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

Nastaran Ranjbar Sahraie, Ulrike I. Kramm (), Julian Steinberg, Yuanjian Zhang, Arne Thomas, Tobias Reier, Jens-Peter Paraknowitsch and Peter Strasser ()
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Nastaran Ranjbar Sahraie: The Electrochemical Energy, Catalysis and Material Science Laboratory, Technical University Berlin
Ulrike I. Kramm: 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

Nature Communications, 2015, vol. 6, issue 1, 1-9

Abstract: 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.

Date: 2015
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DOI: 10.1038/ncomms9618

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