Cationic Surfactant-Type Electrolyte Additive Enables Three-Dimensional Dendrite-Free Zinc Anode for Stable Zinc-Ion Batteries

Zn metal has been considered as a promising anode material for rechargeable aqueous metal-ion batteries. However, the propensity of dendrite growth during plating restricts its practical applications. Herein we propose an effective, low-cost, and nontoxic electrolyte additive, tetrabutylammonium sulfate (TBA2SO4), as the first example of a cationic surfactant-type electrolyte additive in Zn-ion batteries, which can induce the uniform Zn deposition in both electrode preparation and the battery charge/discharge process. Electrochemical characterizations, in situ optical microscopy observation, along with density functional theory (DFT) calculations reveal the unique zincophobic repulsion mechanism, which results in the minimum addition amount of 0.029 g L–1 compared with other reported additives (at least 1g L–1), demonstrating the great potential for practical application. Excellent cycling performance with dendrite-free morphology at different current densities and discharge depths is achieved for both the symmetric cell and the full cell (coupled to α-MnO2) using the as-prepared 3D Zn anode and the proposed additives.