Toward Simultaneous Dense Zinc Deposition and Broken Side‐Reaction Loops in the Zn//V2O5 System

Abstract The Zn//V 2 O 5 system not only faces the incontrollable growth of zinc (Zn) dendrites, but also withstands the cross‐talk effect of by‐products produced from the cathode side to the Zn anode, inducing interelectrode talk and aggravating battery failure. To tackle these issues, we construct a rapid Zn 2+ ‐conducting hydrogel electrolyte (R‐ZSO) to achieve Zn deposition modulation and side reaction inhibition in Zn//V 2 O 5 full cells. The polymer matrix and BN exhibit a robust anchoring effect on SO 4 2− , accelerating Zn 2+ migration and enabling dense Zn deposition behavior. Therefore, the Zn//Zn symmetric cells based on the R‐ZSO electrolyte can operate stably for more than 1500 h, which is six times higher than that of cells employing the blank electrolyte. More importantly, the R‐ZSO hydrogel electrolyte effectively decouples the cross‐talk effects, thus breaking the infinite loop of side reactions. As a result, the Zn//V 2 O 5 cells using this modified hydrogel electrolyte demonstrate stable operation over 1,000 cycles, with a capacity loss rate of only 0.028 % per cycle. Our study provides a promising gel chemistry, which offers a valuable guide for the construction of high‐performance and multifunctional aqueous Zn‐ion batteries.