High‐Fluidity/High‐Strength Dual‐Layer Gel Electrolytes Enable Ultra‐Flexible and Dendrite‐Free Fiber‐Shaped Aqueous Zinc Metal Battery

Abstract Fiber‐shaped aqueous zinc‐ion batteries (FAZIBs) with intrinsic safety, highcapacity, and superb omnidirectional flexibility hold promise for wearable energy‐supply devices. However, the interfacial separation of fiber‐shaped electrodes and electrolytes caused by Zinc (Zn) stripping process and severe Zn dendrites occurring at the folded area under bending condition seriously restricts FAZIBs' practical application. Here, an advanced confinement encapsulation strategy is originally reported to construct dual‐layer gel electrolyte consisting of high‐fluidity polyvinyl alcohol‐Zn acetate inner layer and high‐strength Zn alginate outer layer for fiber‐shaped Zn anode. Benefiting from the synergistic effect of inner‐outer gel electrolyte and the formation of solid electrolyte interphase on Zn anode surface by lysine additive, the resulting fiber‐shaped Zn‐Zn symmetric cell delivers long cycling life over 800 h at 1 mA cm −2 with dynamic bending frequency of 0.1 Hz. The finite element simulation further confirms that dual‐layer gel electrolyte can effectively suppress the interfacial separation arising from the Zn stripping and bending process. More importantly, a robust twisted fiber‐shaped Zn/zinc hexacyanoferrate battery based on dual‐layer gel electrolyte is successfully assembled, achieving a remarkable capacity retention of 97.7% after bending 500 cycles. Therefore, such novel dual‐layer gel electrolyte design paves the way for the development of long‐life fiber‐shaped aqueous metal batteries.