Amphoteric Cellulose‐Based Double‐Network Hydrogel Electrolyte Toward Ultra‐Stable Zn Anode

Abstract Zinc (Zn) metal anode suffers from uncontrollable Zn dendrites and parasitic side reactions at the interface, which restrict the practical application of aqueous rechargeable zinc batteries (ARZBs). Herein, an amphoteric cellulose‐based double‐network is introduced as hydrogel electrolyte to overcome these obstacles. On one hand, the amphoteric groups build anion/cation transport channels to regulate electro‐deposition behavior on Zn (002) crystal plane enabled by homogenizing Zn 2+ ions flux. On the other hand, the strong bonding between negatively charged carboxyl groups and Zn 2+ ions promote the desolvation process of [Zn(H 2 O) 6 ] 2+ to eliminate side reactions. Based on the above two functions, the hydrogel electrolyte enables an ultra‐stable cycling with a cumulative capacity of 7 Ah cm −2 at 20 mA cm −2 /20 mAh cm −2 for Zn||Zn cell. This work provides significant concepts for developing hydrogel electrolytes to realize stable anode for high‐performance ARZBs.