A Multifunctional Gradient Solid Electrolyte Remarkably Improving Interface Compatibility and Ion Transport in...

Solid electrolytes with both interface compatibility and efficient ion transport have been an urgent technical requirement for the practical application of solid-state lithium batteries. Herein, a multifuctional poly(1,3-dioxolane) (PDOL) electrolyte combining the gradient structure from the solid state to the gel state with the Li_6.4La₃Zr_1.4Ta_0.6O₁₂ (LLZTO) interfacial modification layer was designed, in which the "solid-to-gel" gradient structure greatly improved the electrode/electrolyte interface compatibility and ion transport, while the solid PDOL and LLZTO layers effectively improved the interface stability of the electrolyte/lithium anode and the inhibition of the lithium dendrites via their high mechanical strength and forming a stable interfacial SEI composite film. This gradient PDOL/LLZTO composite electrolyte possesses a high ionic conductivity of 2.9 × 10^-4 S/cm with a wide electrochemical window up to 4.9 V vs Li/Li⁺. Compared with the pristine PDOL electrolyte and PDOL solid electrolyte membrane coated with a layer of LLZTO, the gradient PDOL/LLZTO composite electrolyte shows better electrode/electrolyte interfacial compatibility, lower interface impedance, and smaller polarization, resulting in enhanced rate and cycle performances. The NCM622/PDOL-LLZTO/Li battery can be stably cycled 200 times at 0.3C and 25 °C. This multifunctional gradient structure design will promote the development of high-performance solid electrolytes and is expected to be widely used in solid-state lithium batteries.