Steering Interfacial Renovation with Highly Electronegative Cl Modulated Trinity Effect for Exceptional Durable Zinc Anode

The poor anode/electrolyte interface triggered by abysmal dendritic growth and hydrogen evolution reactions (HER) hinders the development of aqueous zinc‐ion batteries (AZIBs). Here, a highly efficient electrolyte is formulated with sucralose (Sucral) additive to refresh solvated structure and steer interfacial renovation, for building highly electronegative Cl‐modulated trinity effect in the bulk‐interface between electrolyte and electrode. Experiment results and theoretical studies jointly reveal that Sucral with highly zincophilic and hydrophilic hydroxyl groups can remodel primary Zn2+ solvation shell and interrupt strong H‐bond network from H2O molecules, thus boosting fast de‐solvation and restricting undesirable HER. Simultaneously, three highly electronegative chlorides in the adsorbed Sucral possessing hydrophobic features can enable a H2O‐poor electric double‐layer (EDL), thus remodeling the Zn surface against corrosion. Additionally, it realizes preferential exposure of the Zn (002) plane for helping uniform interfacial deposition. The synergy of the above factors achieves a prolonged lifespan of 3000 h (1.0 mA cm−2, 1.0 mAh cm−2), much better than that with Sucrose (Suc) electrolyte. The Zn//V2O5 full cell at 5 A g−1 also maintains enhanced stability of 1500 cycles with 160 mAh g−1. In this paper, a unique electrolyte is designed with sucralose (Sucral) to realize a highly electronegative Cl modulated trinity effect for durable Zn anode. Such a built system refreshes solvated structure and steers interfacial renovation to obtain a waterless EDL environment and achieve preferential exposure of the Zn (002). This synergistic effect enhances the stability lifespan of the whole batteries.