Long‐lifespan Zinc‐ion Capacitors Enabled by Anodes Integrated with Interconnected Mesoporous Chitosan Membranes through Electrophoresis‐driven Phase Separation

Abstract The advancement of highly secure and inexpensive aqueous zinc ion energy storage devices is impeded by issues, including dendrite growth, hydrogen evolution and corrosion of zinc anodes. It is essential to modify the interface of zinc anodes that homogenizes ion flux and facilitates highly reversible zinc planarized deposition and stripping. Herein, by coupling zinc ion coordination with acid‐base neutralization under the driving of electrophoresis, manageable mesoscopic phase separation for constructing chitosan frameworks was achieved, thereby fabricating interconnected mesoporous chitosan membranes based heterogeneous quasi‐solid‐state electrolytes integrated with anodes. The framework is constructed by twisted chitosan nanofiber bundles, forming a three‐dimensional continuous spindle‐shaped pore structure. With this framework, the electrolyte provides exceptional ion conductivity of 25.1 mS cm −1 , with a puncture resistance strength of 2.3 GPa. In addition, the amino groups of chitosan molecule can make the surface of the framework positively charged. Thus, reversible zinc planarized deposition is successfully induced by the synergistic effect of stress constraint and electrostatic modulation. As a result, as‐assembled zinc ion capacitor has an excellent cycle life and sustains the capacity by over 95 % after 20000 cycles at a current density of 5 A g −1 . This research presents a constructive strategy for stable electrolytes‐integrated zinc anodes.