Modeling the chemo-mechanical behavior of all-solid-state batteries: a review

Solid-state-batteries (SSBs) present a promising technology for next-generation batteries due to their superior properties including increased energy density, wider electrochemical window and safer electrolyte design. Commercialization of SSBs, however, will depend on the resolution of a number of critical chemical and mechanical stability issues. The resolution of these issues will in turn depend heavily on our ability to accurately model these systems such that appropriate material selection, microstructure design, and operational parameters may be determined. In this article we review the current state-of-the art modeling tools with a focus on chemo-mechanics . Some of the key chemo-mechanical problems in SSBs involve dendrite growth through the solid-state electrolyte (SSE), interphase formation at the anode/SSE interface, and damage/decohesion of the various phases in the solid-state composite cathode. These mechanical processes in turn lead to capacity fade, impedance increase, and short-circuit of the battery, ultimately compromising safety and reliability. The article is divided into the three natural components of an all-solid-state architecture. First, modeling efforts pertaining to Li-metal anodes and dendrite initiation and growth mechanisms are reviewed, making the transition from traditional liquid electrolyte anodes to next generation all-solid-state anodes. Second, chemo-mechanics modeling of the SSE is reviewed with a particular focus on the formation of a thermodynamically unstable interphase layer at the anode/SSE interface. Finally, we conclude with a review of chemo-mechanics modeling efforts for solid-state composite cathodes. For each of these critical areas in a SSB we conclude by highlighting the key open areas for future research as it pertains to modeling the chemo-mechanical behavior of these systems.