Interface-engineered electrolyte-electrode design with lithium nitrate for durable aqueous zinc-ion batteries in sustainable energy applications

초록

Aqueous zinc-ion batteries (AZIBs) are promising candidates for next-generation large-scale renewable energy storage systems owing to their intrinsic safety, cost-effectiveness, and environmental compatibility. However, their practical deployment is limited by dendritic zinc growth, hydrogen evolution, and unstable electrolyte-electrode interfaces, which reduce cycle life and operational reliability. In this work, we present an interface-engineered electrolyte-electrode composite approach utilizing lithium nitrate (LiNO3) as a multifunctional additive to regulate Zn2+ solvation and promote controlled deposition. Through competitive ligand coordination, NO3-anions partially replace H2O and SO42-ligands in the Zn2+ solvation shell, enabling enhanced ionic mobility, uniform metal deposition, and suppressed ZnSO4 aggregate formation. Optimized LiNO3 concentration (0.075 wt.%) yields Zn||Ti half-cells with over 500 stable cycles and an average Coulombic efficiency of 99.7%, while Zn||Zn symmetric cells exhibit dendrite-free operation exceeding 1300 h even under high current densities. Complementary molecular dynamics simulations and experimental characterization reveal preferential deposition along the Zn (002) crystal plane and the formation of a robust, Li3N-containing solid electrolyte interphase, improving interfacial conductivity and corrosion resistance. Full-cell tests with MnO2 cathodes demonstrate an initial specific capacity of 263 mAh & centerdot;g-1, retaining 65% after 300 cycles at 1 A & centerdot;g-1, with Coulombic efficiency consistently above 99.7%. This composite interface design strategy provides a scalable pathway for engineering durable zinc-based batteries, directly supporting the development of high-performance, long-life energy storage modules for grid-level renewable integration and other engineering applications.

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