Underpotential lithium plating on graphite anodes caused by temperature heterogeneity

Significance Metallic lithium plating on the graphite anode is a predominant cause for capacity decays during the fast charging of lithium-ion batteries. This work studies the lithium-plating phenomenon in a previously neglected thermodynamic perspective, taking into account practical temperature distributions within batteries. We show that elevated temperatures could enhance the equilibrium potential of Li 0 /Li + , making local lithium plating more thermodynamically favorable. Furthermore, lithium-plating patterns are correlated with temperature heterogeneities, confirming the preferential lithium plating at high-temperature regions due to both kinetic and thermodynamic origins. These findings provide possible explanations of the heterogeneous lithium-plating morphology, deepen the understandings on the lithium plating phenomenon, and will guide future strategies to realize the extreme fast charging of lithium-ion batteries.