An Asymmetric Cross-Linked Ionic Copolymer Hybrid Solid Electrolyte with Super Stretchability for Lithium-Ion...

Composite solid electrolytes are recommended to be the most promissing strategy for solid-state batteries because they combine the advantages of inorganic ceramics and polymers. However, the huge interfacial resistance between the inorganic ceramic and polymer results in low ionic conductivity, which is still the major impediment that limits their applications. Herein, a novel highly elastic and weakly coordinated ionic copolymer hybrid electrolyte with asymmetric structure based on surface-modified Li_1.5 Al_0.5 Ge_1.5 (PO₄ )₃ by "in situ" polymerization is proposed to improve ionic conductivity and mechanical properties simultaneously. The all-solid hybrids electrolytes exhibit room-temperature ionic conductivity up to 2.61 × 10^-4 S cm^-1 and lithium-ion transference number of 0.41. The hybrids electrolytes can be repeatedly stretching-releasing-stretching, showing a super stretchability with the elongation at break up to 496%. The Li symmetrical cells assembled with the hybrid electrolytes can continuously operate for 800 h at 0.1 mA cm^-2 without discernable dendrites, indicating good interfacial compatibility between the hybrid electrolytes and lithium electrodes. The Li|LiFePO₄ batteries assembled with the hybrid electrolytes deliver an initial discharge specific capacity of 165.5 mAh g^-1 with an initial coulombic efficiency of 94.8% and 154 mAh g^-1 after 100 cycles at 0.1 C, and maintain 95.4% capacity retention after 100 cycles at 0.5 C.