A Predictive Theory of Electrochemical Ostwald Ripening for Electrodeposited Lithium Metal

TL;DR

This paper introduces a theoretical model of electrochemical Ostwald ripening that predicts lithium electrode morphology based on measurable parameters, linking deposition conditions to efficiency and stability.

Contribution

It presents the first predictive framework for lithium electrode morphology, incorporating key parameters like SEI resistance and electrolyte conductivity.

Findings

Model accurately reproduces experimental results

Identifies transition from 2D to 3D growth regimes

Provides analytical expressions for nucleus size and distribution

Abstract

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 non-dendritic regime. The framework explicitly incorporates SEI resistance, electrolyte conductivity, electrode wettability, and current density revealing the transition from 2D SEI-limited to 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 predictive understanding of lithium plating and provides a broadly applicable basis for controlling electrodeposition morphology across diverse electrochemical systems.