Redirected Zn Electrodeposition by an Anti‐Corrosion Elastic Constraint for Highly Reversible Zn Anodes

Abstract With advantages such as high theoretical capacity, low cost, and nontoxicity, Zn metal has been widely investigated as an anode for aqueous batteries. However, the problems of dendrite formation and sustained corrosion originating from severe interfacial side reactions and uncontrolled Zn electrodeposition in aqueous electrolytes significantly slows down the practical application of Zn metal anodes. To address these issues, herein, an anti‐corrosion elastic constraint (AEC) is introduced that is built with nanosized TiO 2 and polyvinylidene fluoride (PVDF) matrix to Zn anode, where the PVDF layer serves as an elastic H 2 O/O 2 ‐blocking layer and the decorated TiO 2 nanoparticles assist uniform Zn electrodeposition. With this corrosion‐inhibition and electrodeposition‐redirection coating, the electrodeposition consistency and thermodynamic stability of the Zn anode are significantly improved, enabling a long‐term stable plating/stripping performance for 2000 h with an ultralow overpotential (<50 mV) and a high average Coulombic efficiency (>99.4%) for 1000 cycles without obvious dendrite formation. Even at a high current density of 8.85 mA cm −2 with limited Zn supply (DOD Zn = 60%), stable Zn deposition is achieved over 250 h. When coupled with a MnO 2 cathode, the AEC‐Zn anode shows a remarkably enhanced full‐cell cycling stability, indicative of high reliability of aqueous Zn batteries for practical application.