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Probing intermediate configurations of oxygen evolution catalysis across the light spectrum

Nature Energy (2024)Cite this article

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Abstract

The oxygen evolution reaction is crucial to sustainable electro- and photo-electrochemical approaches to chemical energy production (for example, H2). Although mechanistic descriptions of the oxygen evolution reaction have been proposed, the frontier challenge is to extract the molecular details of its elementary steps. Here we discuss how advances in spectroscopy and theory are allowing for configurations of reaction intermediates to be elucidated, distinguishing between experimental approaches (static and dynamic) across a range of surface oxygen binding energies on catalysts (from ruthenium to titanium oxides). We outline how interpreting X-ray and optical spectra relies on established and newly implemented computational techniques. A key emphasis is on detecting adsorbed oxygen intermediates at the oxide/water interface by their chemical composition, electronic and vibrational levels and ion–electron kinetic pathways. Integrating the computational advances with the experimental spectra along these lines could ultimately resolve the elementary steps, elucidating how each intermediate leads to another during oxygen evolution reaction.

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Fig. 1: Distinction between pre-equilibrium and non-equilibrium OH* and O*.
Fig. 2: Non-equilibrium detection of hole–polarons.
Fig. 3: Illustrative depiction of the concerted proton–electron trajectory for the polaronic hole-trapping process.
Fig. 4: Non-equilibrium detection of reaction steps in the OER cycle.

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Acknowledgements

This work was supported as part of the Center for Electrochemical Dynamics and Reactions at Surfaces, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Basic Energy Sciences under award DE-SC0023415.

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Authors and Affiliations

  1. Department of Materials Science and Engineering and the Kavli Institute at Cornell for Nanoscale Science, Cornell University, Ithaca, NY, USA

    Jin Suntivich

  2. Thayer School of Engineering, Dartmouth College, Hanover, NH, USA

    Geoffroy Hautier

  3. Department of Materials Science and Engineering, and Wilton E. Scott Institute for Energy Innovation, Carnegie Mellon University, Pittsburgh, PA, USA

    Ismaila Dabo

  4. Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Ethan J. Crumlin

  5. Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Ethan J. Crumlin

  6. Department of Mechanical Engineering, North Carolina Agricultural and Technical State University, Greensboro, NC, USA

    Dhananjay Kumar

  7. Department of Chemistry, the Materials Science and Engineering Program, and the Renewable and Sustainable Energy Institute, University of Colorado Boulder, Boulder, CO, USA

    Tanja Cuk

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Correspondence to Tanja Cuk.

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Suntivich, J., Hautier, G., Dabo, I. et al. Probing intermediate configurations of oxygen evolution catalysis across the light spectrum. Nat Energy (2024). https://doi.org/10.1038/s41560-024-01583-x

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