A high performance composite separator with robust environmental stability for dendrite-free lithium metal batteries

The garnet ceramic Li_6.4La₃Zr_1.4Ta_0.6O₁₂ (LLZTO) modified separators have been proposed to overcome the poor thermal stability and wettability of commercial polyolefin separators. However, the side reaction of LLZTO in the air leads to deterioration of environmental stability of composite separators (PP-LLZTO), which will limit the electrochemical performance of batteries. Herein, the LLZTO with the polydopamine (PDA) coating (LLZTO@PDA) was prepared by solution oxidation, and then applied it to a commercial polyolefin separator to achieve a composite separator (PP-LLZTO@PDA). LLZTO@PDA is stable in the air, and no Li₂CO₃ can be observed on the surface even after 90 days in the air. Besides, LLZTO@PDA coating endows the PP-LLZTO@PDA separator with the tensile strength (up to 103 MPa), good wettability (contact angle 0°) and high ionic conductivity (0.93 mS cm^-1). Consequently, the Li/PP-LLZTO@PDA/Li symmetric cell cycles stably for 600 h without significant dendrites generation, and the assembled Li//LFP cells with PP-LLZTO@PDA-D30 separators deliver a high capacity retention of 91.8% after 200 cycles at 0.1C. This research provides a practical strategy for constructing composite separators with excellent environmental stability and high electrochemical properties.