Laponite-Supported Gel Polymer Electrolyte with Multiple Lithium-Ion Transport Channels for Stable Lithium Metal Batteries

Lithium metal batteries have emerged as a promising candidate for next-generation power systems. However, the high reactivity of lithium metal with liquid electrolytes has resulted in decreased battery safety and stability, which poses a significant challenge. Herein, we present a modified laponite-supported gel polymer electrolyte (LAP@PDOL GPE) that was fabricated using in situ polymerization initiated by a redox-initiating system at ambient temperature. The LAP@PDOL GPE effectively facilitates the dissociation of lithium salts via electrostatic interaction and simultaneously constructs multiple lithium-ion transport channels within the gel polymer network. This hierarchical GPE demonstrates a remarkable ionic conductivity of 5.16 × 10^-4 S cm^-1 at 30 °C. Furthermore, the robust laponite component of the LAP@PDOL GPE forms a barrier against Li dendrite growth while also participating in the establishment of a stable electrode/electrolyte interface with Si-rich components. The in situ polymerization process further improves the interfacial contact, enabling the LiFePO₄/LAP@PDOL GPE/Li cell to exhibit an impressive capacity of 137 mAh g^-1 at 1C, with a capacity retention of 98.5% even after 400 cycles. In summary, the developed LAP@PDOL GPE shows great potential in addressing the critical issues of safety and stability associated with lithium metal batteries while also delivering improved electrochemical performance.