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Integration of theory and experiment in the modelling of heterogeneous electrocatalysis

Nature Energy volume 6, pages 700–705 (2021)Cite this article

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Abstract

Heterogeneous electrocatalysis is critical to many energy conversion processes. Theoretical and computational approaches are essential to interpret experimental data and provide the mechanistic understanding necessary to design more effective catalysts. However, automated general procedures to build predictive theoretical and computational frameworks are not readily available; specific choices must be made in terms of the atomistic structural model and the level of theory, as well as the experimental data used to inform and validate these choices. Here we outline some best practices for modelling heterogeneous systems and present examples in the context of catalysis at metal electrodes and oxides. The level of theory should be chosen for the specific system and properties of interest, and experimental validation is essential from the beginning to the end of the study. Continuous feedback and ultimate integration between experiment and theory enhances the power of calculations to elucidate mechanisms, identify effective descriptors and clarify design principles.

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Fig. 1: The interplay between theory, simulation, experiment and data.
Fig. 2: Electrochemical PCET and interfacial electrostatic potentials.
Fig. 3: Atomistic structural models of a photo-absorber and catalyst for OER.

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Acknowledgements

This material is based on work supported by the National Science Foundation grant no. CHE-1764399 (G.G.) and the Air Force Office of Scientific Research under awards FA9550-18-1-0420 and FA9550-18-1-0134 (S.H.-S.).

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Authors and Affiliations

  1. Department of Chemistry, Yale University, New Haven, CT, USA

    Sharon Hammes-Schiffer

  2. Pritzker School of Molecular Engineering and Department of Chemistry, University of Chicago, Chicago, IL, USA

    Giulia Galli

  3. Materials Science Division, Argonne National Laboratory, Lemont, IL, USA

    Giulia Galli

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  1. Sharon Hammes-Schiffer
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  2. Giulia Galli
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Correspondence to Sharon Hammes-Schiffer or Giulia Galli.

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Peer review information Nature Energy thanks Michal Bajdich, Annabella Selloni and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Hammes-Schiffer, S., Galli, G. Integration of theory and experiment in the modelling of heterogeneous electrocatalysis. Nat Energy 6, 700–705 (2021). https://doi.org/10.1038/s41560-021-00827-4

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