Quantitative experimental and computational analysis of dendritic metal electrodeposition

Instability at the electrode–electrolyte interface during metal electrodeposition promotes non-uniform growth and the formation of dendritic structures, which adversely affect electrochemical performance in various systems, particularly batteries. Because electrodeposition occurs at embedded electrode-electrolyte interfaces, which are moving and deforming boundaries, direct experimental investigation and quantitative comparison with computational models is challenging. In this work, a computational model of the electrodeposition interface is validated using a planar experimental system that enables direct imaging of silver electrodeposition and approximates the geometry of a two-dimensional simulation. While dendritic growth is often investigated qualitatively, little work has been done to quantitatively measure dendritic growth, particularly at nanometer scales. In this study, quantitative parameters for dendritic growth, including electrodeposition density, dendrite branch thickness, and dendrite aspect ratio, are defined and used to validate computational results for silver electrodeposition with results from experimental electrodeposition. The sensitivity of the computational system is evaluated by studying the effects of variations in operating and material parameters on dendritic growth, using the established quantitative parameters. Finally, the computational model is used to explore stable electrodeposition regimes that are challenging to attain experimentally.