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The stability number as a metric for electrocatalyst stability benchmarking

Nature Catalysis volume 1, pages 508–515 (2018)Cite this article

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Abstract

Reducing the noble metal loading and increasing the specific activity of the oxygen evolution catalysts are omnipresent challenges in proton-exchange-membrane water electrolysis, which have recently been tackled by utilizing mixed oxides of noble and non-noble elements. However, proper verification of the stability of these materials is still pending. Here we introduce a metric to explore the dissolution processes of various iridium-based oxides, defined as the ratio between the amounts of evolved oxygen and dissolved iridium. The so-called stability number is independent of loading, surface area or involved active sites and provides a reasonable comparison of diverse materials with respect to stability. The case study on iridium-based perovskites shows that leaching of the non-noble elements in mixed oxides leads to the formation of highly active amorphous iridium oxide, the instability of which is explained by the generation of short-lived vacancies that favour dissolution. These insights are meant to guide further research, which should be devoted to increasing the utilization of highly durable pure crystalline iridium oxide and finding solutions to stabilize amorphous iridium oxides.

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Fig. 1: Crystal structure of the investigated materials.
Fig. 2: XPS results for pristine Ba2PrIrO6, amorphous IrOx and crystalline IrO2.
Fig. 3: Investigation of iridium dissolution during OER.
Fig. 4: Comparison of the investigated materials in terms of activity.
Fig. 5: Online observation of lattice oxygen evolution.
Fig. 6: Sketch of the simplified OER reaction mechanism with dissolution pathways.
Fig. 7: Investigation of S–number and lifetime depending on the current load.

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Acknowledgements

The authors acknowledge funding by the German Federal Ministry of Education and Research (BMBF) within the Kopernikus Project P2X and a further project (Kz: 033RC1101A). S.G. acknowledges financial support from BASF. O.K. acknowledges financial support from the Alexander von Humboldt Foundation. E.P. and T.O. acknowledge financial support from the IMPRS-SurMat doctoral program. K.J.J.M. acknowledges financial support from the DFG under project number MA4819/4-1. L.F. and Z.L. acknowledge support from the Agence Nationale de la Recherche grant SOCRATE ANR-15-CE30-0009-01. Additional thanks go to K. Hengge and T. Gänsler for carrying out the TEM and SAED measurements.

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Author notes

  1. These authors contributed equally: Simon Geiger, Olga Kasian.

Authors and Affiliations

  1. Department of Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Düsseldorf, Germany

    Simon Geiger, Olga Kasian, Marc Ledendecker, Enrico Pizzutilo, Andrea M. Mingers, Karl J. J. Mayrhofer & Serhiy Cherevko

  2. Leiden Institute of Chemistry, Leiden University, Leiden, the Netherlands

    Wen Tian Fu, Oscar Diaz-Morales & Marc T. M. Koper

  3. Laboratoire de Physique des Solides, CNRS, Université Paris-Sud, Orsay, France

    Zhizhong Li & Luc Fruchter

  4. Institute for Materials, Ruhr-Universität Bochum, Bochum, Germany

    Tobias Oellers & Alfred Ludwig

  5. Helmholtz-Institute Erlangen-Nürnberg for Renewable Energy (IEK-11), Forschungszentrum Jülich GmbH, Erlangen, Germany

    Karl J. J. Mayrhofer & Serhiy Cherevko

  6. Department of Chemical and Biological Engineering, Friedrich-Alexander-Universität Erlangen-Nürnberg, Erlangen, Germany

    Karl J. J. Mayrhofer

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Contributions

S.G. composed the manuscript and performed electrochemical dissolution measurements. O.K. carried out OLEMS measurements, IrO2-sputtering and XPS. A.M.M. carried out ICP-MS analysis. W.T.F. and O.D.-M. synthesized double-perovskite powders. Z.L. and L.F. synthesized SrIrO3 films. T.O. and A.L. contributed by allocating sputtered iridium dots. S.G., O.K., M.L., E.P., M.T.M.K., K.J.J.M. and S.C. contributed through scientific discussions and revision of the manuscript.

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Correspondence to Simon Geiger or Serhiy Cherevko.

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Supplementary Notes 1–6; Supplementary Methods; Supplementary Figures 1–14; Supplementary Table 1; Supplementary References

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Geiger, S., Kasian, O., Ledendecker, M. et al. The stability number as a metric for electrocatalyst stability benchmarking. Nat Catal 1, 508–515 (2018). https://doi.org/10.1038/s41929-018-0085-6

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