This work reports a networked solid polymer electrolyte (N-u-SPE) for lithium-ion batteries (LIBs), which comprises a lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salt and poly(ethylene oxide) (PEO) chains cross-linked through poly(hexamethylene diisocyanate) (PHDI) by forming of urethane linkage. The networked configuration prevents crystallization between PEO chains, maintains high segmental motion and enhances the dissociation degree of lithium salt. The N-u-SPE exhibits a high ionic conductivity of 1.0 x 10-4 S cm-1 at 25 oC and small activation energy of 3.5 kJ mol-1 for ion motion. The N-u-SPE also exhibited fire self-extinguishing feature, which is beneficial to the safety of the resulting LIBs. A battery assembled using Li metal anode, LiFePO4 cathode, and the N-u-SPE, i.e., Li|N-u-SPE|LiFePO4, delivered a capacity of 158 mAh g-1 at 0.1 C (based on the theoretical capacity of LiFePO4, 170 mAh g-1) at room temperature and could be charged and discharged at 3 C. This battery exhibited excellent charge-discharge cycling stability, remaining approximate 140 mAh g-1 in capacity after 100 cycles of charge-discharge at 0.3 C. This work demonstrates the superiority of urethane linkages in suppressing crystallization tendency, enhancing lithium salt dissociation, ionic conductivity and mechanical strength to PEO-based SPEs for room temperature LIBs.

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