Interfacial Chemistry Regulation via Multifunctional Additive for Aqueous Zinc Metal Batteries

Abstract Aqueous zinc metal batteries (AZMBs) are constrained by water-induced side reactions and non-uniform Zn deposition. Herein, we introduce 3,4-dihydroxycyclobut-3-ene-1,2-dione (SA) as an electrolyte additive to regulate molecular interface chemistry. The introduction of SA disrupts the intrinsic hydrogen-bond network in the electrolyte, suppressing the activity of free water. Density functional theory calculations further demonstrate that SA preferentially binds to the Zn (100) and (101) surfaces over the (002) plane, which effectively limits the growth of high-energy facets and promotes oriented nucleation along the (002) texture, yielding a dense and uniform zinc deposit. Benefiting from these synergistic effects, the Zn//Zn symmetric cell achieves a stable cycling lifespan exceeding 2500 h, while the Zn//Cu asymmetric cell maintains a high Coulombic efficiency of 99.4% over 1000 cycles. This work offers an effective pathway for enhancing the performance of AZMBs.