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Integration of theory and experiment in the modelling of heterogeneous electrocatalysis.

Journal Article · · Nature Energy
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Theoretical modelling is essential to deepen our understanding of heterogeneous electrocatalytic energy conversion processes, such as water splitting. Here, Sharon Hammes-Schiffer and Giulia Galli offer their perspectives on the best strategies for successfully studying such systems. 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.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
Air Force Research Laboratory (AFRL) - Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF)
DOE Contract Number:
AC02-06CH11357
OSTI ID:
1868962
Journal Information:
Nature Energy, Vol. 6, Issue 7
Country of Publication:
United States
Language:
English

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