Negatively Charged Laponite Sheets Enhanced Solid Polymer Electrolytes for Long-Cycling Lithium-Metal Batteries

Solid polymer electrolytes suffer from the low ionic conductivity and poor capability of suppressing lithium dendrites, which have greatly hindered the practical application of solid-state lithium-metal batteries. Here, we report a novel laponite sheet (LS) with a large negatively charged surface as an additive in a solid composite electrolyte (poly(ethylene oxide)-LS) to rearrange the lithium-ion environment and enhance the mechanical strength of the electrolytes (PEO-LS). The strong electrostatic regulation of laponite sheets assists the dissociation of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) and constructs multiple transport channels for free lithium ions, achieving a high ionic conductivity of 1.1 × 10^-3 S cm^-1 at 60 °C. Furthermore, LS facilitates the in situ formation of a LiF-rich interface because of the boosting TFSI^- anion concentration, which significantly suppresses lithium dendrites and prevents short circuit. As a result, the assembled LiFePO₄|PEO-LS|Li battery demonstrates a long cycle life of over 800 cycles and a high Coulombic efficiency of 99.9% at 1C and 60 °C. When paired with a high-voltage NCM811 cathode, the battery also demonstrates excellent cycling stability and rate capability.