Polydopamine-Coated Garnet Particles Homogeneously Distributed in Poly(propylene carbonate) for the Conductive and Stable Membrane Electrolytes of Solid Lithium Batteries

Flexible membrane electrolytes consisting of Li6.4La3Zr1.4Ta0.6O12 (LLZTO) fillers in poly(propylene carbonate) (PPC) are considered promising for developing solid lithium batteries with high energy density and safety. However, LLZTO particles tend to agglomerate owing to their high surface energy, especially concerning their distribution in PPC that has low surface energy. Moreover, basic LLZTO particles attack PPC, resulting in its decomposition. Such problems make it difficult to achieve membrane electrolytes of PPC/LLZTO with high conduction and stability. In this work, continuous polydopamine (PDA) layers with a thickness of 4 nm are coated on LLZTO particles. Characterized by synchrotron X-ray microtomography and scanning electron microscopy, the PDA-coated LLZTO particles show homogeneous dispersion in PPC, which is attributed to the reduced surface energy of the LLZTO particles. Besides, this coating hinders the reaction between LLZTO and PPC, which improves the chemical stability of the membrane electrolytes. Consequently, the cells based on membrane electrolytes with PDA-coated LLZTO particles in PPC show improved electrochemical performance and cycling stability. These results demonstrate that the strategy of coating basic LLZTO particles is powerful for enhancing their usability in the high- performance membrane electrolytes for solid lithium batteries.