The irreversible chemistry of the Zn anode, attributed to dendrite growth and parasitic side reactions, is a major constraint on the practical application of aqueous zinc-ion batteries. Herein, polyelectrolyte complexes (CPs) containing rich quaternary ammonium and carboxylate groups were developed as artificial protective layers to systematically and efficiently regulate Zn plating/stripping. By virtue of their unique amphoteric characteristic, a self-adaptive built-in electric field could be generated at the interface. Comprehensive experimental and computational analyses demonstrated that the as-generated built-in internal electric field caused prominent divergence of surface properties. The enriched Zn²⁺ flux and homogenized charge distribution could dynamically eliminate local charge accumulation at the interface and offer highly oriented, dendrite-free Zn deposition. Owing to the intrinsic self-healing feature of the CPs, the as-proposed electric field modulation strategy presents long-term effectiveness. Correspondingly, the cycling durability of the Zn anode was prolonged from 91 to 6330 h at 0.5 mA cm⁻² (∼70-fold enhancement). A promoted electrochemical performance of full cells was also demonstrated by coupling the CP-protected Zn anode with I₂ or NH₄V₄O₁₀ cathodes. In particular, a remarkable capacity maintenance was observed with Zn‖I₂ cells, with an ultraslow decay rate of 0.005‰ per cycle after 30000 cycles (over 290 days).

中文翻译：

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通过构建内置内部电场动态消除局部电荷积累，实现可逆锌化学


由于枝晶生长和寄生副反应，锌阳极的不可逆化学性质是水系锌离子电池实际应用的主要限制。在此，开发了含有丰富季铵和羧酸盐基团的聚电解质复合物（CP）作为人工保护层，以系统有效地调节镀锌/剥离。凭借其独特的两性特性，可以在界面处产生自适应的内置电场。综合实验和计算分析表明，所产生的内置内部电场导致表面特性的显着差异。富集的 Zn ²⁺ 通量和均匀的电荷分布可以动态消除界面处的局部电荷积累，并提供高度定向、无枝晶的 Zn 沉积。由于CP固有的自愈特性，所提出的电场调制策略具有长期有效性。相应地，Zn 阳极的循环耐久性在 0.5 mA cm ⁻² 下从 91 小时延长至 6330 小时（提高了约 70 倍）。通过将 CP 保护的 Zn 阳极与 I ₂ 或 NH ₄ V ₄ O ₁₀ 电池中观察到显着的容量维持，在 30000 次循环（超过 290 天）后，每个循环的超慢衰减率为 0.005‰。