Manipulating Interfacial Dissolution–Redeposition Dynamics to Resynthesize Electrode Surface Chemistry

The solid–liquid electrochemical interface offers a reactive environment for interfacial reactions to tailor electrode surface chemistry under operating conditions. Herein, we demonstrate that the dissolution and redeposition kinetics of transition metal cations, a ubiquitous phenomenon at the electrochemical interface, can be manipulated to regulate the chemical composition and crystal structure of the electrode surface, as well as the overall electrochemical performance. Foreign cations (e.g., Ti4+), either added as electrolyte additives or dissolved from surface coatings, can rapidly participate in the electrode dissolution–redeposition process and facilitate the establishment of the dissolution–redeposition equilibrium. Our work expands the control over the electrochemical reactions at the solid–liquid interface and provides new insights into interfacial studies in electrochemistry and surface science.