Abstract

Aqueous zinc-ion batteries (AZIBs) are poised to play a pivotal part in meeting the growing demands for energy storage and powering portable electronics for their superior security, affordability, and environmentally friendly characteristics. However, the detrimental side reactions occurring at the zinc anode and the dendrite caused by uneven zinc plating/stripping have greatly compromised the cycling life of AZIBs, thereby impeding their practical prospects. In this study, the interfacial comodulation strategy was employed by combining the "electrostatic shielding" effect of cations with the characteristic adsorption of anions. Two molar ZnSO4 served as the matrix, and sodium hydroxyethyl sulfonate (SHES) was selected as a low-cost, nontoxic additive. Experimental results confirm that SHES and zinc anode exhibit robust interactions that lead to the formation of an electrostatic shield and a dynamic adsorption layer at the interface, thereby suppressing hydrogen evolution and corrosion. The combined "electrostatic shielding" effect of sodium ions and the robust characteristic adsorption of hydroxyethyl sulfonate anions serve to guide the directed three-dimensional (3D) diffusion of Zn2+, facilitating rapid, stable, and uniform deposition of zinc. Due to these effects, incorporating 0.2 M SHES as an additive extends the cycle life beyond 3600 h and enables a highly reversible process of deposition and stripping in symmetric cells. Additionally, the Zn-Cu half-cell exhibits reliable cycling for over 1400 cycles, achieving an average Coulombic efficiency of 99.6%. Moreover, the introduction of this additive substantially enhances the performance of Zn-MnO2 and Zn-NH4V4O10 full cells. This study demonstrates the practical feasibility of achieving anodes with high reversibility in AZIBs through the implementation of a strategy that involves anion adsorption at the interface, which holds paramount significance for the practical application of AZIBs.

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