Interfacial Charge Orchestration for Durable Aqueous Zn Batteries

Aqueous Zn||MnO₂ 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 MnO₂, leading to poor redox reversibility and electrode passivation. Here, we report a MoS₂-MnO₂-electrolyte triple-interface design that enables interfacial charge orchestration to reshape interfacial chemistry and charge transport dynamics. MoS₂ catalyzes H₂O dissociation to facilitate efficient H⁺-redox, while Mo sites stabilize the interfacial pH via OH^- adsorption. Concurrently, the MoS₂-MnO₂ heterojunction accelerates electron transfer through synergistic chemical-electrochemical pathways. The resulting Zn||MoS₂-MnO₂ 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.