Processes occurring at solid-gas, solid-liquid, and solid-solid interfaces are critical to the functionality of most energy storage and conversion devices. In many instances, these interfaces tend to be highly heterogeneous, which introduces additional complexities that must be addressed by diagnostic methods. Although predictive modeling based on ab initio simulations offers a unique set of tools for unbiased understanding of interfaces, accessing their full chemical and structural complexity under realistic operating conditions remains a significant challenge. In this talk, I will outline some key difficulties associated with predictive modeling of complex interfaces and review our recent efforts coupling ab initio molecular dynamics with advanced X-ray spectroscopy and other high-fidelity experimental probes to understand interfacial chemistry and transport. Drawing upon examples from our recent work on solid-state batteries, hydrogen storage, and hydrogen production, I will show how theoretical modeling and experimental characterization can operate hand-in-hand, with experiments aiding the validation and assembly of accurate interface models, and theory aiding the interpretation of complex spectra. The examples will specifically highlight the importance of accounting for structural and chemical changes induced by the presence of the interface under electrochemical conditions, such as surface oxidation and reconstruction, which profoundly alter materials behavior with consequences for durability and efficiency. Specific topics to be discussed will include grain boundary effects in solid-state electrolytes, as well as electrochemical oxidation processes at interfaces in materials for hydrogen storage and production.

Predicting properties of complex interfaces for energy storage by integrating ab initio simulations with high-fidelity experiments

256th National Meeting (2018)

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