ABSTRACT Zn‐based batteries are promising candidates for sustainable, large‐scale energy storage. However, their practical deployment is hindered by dendritic Zn growth, parasitic side reactions and sluggish interfacial Zn 2+ transport. Inspired by phospholipid membranes, we introduce a biomimetic zwitterionic hydrogel electrolyte (PAMC) to integrate 2‐methacryloyloxyethyl phosphorylcholine, polyacrylamide and trace acrylic acid into a mechanically robust network featuring strong electrode adhesion and hierarchical Zn 2+ pathways. The zwitterionic moieties regulate the primary Zn 2+ solvation structure by partially replacing water ligands, thereby reducing the desolvation energy barriers and homogenize Zn 2+ flux at the electrode interface. Consequently, PAMC delivers a high ionic conductivity of 44.94 mS cm −1 and a record Zn 2+ transference number of 0.75, enabling dendrite‐free Zn deposition and suppressed hydrogen evolution. Symmetric Zn||Zn cells exhibit stable cycling for over 2200 h, while Zn||Cu cells maintain highly reversible Zn plating/stripping for more than 2000 h. Furthermore, full cells with activated carbon, NaV 3 O 8 and I 2 cathodes demonstrate outstanding cycling stability and rate capability. When integrated with a perovskite solar cell, the Zn||I 2 battery achieves an overall conversion efficiency of 13.3%, representing the highest reported to date for this category. This biomimetic electrolyte design establishes a universal platform for highly reversible Zn anodes and sustainable energy‐storage systems.
Guo et al. (Sun,) studied this question.
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