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The liquid electrolyte in conventional zinc/manganese dioxide (Zn/MnO2) batteries conduces to the capacity limitation of one‐electron redox from MnO2 to MnOOH, as well as undesired Mn loss with capacity deterioration. Herein, to conquer these challenges, a new idea is proposed on the precise proton redistribution in the hydrogel electrolyte for the preferred two‐electron redox reaction. Specifically, an acidic layer in the hydrogel adjoins the MnO2 cathode to maintain the two‐electron redox, a neutral layer adjoins the zinc anode to inhibit the dendrite growth, which is separated by a mildly alkaline layer to immobilize the proton distribution. The two‐electron redox of MnO2/Mn2+ and anode protection are demonstrated to play key roles in battery performance. Such a battery presents specific capacities of 516 mA h g−1 at 0.05 A g−1, as well as a capacity retention of 93.18% at 5 A g−1 after 5000 cycles without extra Mn2+ addition in the electrolyte. More importantly, fibrous Zn/MnO2 batteries using the tri‐layer electrolyte can sustain 2000 cycles with high initial capacity of 235 mAh g−1 at 1 A g−1. After 6000 times folding in 180°, it can maintain 99.54% capacity. When integrated into user's clothing or portable accessories, the fibrous battery is demonstrated as a great potential in wearable electronics. [ABSTRACT FROM AUTHOR]

Precise Proton Redistribution for Two-Electron Redox in Aqueous Zinc/Manganese Dioxide Batteries (Adv. Keywords: fibrous Zn/MnO 2 batteries; high specific capacity; hydrogel electrolytes; prolonged cycling stability; two-electron redox EN fibrous Zn/MnO 2 batteries high specific capacity hydrogel electrolytes prolonged cycling stability two-electron redox 1 1 1 11/08/21 20211104 NES 211104 B Zn/MnO SB 2 sb Batteries b In article number 2102055, Yagang Yao, Guo Hong and co-workers develop a tri-layer hydrogel electrolyte to precisely redistribute protons in aqueous zinc/MnO SB 2 sb batteries, which synchronously triggers two-electron redox of MnO SB 2 sb /Mn SP 2+ sp at the cathode and zinc protection at the anode. Fibrous Zn/MnO 2 batteries, high specific capacity, hydrogel electrolytes, prolonged cycling stability, two-electron redox. [Extracted from the article]