Building Metal‐Molecule Interface towards Stable and Reversible Zn Metal Anodes for Aqueous Rechargeable Zinc Batteries

Abstract Aqueous zinc ion batteries (AZIBs) are receiving increasing attention for large‐scale energy storage systems owing to their appealing features with intrinsic safety, low cost, and scalability. Unfortunately, the water‐induced parasitic reactions and dendrite growth on the Zn anode severely impede the further development of AZIBs. Herein, a thiourea additive is introduced into ZnSO 4 electrolyte to construct unique metal‐molecule interface for simultaneously regulating the Zn anode interface chemistry and the bulk electrolyte environment. Experimental results and theoretical calculations reveal that the formed metal‐molecule interface can not only serve as a corrosion inhibitor for alleviating the water‐induced side reactions, but also act as a Zn 2+ ion regulator for promoting the homogenous Zn deposition, thus achieving a corrosion‐free and dendrite‐free Zn anode. Consequently, the Zn|Zn symmetric cell exhibits an extended lifespan of 1200 h at 1 mA cm –2 , 1mAh cm –2 , and a high cumulative capacity of 3000 mAh cm –2 at 10 mA cm –2 . When paired with V 2 O 5 cathode, the Zn|V 2 O 5 full cell delivers a high capacity retention of 76.0% after 1000 cycles at 1 A g –1 . This study paves a new way to modulate Zn electrode interface chemistry by the novel design of metal‐molecule interface for advanced rechargeable Zn metal batteries and beyond.