(Invited) Multiscale Modeling and Theory Experiment Integration for Understanding Complex Interfaces in Materials for Hydrogen Production and Storage

Abstract

Chemical processes occurring at solid-gas, solid-liquid, and solid-solid interfaces critically determine the performance and durability of hydrogen production and storage technologies. While probing behavior of these interfaces under operating conditions remains challenging, recent progress in predictive multiscale modeling methods together with high-fidelity experimental characterization has led to significant advancements in understanding how microscopic interfacial processes translate to macroscopic device behavior. In this talk, we will provide an overview of our materials modeling efforts within the DOE HydroGEN, HyMARC, and H2NEW hydrogen production and storage consortia, which span ab-initio atomistic modeling to macroscopic device modeling while leveraging state-of-art experimental characterization to ensure fidelity of interpretation. Concrete examples will be provided from our recent activities focused on identifying factors that dictate performance and durability of materials under operating conditions. In particular, we will discuss how computational models have helped to elucidate mechanisms of interface chemistry, formation of new phases, and the impact of interfaces on key reaction pathways that are intimately related to the device performance and durability. We will also illustrate how experimental characterization data has been incorporated to constrain the models and obtain new understanding of interfacial phenomena. Finally, we will discuss how the obtained knowledge may be used to develop strategies for improving materials used in hydrogen production and storage technologies. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.