Bridging Atomistic, Mesoscale, and Systems Perspectives in the Design of Vanadium-Based Energy Storage Technologies

Abstract

Several origins of battery performance degradation are traceable to multi-field and multi-physics coupling originating at atomistic scales, manifested at mesoscale dimensions, and compounded up to the level of electrode architectures. A detailed understanding of electrochemistry—mechanics coupling and resulting emergent phenomena across many decades of length scales is imperative to unlock unexploited performance from existing battery chemistries, develop dynamic process controls, and design next-generation materials and architectures purpose-built to alleviate common modes of degradation and enable the energy transition. The close coupling between mechanics and electrochemistry plays an especially prominent role in phase-transforming electrode materials. In these systems, intercalation gives rise to multi-phase coexistence regimes, which result in significant coherency strains at the interfaces between differently lithiated phases. In this first portion of this dissertation, synchrotron-based hyperspectral X-ray spectromicroscopy experiments, coupled with spectral standards, provide a direct examination of phase evolution upon Li-ion intercalation into V2O5. Here the role of nucleation limitations, strain, curvature, and defects on the spatial evolution of composition and stress gradients is demonstrated. Integration of statistical regression and machine learning approaches showcase recent developments toward achieving real-time process control of intercalation phenomena.

In the final portion of this work, atomistic and mesoscale perspectives will be woven together with considerations of materials criticality, policy, and life cycle assessment to provide a macroscopic view of the energy storage requirements for grid- level storage applications. Industry data on vanadium consumption in different sectors, compilations of public data on largescale grid-level storage, and life cycle inventories are utilized to develop a detailed assessment of the potential impact of vanadium redox flow batteries to reduce carbon emissions.