Aqueous zinc-ion batteries (ZIBs) have received extensive attention due to the intrinsic advantages of high safety, low cost and environmental friendliness. But detrimental side reactions and dendrite problems resulting from high desolvation penalty and inhomogeneous Zn²⁺ flux at the interface severely hindered their practical applications. Herein, a novel polyacrylamide-poly (ethylene glycol) diacrylate-carboxymethyl cellulose (PMC) hydrogel electrolyte is designed to overcome these obstacles through reducing the desolvation energy barrier and guiding the preferential orientation of Zn deposition simultaneously. Theoretical calculation and experimental results reveal that the desolvation activation energy of the PMC hydrogel electrolyte (36.42 kJ mol⁻¹) is substantially lower than that of conventional ZnSO₄ aqueous electrolyte (62.31 kJ mol⁻¹) due to the regulated Zn²⁺ solvation structure. Based on the high binding energy between amide groups and Zn²⁺, polymer chains in PMC also serve as facile Zn²⁺ transport channels to guide the uniform deposition behavior on the Zn (002) crystal surface, which is verified by the grazing incidence XRD analysis. Consequently, an ultra-long cycle life of 5000 h with a high coulombic efficiency of 99.5% is achieved by using the PMC hydrogel electrolyte. Considering the simple one-pot synthesizing method, the PMC hydrogel electrolyte provides new opportunities for developing practical ZIBs.

水系锌离子电池（ZIBs）由于具有高安全性、低成本和环境友好的内在优势而受到广泛关注。但是由于界面处的高去溶剂化损失和不均匀的Zn ²⁺通量导致的有害副反应和枝晶问题严重阻碍了它们的实际应用。在此，设计了一种新型聚丙烯酰胺-聚（乙二醇）二丙烯酸酯-羧甲基纤维素（PMC）水凝胶电解质，通过降低去溶剂化能垒并同时引导Zn沉积的优先取向来克服这些障碍。理论计算和实验结果表明，PMC水凝胶电解质的去溶剂化活化能（36.42 kJ mol ^-1) 明显低于常规 ZnSO ₄水性电解质 (62.31 kJ mol ^-1 )，这是由于受调节的 Zn ²⁺溶剂化结构所致。基于酰胺基团与 Zn ²⁺之间的高结合能，PMC 中的聚合物链也可作为 Zn ²⁺传输通道，引导 Zn (002) 晶体表面的均匀沉积行为，这一点已通过掠入射 XRD 验证分析。因此，通过使用 PMC 水凝胶电解质，可实现 5000 小时的超长循环寿命和 99.5% 的高库仑效率。考虑到简单的一锅法合成方法，PMC水凝胶电解质为开发实用的ZIBs提供了新的机会。