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Tailoring electrolyte phase separation for high-rate solid-state lithium metal batteries
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DOI：10.1038/s41467-026-74094-w.png)
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Abstract
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Solid polymer electrolytes are attractive for solid-state lithium metal batteries due to their flexibility and safety but suffer from low ionic conductivity and unstable interfaces. Conventional polymerization-induced phase separation strategies enhance ion transport yet rely on external components such as deep eutectic solvents or ionic liquids, increasing cost and complexity. Here, a LiTFSI-mediated in-situ polymerization strategy is developed to induce controllable phase separation in a poly(vinylene carbonate) matrix using a single solvent. Electrostatic interactions between lithium salts and the polymer drive self-organized dual phases that combine mechanical robustness with efficient ion transport. The resulting PVC electrolyte achieves a tunable ionic conductivity from 0.20 to 0.92 mS/cm at 25 °C and a high lithium-ion transference number of 0.78. Li|PVC-24h | LiFePO4 cells achieve 121.4 mAh/g at 5 C (12 min) with 90% capacity retention after 4000 cycles, demonstrating a scalable approach for high-performance polymer electrolytes. The growing demand for portable electronics calls for lithium-ion batteries with higher energy density and longer cycle life. Here, the authors develop a facile phase-separation strategy to tailor polymer electrolytes through precise control of polymerization time, enabling high ionic conductivity, a large lithium-ion transference number and extended cycling stability in lithium metal batteries.
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