Energy storage and conversion devices rely on chemical process occurring at solid-gas, solid-liquid, and solid-solid interfaces. Probing behavior of these interfaces under operating conditions presents significant challenges; however, predictive modeling offers an opportunity for providing key insights into interface chemistry, particularly when operating in tandem with high-fidelity experimental characterization techniques.

Within the DOE Hydrogen Materials—Advanced Research Consortium (HyMARC) and the HydroGEN Advanced Water Splitting Materials Consortium, we are using multiscale models to understand properties of reactive interfaces for the production and storage of hydrogen. I will provide an overview of our materials modeling strategy within these consortia, ranging from first-principles calculations of interface chemistry to continuum methods for microstructure-level properties. I will then review some of our recent activities for simulating thermodynamic and kinetic properties of hydrogen-related materials. Specific examples will be given of how these computational models have helped to elucidate mechanisms of interface chemical reactions, the formation of new phases, and the impact of solid-state interfaces on key reaction pathways. I will also show how simulations have been combined with experimental probes to improve models and obtain new understanding of materials interfaces under operating conditions. Finally, I will discuss how this understanding is being used to guide new strategies for improving materials functionality for hydrogen storage and production.

This work performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.