Self‐Smoothing Deposition Behavior Enabled by Beneficial Potential Compensating for Highly Reversible Zn‐Metal Anodes

Abstract

AbstractRealizing compact dendrite‐free zinc (Zn) plating is crucial to avoiding premature battery failure caused by internal short‐circuits, which is highly determined by the interface electric field (ψi) distribution. Herein, a concept of “potential compensating” is shown on Zn anodes to stimulate its self‐smoothing deposition behavior for durable batteries. A homogeneous ψi with elevated potential intensity is successfully built at the Zn/electrolyte interface via the selective adsorption of highly polarized propylene glycol (PG) molecules, which facilitate the formation of dense and uniform Zn electroplating patterns. Moreover, the PG additive can simultaneously reshape the structure of Zn2+‐solvation sheath and immobilize the H‐bonding networks in bulk electrolyte, enabling Zn anodes with exceptional electrochemical reversibility (99.6%) and ultralong calendar life (3500 h), as revealed by joint spectroscopic and electrochemical analyses. More importantly, full cells with PG safeguard can deliver desirable cycling stability even at an elevated temperature (50 °C) and low N/P ratios (cathode mass loading up to 14.38 mg cm−2). This study presents new insight into the rational design of stable practical electrolytes and interfacial chemistry regulation for sustainable zinc batteries.