Tailoring Interfacial Chemistry Using S═O Bonds and Sulfur Vacancies of MoS₂-PEO for Stable Zinc Anode

Although aqueous zinc-ion batteries (AZIBs) have attracted considerable attention due to their high safety and low cost, their commercial application is hindered by dendrite formation and hydrogen evolution. Herein, a multifunctional artificial interphase protection layer of MoS₂-PEO with sulfur vacancies (SVs) and S═O bonds was constructed on the zinc anode, where SVs accelerate interfacial charge transfer and polyethylene oxide (PEO) chains reduce the desolvation energy barrier of Zn²⁺, while the S═O bonds combine with PEO to reconstruct the interfacial hydrogen-bonding network. Based on these synergistic effects, this can achieve three-dimensional dense nucleation of Zn deposition and effectively suppress the hydrogen evolution side reaction. As a result, the symmetric cell achieves stable cycling over 500 h at 20 mA cm^-2. The full cells maintain 80.76% capacity retention after 2400 cycles at 0.2 A g^-1. Moreover, the pouch cell achieves 99 mAh g^-1 and 98.86% capacity retention after 300 cycles. The work opens a new avenue for the development of dendrite-free anodes in aqueous metal batteries.