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To address the persistent challenges of dendrite growth, hydrogen evolution, and corrosion in aqueous Zn-ion batteries, this study demonstrates the construction of a zincophilic-hydrophobic TiO2 interfacial layer on the Zn anode. This was achieved by grafting hydrophobic methacryloxypropyl groups (CH2 = C(CH3)COO(CH2)3—) onto nano-TiO2 via the silane coupling agent (KH570). The grafted hydrocarbon chains act as a hydrophobic barrier, impeding H2O diffusion and promoting the desolvation of hydrated Zn2+ to suppress side reactions. Simultaneously, the abundant Ti—OH groups on TiO2 serve as zincophilic sites, increasing local Zn2+ concentration and facilitating uniform deposition. The modified Zn anode exhibited a transition from hydrophilic (79°) to hydrophobic (105°) wetting behavior and a significantly reduced charge-transfer resistance. Consequently, it delivered exceptional cycling stability exceeding 800 hours at 1 mA·cm-2 and 1 mAh·cm-2. This work provides a novel interfacial design strategy for high-performance zinc anodes.
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