Robust zincophilic-hydrophobic protection layer induces preferential growth of (0 0 2) crystal plane towards ultra-stable Zn anode

The practical deployment of aqueous zinc-ion batteries (AZIBs) in large-scale energy storage applications is hampered by short cycle lifespans and limited zinc utilization due to uncontrollable dendrite growth and water-induced side reactions. Herein, we propose an environmentally friendly electrolyte additive, 2-acrylamido-2-methylpropanesulfonic acid (AMPS), which features dual zincophilic sites and a hydrophobic group, to enhance Zn stability. Theoretical calculations and experimental characterizations demonstrate that AMPS can firmly adsorb onto the Zn (0 0 2) plane through its dual zincophilic sites ([sbnd]SO₃H and [sbnd]NH[sbnd]CO), while the C[dbnd]C hydrophobic group orients toward the electrolyte, ultimately forming a stable zincophilic/hydrophobic interface on the Zn electrode in situ. This unique structure not only inhibits water-induced side hydrogen evolution reactions but also induces preferential deposit propagation along the (0 0 2) crystal plane. Benefiting from this synergetic effect, the Zn//Cu asymmetric cell with AMPS electrolyte maintains an ultrahigh average coulombic efficiency of 99.8 % for over 2500 cycles at 2 mA cm⁻², achieving 1 mAh cm⁻². Furthermore, the Zn//MnO₂ full cell shows a high-capacity retention of 67.7 % at 1.8 A g⁻¹ after 1000 cycles, confirming the effectiveness of the AMPS additive in improving the cyclability and performance of AZIBs.