Montmorillonite Interfacial Chemistry Regulation on Homogeneous Zn Deposition: A Microenvironment‐Controlled Additive Strategy for Sustainable Zinc Metal Anodes

Aqueous zinc (Zn) metal batteries (AZBs) have emerged as highly promising candidates for large-scale energy storage systems because of their inherent safety and cost-effectiveness. However, their practical implementation remains constrained by parasitic side reactions and uncontrolled dendrite growth at the metallic Zn anode. Herein, a microenvironment-controlled additive strategy is proposed via employing phytic acid-functionalized montmorillonite (MPA) nanosheets as electrolyte additives for highly durable AZBs. The MPA nanosheets spontaneously assemble onto the surface of the Zn anode through interfacial self-adsorption, effectively suppressing parasitic reactions. Moreover, the regulation of interfacial chemistry enhances the zincophilic characteristic, enabling precise modulation of Zn²⁺ flux distribution and directing homogeneous Zn electrodeposition through spatially controlled ion coordination. As a result, the Zn||Zn symmetric cell with the MPA additives achieves a stable cycle for over 2800 h at 2 mA cm^-2. The assembled Zn||VO₂ full cell within the modified electrolyte maintains exceptional cycling stability of 89.5% after 1000 cycles. This work presents a facile and efficient microenvironment-regulated additive strategy for homogeneous Zn deposition, aimed at achieving highly reversible AZBs.