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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]

As one of the most promising candidates in wearable energy storage devices, aqueous fibrous zinc metal batteries (AFZMBs) remain limited by some severe challenges, such as short life span and unstable capacity performance, etc. In this work, the stability of AFZMB is extended by fabricating an innovative stratified deposition framework (SDF) anode. The as‐prepared SDF electrode can achieve a stratified deposition of Zn metals from the bottom layer to the top layer due to the different overpotentials and binding energy of Zn deposition. Compared with commercial Zn fibers, this dexterous structure provides enough deposition space for Zn metals between the separator and the electrode, dramatically alleviating conventional dendrite puncture and prolonging life expectancy by an order of magnitude. It is found that SDF/AFZMB exhibits a long circulation of 2000 cycles with 89.0% capacity retention at 5 C with superior flexibility, demonstrating potential for application in future wearable electronics. [ABSTRACT FROM AUTHOR]

Keywords: aqueous electrolyte; fibrous zinc battery; flexibility; prolonged cycling; stratified deposition framework EN aqueous electrolyte fibrous zinc battery flexibility prolonged cycling stratified deposition framework 1 1 1 04/29/21 20210428 NES 210428 In article number 2100214, Yagang Yao, Guo Hong and co-workers improve the cycling stability of the aqueous fibrous zinc metal batteries by controlling the zinc deposition priority from bottom to surface in an innovative stratified deposition framework anode, which minimizes the growth of zinc dendrites and boosts the development of wearable devices. Aqueous electrolyte, fibrous zinc battery, flexibility, prolonged cycling, stratified deposition framework Zinc Metal Batteries: Stratified Zinc-Binding Strategy toward Prolonged Cycling and Flexibility of Aqueous Fibrous Zinc Metal Batteries (Adv. [Extracted from the article]