In-Situ Polymerization of Monomers into Porous LiFePO4 Cathode for All-Solid-State Lithium Metal Batteries

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Solid-state Li metal batteries are about to transform the energy storage landscape by delivering high specific energy with improved safety. But the slow Li⁺ transport caused by tortuous pathways and high interfacial resistance remains a critical challenge. Here, we report an integrated cathode–catholyte–separator architecture in which a porous LiFePO₄ cathode is infiltrated with a cross-linkable polymer electrolyte to eliminate voids and maximize interfacial contact. The composite polymer electrolyte, which comprises polypropylene carbonate, polyethylene glycol methyl ether acrylate, polyethylene glycol diacrylate, and 2,2′-azobis(2-methylpropionitrile) with LiTFSI salt, extends above the cathode surface to form a continuous and controllable separator thickness. The composite exhibits an ionic conductivity of 5 × 10⁻⁴ S cm⁻¹ at 60 °C and a void-free microstructure confirmed by SEM–EDS mapping. Operando EIS under galvanostatic cycling reveals a slight impedance rise at 4.2 V and 2.4 V after 30 cycles, revealing the formation of solid electrolyte interphase and cathode electrolyte interphase. This architecture delivers a stable gravimetric capacity of ~150 mAh g⁻¹ at 80 mA g⁻¹ for 150 cycles. This work provides a practical route for kinetically favorable Li⁺ transport, offering a pathway toward high-performance solid-state Li metal batteries. Figure 1

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