Emergent Mind

Abstract

We present a coupled mechanistic approach that elucidates the intricate interplay between stress and electrochemistry, enabling the prediction of the onset of instabilities in Li-metal anodes and the solid electrolyte interphase (SEI) in liquid-electrolyte Li-metal batteries. Our continuum theory considers a two-way coupling between stress and electrochemistry, includes Li and electron transport through SEI, incorporates effects of Li viscoplasticity, includes SEI and electrolyte interface surface energy and evaluates crucial roles of these mechanistic effects on the continuously evolving anode surface due to the viscoplastic deformation of lithium. In the model, spatial current density evolves with the stress-induced potential across the deformed anode/SEI interface. We assume SEI as a homogeneous, artificial layer on the Li-anode, which allows the investigation of the mechanical and electrochemical properties of the SEI systematically. Subsequently, we solve a set of coupled electrochemistry and displacement equations within the SEI and anode domains. The model is implemented numerically by writing a user element subroutine in Abaqus/Standard. We conduct numerical simulations under various galvanostatic conditions and SEI properties and predict conditions for anode instability. We find that Li viscoplasticity is one of the key attributes that drives instability in the Li-anode and show that applying a soft artificial SEI layer on the Li-anode to minimize viscoplastic deformation can be an effective method. We also report the role of artificial SEI elasticity and thickness on anode stability. Selected stability maps are provided as a design aid for artificial SEI.

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