanjian Zhang

    (School of Chemistry and Chemical Engineering, Southeast University)

  • Arne Thomas

    (Technical University Berlin)

  • Tobias Reier

    (The Electrochemical Energy, Catalysis and Material Science Laboratory, Technical University Berlin)

  • Jens-Peter Paraknowitsch

    (Technical University Berlin)

  • Peter Strasser

    (The Electrochemical Energy, Catalysis and Material Science Laboratory, Technical University Berlin)

Abstract

Carbon materials doped with transition metal and nitrogen are highly active, non-precious metal catalysts for the electrochemical conversion of molecular oxygen in fuel cells, metal air batteries, and electrolytic processes. However, accurate measurement of their intrinsic turn-over frequency and active-site density based on metal centres in bulk and surface has remained difficult to date, which has hampered a more rational catalyst design. Here we report a successful quantification of bulk and surface-based active-site density and associated turn-over frequency values of mono- and bimetallic Fe/N-doped carbons using a combination of chemisorption, desorption and 57Fe Mössbauer spectroscopy techniques. Our general approach yields an experimental descriptor for the intrinsic activity and the active-site utilization, aiding in the catalyst development process and enabling a previously unachieved level of understanding of reactivity trends owing to a deconvolution of site density and intrinsic activity.

Suggested Citation

  • Nastaran Ranjbar Sahraie & Ulrike I. Kramm & Julian Steinberg & Yuanjian Zhang & Arne Thomas & Tobias Reier & Jens-Peter Paraknowitsch & Peter Strasser, 2015. "Quantifying the density and utilization of active sites in non-precious metal oxygen electroreduction catalysts," Nature Communications, Nature, vol. 6(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:6:y:2015:i:1:d:10.1038_ncomms9618
    DOI: 10.1038/ncomms9618
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    Cited by:

    1. Jiaming Miao & Cheng Lin & Xiaojia Yuan & Yang An & Yan Yang & Zhaosheng Li & Kan Zhang, 2024. "Supramolecular catalyst with [FeCl4] unit boosting photoelectrochemical seawater splitting via water nucleophilic attack pathway," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Wanlin Zhou & Hui Su & Weiren Cheng & Yuanli Li & Jingjing Jiang & Meihuan Liu & Feifan Yu & Wei Wang & Shiqiang Wei & Qinghua Liu, 2022. "Regulating the scaling relationship for high catalytic kinetics and selectivity of the oxygen reduction reaction," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    3. Lopes, Thiago & Beruski, Otavio & Manthanwar, Amit M. & Korkischko, Ivan & Pugliesi, Reynaldo & Stanojev, Marco Antonio & Andrade, Marcos Leandro Garcia & Pistikopoulos, Efstratios N. & Perez, Joelma , 2019. "Spatially resolved oxygen reaction, water, and temperature distribution: Experimental results as a function of flow field and implications for polymer electrolyte fuel cell operation," Applied Energy, Elsevier, vol. 252(C), pages 1-1.

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