A Multifunctional Zwitterion Electrolyte Additive for Highly Reversible Zinc Metal Anode

Although zinc metal anode is promising for zinc-ion batteries (ZIBs) owing to high energy density, its reversibility is significantly obstructed by uncontrolled dendrite growth and parasitic reactions. Optimizing electrolytes is a facile yet effective method to simultaneously address these issues. Herein, 2-(N-morpholino)ethanesulfonic acid (MES), a pH buffer as novel additive, is initially introduced into conventional ZnSO₄ electrolyte to ensure a dendrite-free zinc anode surface, enabling a stable Zn/electrolyte interface, which is achieved by controlling the solvated sheath through H₂O poor electric double layer (EDL) derived from zwitterionic groups. Moreover, this zwitterionic additive can balance localized H⁺ concentration of the electrolyte system, thus preventing parasitic reactions in damaging electrodes. DFT calculation proves that the MES additive has a strong affinity with Zn²⁺ and induces uniform deposition along (002) orientation. As a result, the Zn anode in MES-based electrolyte exhibits exceptional plating/stripping lifespan with 1600 h at 0.5 mA cm⁻² (0.5 mAh cm⁻²) and 430 h at 5.0 mA cm⁻² (5.0 mAh cm⁻²) while it maintains high coulombic efficiency of 99.8%. This work proposes an effective and facile approach for designing dendrite-free anode for future aqueous Zn-based storage devices.