A Predictive Theory of Electrochemical Ostwald Ripening for Electrodeposited Lithium Metal

Abstract: In this work, we present a theoretical framework that describes the evolution of lithium nuclei under the competing effects of electroplating and surface energy-driven redistribution (electrochemical Ostwald ripening). Our model introduces a formulation that accounts for solid electrolyte interphase (SEI) resistance, electrolyte conductivity, and electrode wettability, capturing the transition from SEI to electrolyte-limited growth regimes. We identify asymptotic behaviors for high and low current densities, quantify the conditions under which ripening dominates, and derive analytical expressions for nucleus size, density, and surface coverage. Model predictions show excellent agreement with experimental data across multiple datasets. The results reveal how SEI and electrolyte conductivity, current density and metal-electrode contact angle govern deposition morphology and Coulombic efficiency. Based on these insights, we outline experimentally accessible guidelines to improve battery efficiency and cycling stability - offering a simple yet predictive approach for optimizing metal electrodeposition processes in battery systems and beyond.