All-polymer aqueous batteries, using polymers for electrodes and electrolytes, offer advantages for wearable electronics due to their ease of processing, inherent safety, and sustainability. However, instability of polymer electrode redox products in aqueous environments limits performance. This work reports a polymer-aqueous electrolyte that stabilizes these products by modulating solvation layers and forming a solid-electrolyte interphase (SEI). Polyaniline (PANI), used as symmetric electrodes, demonstrates high capacity (139 mAh/g), energy density (153 Wh/kg), and cycle life (92% retention after 4800 cycles). Spectroscopic analyses elucidate the hydration structure, SEI, and dual-ion doping mechanism. Large-scale flexible batteries showcase excellent flexibility and recyclability, signifying a new approach to sustainable, wearable energy storage.

Yang Hong, Kangkang Jia, Yueyu Zhang, Ziyuan Li, Junlin Jia, Jing Chen, Qimin Liang, Huarui Sun, Qiang Gao, Dong Zhou, Ruhong Li, Xiaoli Dong, Xiulin Fan, Sisi He