Simultaneous Inhibition of Vanadium Dissolution and Zinc Dendrites by Mineral‐Derived Solid‐State Electrolyte for High‐Performance Zinc Metal Batteries

Designing solid electrolyte is deemed as an effective approach to suppress the side reaction of zinc anode and active material dissolution of cathodes in liquid electrolytes for zinc metal batteries (ZMBs). Herein, kaolin is comprehensively investigated as raw material to prepare solid electrolyte (KL−Zn) for ZMBs. As demonstrated, KL−Zn electrolyte is an excellent electronic insulator and zinc ionic conductor, which presents wide voltage window of 2.73 V, high ionic conductivity of 5.08 mS cm−1, and high Zn2+ transference number of 0.79. For the Zn//Zn cells, superior cyclic stability lasting for 2200 h can be achieved at 0.2 mA cm−2. For the Zn//NH4V4O10 batteries, stable capacity of 245.8 mAh g−1 can be maintained at 0.2 A g−1 after 200 cycles along with high retention ratio of 81 %, manifesting KL−Zn electrolyte contributes to stabilize the crystal structure of NH4V4O10 cathode. These satisfying performances can be attributed to the enlarged interlayer spacing, zinc (de)solvation‐free mechanism and fast diffusion kinetics of KL−Zn electrolyte, availably guaranteeing uniform zinc deposition for zinc anode and reversible zinc (de)intercalation for NH4V4O10 cathode. Additionally, this work also verifies the application possibility of KL−Zn electrolyte for Zn//MnO2 batteries and Zn//I2 batteries, suggesting the universality of mineral‐based solid electrolyte. Kaolin is demonstrated as an effective material to prepare Zn‐based solid electrolyte (KL‐Zn), which simultaneously eliminates the interfacial side reactions of zinc anode and inhibits the vanadium dissolution of NH4V4O10 cathode, endowing high reversible capacity and superior cyclic stability for Zn//NH4V4O10 batteries.