Abstract

It is experimentally demonstrated recently that the complicated temperature dependence of lithium electrodeposition, which remains unclear and requires further exploration, may provide a regulatory strategy for suppressing dendrites. In order to explore the underlying physics of temperature-dependent performance of lithium metal batteries, we utilize a comprehensive model including the electrochemical process of lithium electrodeposition, the non-uniform solid electrolyte interface (SEI) evolution on the moving dendrite surface and their interaction with incorporating the thermal effects, where the temperature dependencies of the SEI formation, lithium electrodeposition and bulk diffusion kinetic are assumed to follow Arrhenius-type dependencies independently. On the basis of present work, we are able to evaluate the competition mechanisms of the interfacial reactions between SEI formation and lithium dendrite growth with a series of governing mechanisms including different ambient temperature, applied current density and surface geometric curvature. The results show that the inhomogeneity of SEI layer controlled by multiple factors finally determine whether or not the lithium dendrite can be suppressed at elevated temperature, which provide a new perspective into the underlying thermo-electro-chemical performance and may be instructive for the interfacial design of rechargeable batteries.

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