Decarbonization of the grid and transportation sectors requires next-generation energy storage solutions capable of delivering higher capacity, reliability, and safety compared to today’s solutions. Solid-state devices, including solid-state batteries for electrical energy storage and metal hydrides for hydrogen energy storage, are particularly attractive, promising compact, high-density storage with a wide array of materials possibilities. However, key cyclability and performance issues remain, in large part associated with chemical and electrochemical reactions occurring at buried complex interfaces that are difficult to probe. I will provide an overview of how we are using multiscale computational simulations within the LLNL LEAF Center and the U.S. Department of Energy national laboratory consortia to model interfacial processes in solid-state batteries and hydrogen storage materials. Drawing upon recent examples from garnet solid-state batteries and TiFe-based hydrogen storage systems, I will show how atomic-scale simulations are being combined with graph-theoretic approaches, machine learning tools, and mesoscale models to probe transport and mechanics. Specific examples will be given of how simulations have elucidated mechanisms of interfacial chemical reactions, the formation of new phases, and the impact of grain boundaries and heterogeneous interfaces on key degradation modes. I will also show how simulations are being combined with experimental probes to improve models and obtain new understanding of solid materials interfaces under operating conditions.
This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.
Laboratory for Materials Simulations LMS