An ionically cross-linked composite hydrogel electrolyte based on natural biomacromolecules for sustainable zinc-ion batteries†

Zinc-ion batteries (ZIBs) are regarded as promising power sources for flexible and biocompatible devices due to their good sustainability and high intrinsic safety. However, their applications have been hindered by the issues of uncontrolled Zn dendrite growth and severe water-induced side reactions in conventional liquid electrolytes. Herein, an ionically cross-linked composite hydrogel electrolyte based on natural biomacromolecules, including iota-carrageenan and sodium alginate, is designed to promote highly efficient and reversible Zn plating/stripping. The abundant functional groups of macromolecules effectively suppress the reactivity of water molecules and facilitate uniform Zn deposition. Moreover, the composite hydrogel electrolyte exhibits a high ionic conductivity of 5.89 × 10⁻² S cm⁻¹ and a Zn²⁺ transference number of 0.58. Consequently, the Zn‖Zn symmetric cell with the composite hydrogel electrolyte shows a stable cycle life of more than 500 h. Meanwhile, the Zn‖NH₄V₄O₁₀ coin cell with the composite hydrogel electrolyte retains a high specific capacity of approximately 200 mA h g⁻¹ after 600 cycles at 2 A g⁻¹. The Zn‖NVO pouch cell based on the composite hydrogel electrolyte also shows a high specific capacity of 246.1 mA h g⁻¹ at 0.5 A g⁻¹ and retains 70.7% of its initial capacity after 150 cycles. The pouch cell performs well at different bending angles and exhibits a capacity retention rate of 98% after returning to its initial state from 180° folding. This work aims to construct high-performance hydrogel electrolytes using low-cost natural materials, which may provide a solution for the application of ZIBs in flexible biocompatible devices.