Manipulating Deposition Behavior by Polymer Hydrogel Electrolyte Enables Dendrite‐Free Zinc Anode for Zinc‐Ion Hybrid Capacitors

Rechargeable aqueous zinc-ion hybrid capacitors (ZHCs) have aroused unprecedented attention because of their high safety, cost effectiveness, and environmental compatibility. However, the intractable issues of dendrite growth and side reactions at the electrode-electrolyte interface deteriorate durability and reversibility of Zn anodes, deeply encumbering the large-scale application of ZHCs. Concerning these obstacles, a negatively charged carboxylated chitosan-intensified hydrogel electrolyte (CGPPHE) with cross-linked networks is reported to stabilize Zn anodes. Beyond possessing good mechanical characteristics, the CGPPHE with polar groups can reduce the desolvation energy barrier of hydrated Zn2+ , constrain the 2D Zn2+ diffusion, and uniformize electric field and Zn2+ flux distributions, assuring dendrite-free Zn deposition with high plating-stripping efficiency. Concurrently, the hydrophilic CGPPHE alleviates harmful hydrogen evolution and corrosion by abating water activity. Accordingly, Zn|CGPPHE|Zn and Zn|CGPPHE|Cu cells exhibit an extended life exceeding 350 h (1600 mAh cm-2 cumulative capacity under 20 mA cm-2 ) and a high average coulombic efficiency of 98.2%, respectively. The resultant flexible ZHCs with CGPPHE and template-regulated carbon cathode present perfect properties in capacity retention (97.7% over 10 000 cycles), energy density (91.8 Wh kg-1 ), and good mechanical adaptability. This study provides insight into developing novel hydrogel electrolytes toward highly rechargeable and stable ZHCs.