Ion Highway Regulator Enables Highly Reversible Zinc Metal Anode

ABSTRACT The issue of zinc dendrites and chaotic Zn 2+ deposition at electrode/electrolyte interface significantly hindered commercialization of aqueous zinc metal batteries (AZMBs). Therefore, we propose a Zn 2+ highway regulator strategy by introducing nano‐zirconium silicate interphase (ZSP) to address the above issues. ZSP with low Zn 2+ migration energy barrier of ZrSiO 4 can facilitate Zn 2+ transport efficiency and inhibit dendrite growth, thereby achieving highly reversible zinc metal anode. The featured ZSP@Zn//ZSP@Zn symmetric cell demonstrates an ultra‐long cycle life exceeding 4700 h at 0.25 mA cm −2 (0.25 mAh cm −2 ). Even under a deep depth of discharge ≈85.4%, it still maintains stable operation for over 400 h. Furthermore, the advanced NH 4 V 4 O 10 //ZSP@Zn full cell, featuring a high mass loading of 15.25 mg cm −2 (N/P = 2.1), exhibited stable performance over 520 cycles (1 A g −1 ), retaining 80.48% of initial capacity (187.32 mAh g −1 ). More surprisingly, the feature pouch cell with a loading of 11.96 mg cm −2 (N/P = 2.3) demonstrated excellent performance (maximum capacity of 209.22 mAh g −1 ), maintaining a capacity retention rate of 81.14% after 150 cycles at 0.8 A g −1 . This strategy provides a new avenue for highly reversible AZMBs.