Co‐Regulating Solvation Structure and Hydrogen Bond Network via Bio‐Inspired Additive for Highly Reversible Zinc Anode

Abstract

The feasibility of aqueous zinc-ion batteries for large-scale energy storage is hindered by the inherent challenges of Zn anode. Drawing inspiration from cellular mechanisms governing metal ion and nutrient transport, erythritol is introduced, a zincophilic additive, into the ZnSO₄ electrolyte. This innovation stabilizes the Zn anode via chelation interactions between polysaccharides and Zn²⁺. Experimental tests in conjunction with theoretical calculation results verified that the erythritol additive can simultaneously regulate the solvation structure of hydrated Zn²⁺ and reconstruct the hydrogen bond network within the solution environment. Additionally, erythritol molecules preferentially adsorb onto the Zn anode, forming a dynamic protective layer. These modifications significantly mitigate undesirable side reactions, thus enhancing the Zn²⁺ transport and deposition behavior. Consequently, there is a notable increase in cumulative capacity, reaching 6000 mA h cm⁻² at a current density of 5 mA cm^-2. Specifically, a high average coulombic efficiency of 99.72% and long cycling stability of >500 cycles are obtained at 2 mA cm^-2 and 1 mA h cm^-2. Furthermore, full batteries comprised of MnO₂ cathode and Zn anode in an erythritol-containing electrolyte deliver superior capacity retention. This work provides a strategy to promote the performance of Zn anodes toward practical applications.