Dynamic Regulation of Interfacial Micro‐Environment for High Thermodynamics and Kinetics Enabling Stable and Reversible Zn Anode

ABSTRACT Aqueous zinc ion batteries (AZIBs) hold enormous potential as novel energy devices in light of their high safety, reasonable cost, and eco‐economic. While their application on a wide scale is restricted by the notorious dendrite growth and side reactions at the Zn anode/electrolyte interface. Herin, a dynamic regulation of interfacial micro‐environment strategy is proposed, introducing a green and safe hydroxyethyl cellulose (HEC) electrolyte additive to build highly stable and reversible Zn anode. Experiment and calculation results demonstrate that HEC can preferentially adsorb on Zn anode surface and create an HEC‐rich transition layer in inner Helmholtz plane (IHP) during plating/stripping. This layer can shield the parasitic reactions induced by active water and facilitate Zn uniform deposition. Meanwhile, HEC can reconstruct the Zn ²⁺ solvation sheath in outer Helmholtz plane (OHP), which accelerates Zn ²⁺ desolvation kinetics. Consequently, the Zn//Zn cells containing HEC electrolyte additive cycle stably for 2300 h and over 350 h at 1 and 30 mA cm ⁻² , respectively. It also endows Zn anode with excellent reversibility, maintaining high Coulombic efficiency of 99.4% over 600 cycles. After 3000 cycles, the Zn//AC@MnO ₂ full cell with HEC electrolyte additive continues to exhibit outstanding cycling performance, retaining 85.2% of its initial capacity.