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For solid-state electrolyte in lithium-ion batteries, high crystal boundary impedance leads to tough electrolyte-electrode interfacial issues. Here, we introduce garnet Li6.4La3Zr1.4Ta0.6O12 (LLZTO) nanoparticles and succinonitrile (SN) into thermal polyurethane (TPU) to fabricate a composite solid-state electrolyte (TPU/LLZTO/SN), achieving high ionic conductivity of 6.452 × 10−4 S cm−1. The TPU polymer with specific soft and hard segments allows lithium ions fast transport and holds good mechanical strength as the electrolyte matrix. The ionic conductor LLZTO further improves the ionic conductivity and mechanical property of the composite electrolyte membrane. Additional SN supplies the electrolyte’ wide electrochemical stabilization window, and enhances the metallic lithium compatibility of the TPU matrix. As a result, the as prepared TPU/LLZTO/SN electrolyte presents high lithium ions transference number of 0.64, and also good mechanical property.

[Display omitted] • Thermal polyurethane with specific soft and hard segments is designed as the matrix of composite solid-state electrolyte. • Thermal polyurethane allows fast transport of lithium ions and holds good mechanical strength. • LLZTO nanoparticles enhance the ionic conductivity and strengthen the mechanical intensity. • The succinonitrile reduces the crystallization of the thermal polyurethane and facilitates the lithium ions transfer. For solid-state electrolyte in lithium-ion batteries, high crystal boundary impedance leads to tough electrolyte-electrode interfacial issues. Here, we introduce garnet Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) nanoparticles and succinonitrile (SN) into thermal polyurethane (TPU) to fabricate a composite solid-state electrolyte (TPU/LLZTO/SN), achieving high ionic conductivity of 6.452 × 10−4 S cm−1. The TPU polymer with specific soft and hard segments allows lithium ions fast transport and holds good mechanical strength as the electrolyte matrix. The ionic conductor LLZTO further improves the ionic conductivity and mechanical property of the composite electrolyte membrane. Additional SN supplies the electrolyte' wide electrochemical stabilization window, and enhances the metallic lithium compatibility of the TPU matrix. As a result, the as prepared TPU/LLZTO/SN electrolyte presents high lithium ions transference number of 0.64, and also good mechanical property. [ABSTRACT FROM AUTHOR]