Interfacial Charge Orchestration for Durable Aqueous Zn Batteries

Abstract Aqueous Zn||MnO 2 batteries offer a compelling solution for large‐scale, low‐cost, and safe energy storage, yet their cycle life remains inadequate for practical applications. This instability stems from intertwined H⁺/OH − interfacial reactions and the intrinsically low conductivity of MnO 2 , leading to poor redox reversibility and electrode passivation. Here, we report a MoS 2 –MnO 2 –electrolyte triple‐interface design that enables interfacial charge orchestration to reshape interfacial chemistry and charge transport dynamics. MoS 2 catalyzes H 2 O dissociation to facilitate efficient H⁺‐redox, while Mo sites stabilize the interfacial pH via OH − adsorption. Concurrently, the MoS 2 –MnO 2 heterojunction accelerates electron transfer through synergistic chemical‐electrochemical pathways. The resulting Zn||MoS 2 –MnO 2 cells deliver extraordinary durability, maintaining 92.7% capacity after 10,000 cycles at 20 C, and pouch‐scale devices with 5.2 mAh cm −2 high areal capacity exhibit stable cycling. This work establishes a cross‐scale strategy in which ordered interfacial charge orchestration couples microenvironment regulation with multi‐step transport control, advancing aqueous Zn batteries toward grid‐level application.