Predictive Theory of Electrochemical Ostwald Ripening for Electrodeposited Lithium Metal

Electrode morphology critically determines the stability and efficiency of lithium metal anodes, yet no predictive framework has explained how measurable parameters control deposition. Here we introduce the first theoretical model of electrochemical Ostwald ripening, capturing the competition between electroplating and surface-energy-driven redistribution and identifying it as the governing process behind morphology evolution in the nondendritic regime. The framework explicitly incorporates solid electrolyte interphase (SEI) resistance, electrolyte conductivity, electrode wettability, and current density, revealing the transition from a 2D SEI-limited to a 3D electrolyte-limited growth. The model yields analytical expressions for nucleus size, density, and distribution that quantitatively reproduce independent experimental results and establishes a direct link between plating conditions, morphology, and Coulombic efficiency. By providing experimentally accessible relationships between key parameters and deposition outcomes, the framework enables a predictive understanding of lithium plating and provides a broadly applicable basis for controlling electrodeposition morphology across diverse electrochemical systems.