Aqueous zinc-ion batteries (AZIBs) are charming devices for large-scale power grid energy storage because of their characteristics of environment friendliness, low cost, high abundance, and safe operation. However, the inferior reversibility of the anode and the loss of cathode capacity always hinder the application of AZIBs. Herein, we propose a simple multifunctional electrolyte additive, diethylenetriamine (DETA), which can inhibit the formation of zinc dendrites and the occurrence of side reactions on the anode, reconstruct the solvated structure and uniform ion flux in the electrolyte, restrain the dissolution of active materials, and induce the crystal transformation on the cathode concurrently. Molecular dynamics Simulation and density functional theory both verified the extraordinary efficacy of DETA. With the assistance of DETA, the Zn anode gained a life of up to 2000 h, and the cathode with commercial V2O5 retained a capacity of 125.2 mA h g–1 at the 1000th discharge process. From the perspective of practical application, this work can open up the application prospect of AZIBs in large-scale energy storage and provide reference for the subsequent works. The findings will greatly promote the application of AZIBs in large-scale energy storage and provide more inspiration for future research.

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