Intercepting Dendrite Growth With a Heterogeneous Solid Electrolyte for Long‐Life All‐Solid‐State Lithium Metal Batteries

Abstract

The application of lithium metal anode in all‐solid‐state batteries has the potential to achieve both high energy density and safety performance. However, the presence of serious dendrite issues hinders this potential. Here, the ion transport pathways and orientation of dendrite growth are regulated by utilizing the differences of ionic conductivity in heterogeneous electrolytes. The in situ formed Li–Ge alloy phases from the spontaneous reaction between Li10GeP2S12 and the attracted dendrites greatly enhance the ability to resist dendrite growth. As an outcome, the heterogeneous electrolyte achieves a high critical current density of 2.1 mA cm−2 and long‐term stable symmetrical battery operation (0.3 mA cm−2 for 17 000 h and 1.0 mA cm−2 for 2000 h). Besides, due to the superior interfacial stability and low interface impedance between the heterogeneous electrolyte and lithium anode, the Li||LiNi0.8Co0.1Mn0.1O2 full battery exhibits great cycling stability (80.5% after 500 cycles at 1.0 mA cm−2) and rate performance (125.4 mAh g at 2.0 mA cm−2). This work provides a unique strategy of interface regulation via heterogeneous electrolytes design, offering insights into the development of state‐of the‐art all‐solid‐state batteries.