Aqueous zinc‐ion batteries (ZIBs) are playing an increasingly important role in the field of energy storage. However, their practical applications are handicapped by severe dendrite formation and side reactions on zinc anodes. Herein, a low‐concentration high‐entropy (HE) electrolyte strategy is proposed to achieve high reversibility and ultra‐durable zinc metal anode. Specifically, this HE electrolyte features multiple anions participating in coordination and highly disordered solvation shells, which would disrupt intrinsic H‐bond network between water molecules and suppress interfacial side reactions. Moreover, these diversified weakly solvated structures can lower solvation energy of Zn2+ solvation configurations and enhance zinc ion diffusion kinetics, promoting uniform Zn deposition and electrode interface stability. Consequently, Zn||Zn symmetric cells exhibit over 2,000 hours of cycling stability, and Zn||Cu asymmetric cells achieve high average Coulombic efficiency of 99.9% over 500 cycles. Furthermore, the Zn||PANI full cell with optimized HE‐50mM electrolyte delivers a high specific capacity of 110.7 mAh g‐1 over 2,000 cycles at 0.5 A g‐1 and a capacity retention of 70.4% at 15 A g‐1 after 10,000 cycles. Remarkably, even at a low temperature of ‐20 °C, the Zn||PANI full cells equipped with HE‐50mM electrolyte still demonstrate long‐term cycling stability over 600 cycles with high‐capacity retention of 93.5%.

中文翻译：

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用于超稳定锌金属负极的高熵电解质，具有高无序溶剂化结构


水系锌离子电池 （ZIB） 在储能领域发挥着越来越重要的作用。然而，它们的实际应用受到严重的枝晶形成和锌阳极上的副反应的阻碍。在此，提出了一种低浓度高熵 （HE） 电解质策略，以实现高可逆性和超耐用的锌金属负极。具体来说，这种 HE 电解质具有多个阴离子参与配位和高度无序的溶剂化壳层，这将破坏水分子之间的内禀 H-键网络并抑制界面副反应。此外，这些多样化的弱溶剂化结构可以降低 Zn2+ 溶剂化构型的溶剂化能并增强锌离子扩散动力学，促进 Zn 均匀沉积和电极界面稳定性。因此，Zn||Zn 对称电池表现出超过 2,000 小时的循环稳定性，并且 Zn||Cu 不对称电池在 500 次循环中实现了 99.9% 的平均库仑效率。此外，Zn||采用优化的 HE-50 mM 电解液的 PANI 全电池在 0.5 A g-1 下循环 2,000 次循环可提供 110.7 mAh g-1 的高比容量，在 10,000 次循环后，在 15 A g-1 下可提供 70.4% 的容量保持率。值得注意的是，即使在 -20 °C 的低温下，Zn||配备 HE-50 mM 电解质的 PANI 全电池在 600 次循环中仍表现出长期循环稳定性，高容量保留率为 93.5%。