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Direct measurement of the oxygen reduction reaction kinetics on iron phthalocyanine using advanced transient voltammetry

Nature Catalysis volume 7, pages 139–147 (2024)Cite this article

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Abstract

Platinum group metal (PGM)-free catalysts are promising candidates to replace PGM catalysts for the oxygen reduction reaction in fuel cells. While methodologies to determine the number of active sites are under intense development, experimentally quantifying the parameters governing the kinetics of the reaction remains rare, albeit its potential for paving the pathways for future catalysts development. The use of transient voltammetry to probe electrocatalytic reactions by varying the measurement timescales and quantifying the reaction parameters via detailed microkinetic models has shown immense success in uncovering hidden mechanistic insights, connecting theory and experiments. Here we present the application of Fourier-transformed alternating-current voltammetry for analysis of the oxygen reduction reaction electrocatalysis on a model PGM-free catalyst, iron-phthalocyanine, to decipher the kinetic and thermodynamic parameters governing the reaction. These parameters are used to shed light on the limiting steps governing the reaction and to present possible avenues to increase the performance of PGM-free catalysts.

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Fig. 1: Rotating ring disc measurement and CV of FePc adsorbed on XC72.
Fig. 2: FTacV measurements.
Fig. 3: Comparison between the experimental and simulated FTacV harmonics.
Fig. 4: Comparison of simulated and experimental kinetic currents.
Fig. 5: Experimentally determined free-energy diagrams.
Fig. 6: Simulated kinetic currents, redox and adsorption kinetics constants.

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All data and codes are available from the authors upon request.

Code availability

All simulations in this work were conducted using codes available for download on GitHub (https://github.com/Snitkoff-Sol/Reaction-parameters-of-ORR.git).

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Acknowledgements

This work was conducted in the framework of the Israeli Fuel Cells and Hydrogen Consortium (IFCC), and the Hydrogen Technologies Center (H2Tech), part of the Israel National Institute for Sustainable Energy (NISE). It was supported by the Israel Ministry of Energy, The Israel Ministry of Science, and the Israel Science Foundation (ISF). R.Z.S.-S. thanks the Israeli Ministry of Energy for his fellowship.

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Authors and Affiliations

  1. Department of Chemistry, Bar-Ilan Center for Nanotechnology and Advanced Materials, Bar-Ilan University, Ramat-Gan, Israel

    Rifael Z. Snitkoff-Sol, Or Rimon & Lior Elbaz

  2. School of Chemistry, Monash University, Clayton, Victoria, Australia

    Alan M. Bond

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R.Z.S.-S. contributed to the ideation of this work, conducted most of the experiments in this work, wrote the model and simulation, analysed most of the data, and contributed to the writing of this manuscript. O.R. helped with some of the FTacV measurements, A.M.B. contributed to the analysis and provided valuable insights, and L.E. contributed to the ideation of this work, analysis and writing of this manuscript.

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Correspondence to Lior Elbaz.

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Snitkoff-Sol, R.Z., Rimon, O., Bond, A.M. et al. Direct measurement of the oxygen reduction reaction kinetics on iron phthalocyanine using advanced transient voltammetry. Nat Catal 7, 139–147 (2024). https://doi.org/10.1038/s41929-023-01086-0

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