Tailoring Interfacial Chemistry Using S═O Bonds and Sulfur Vacancies of MoS ₂ ‐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 MoS 2 ‐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 Zn 2+ , 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.