Dendrites proliferation and parasitic side reactions on zinc metal anodes (ZMAs) severely weaken the energy efficiencies of aqueous zinc metal batteries (AZMBs). Herein, an effective Helmholtz plane (HP) reconstruction mechanism on ZMAs in ZnSO₄ electrolyte activated by zinc pyrrolidone carboxylate (PCA-Zn) additive is proposed. Systematical experiments together with numerical simulations identified that the dissociated PCA⁻ anions featuring bis-zincophilic-terminal preferentially adhere to the ZMAs surface with carboxyls serving as anchors to replace H₂O and SO₄²⁻, reshaping an H₂O/SO₄²⁻-repellent HP to restrain water-triggered side reactions. Meanwhile, the other free zincophilic carbonyl terminals of PCA⁻ anions endow the restructured HP with spatial confinement effect on Zn²⁺, effectively suppressing their rampant in-plane diffusion and homogenizing ions flux during Zn deposition. Moreover, the HP exhibits a self-repair behavior against unexpected electrode surface damage upon cycling. Benefiting from the multifunctional HP that enables more stable ZMAs/electrolyte interphasial chemistry, an excellent Zn||Zn symmetric electroplating/stripping cyclic durability exceeding 300 h under a depth of discharge up to 40% (20 mA cm⁻²/20 mAh cm⁻²) is achieved, accounting for significantly boosted rechargeability (89.7% capacity holding ratio after 5000 cycles) of the carbon-cloth@polyaniline||ZMA full AZMBs compared to that without PCA-Zn additive (malfunction after only 960 cycles).

锌金属阳极 (ZMA) 上的枝晶增殖和寄生副反应严重削弱了水系锌金属电池 (AZMB) 的能量效率。在此，提出了在由吡咯烷酮羧酸锌 (PCA-Zn) 添加剂活化的ZnSO ₄电解质中 ZMA 的有效亥姆霍兹平面 (HP) 重构机制。系统实验和数值模拟表明，具有双亲锌末端的游离 PCA 阴离子优先附着在 ZMAs 表面，羧基作为锚取代 H ² _O和 SO ₄ ²⁻，重塑 H ₂ O/SO ₄ ^{2 −}- 防水 HP 可抑制水引发的副反应。^{同时，PCA -}阴离子的其他游离亲锌羰基末端赋予重构的 HP 对 Zn ²⁺的空间限制作用，有效抑制其在 Zn 沉积过程中猖獗的面内扩散和均匀化离子通量。此外，HP 表现出自我修复行为，可防止循环时意外的电极表面损坏。受益于能够实现更稳定的 ZMA/电解质界面化学的多功能 HP，出色的 Zn||Zn 对称电镀/剥离循环耐久性超过 300 小时，放电深度高达 40%（20 mA cm -2 /20 ^mAh cm ^{- 2个}）实现了，与没有 PCA-Zn 添加剂（仅 960 次循环后出现故障）相比，carbon-cloth@polyaniline||ZMA 全 AZMB 的可充电性（5000 次循环后容量保持率为 89.7%）显着提高。