Poly(ethylene oxide) (PEO)-based polymer electrolytes are promising candidates for solid-state electrolytes in safer, next generation lithium metal batteries. Despite their benefits however, PEO-based electrolyte exhibits highly crystalline ethylene oxide chains that provide poor ionic conductivity and, thus severely limit its practical application. Here, we report the use of hydroxypropyl trimethylammonium bis(trifluoromethane) sulfonimide chitosan salt (HACC-TFSI), which is an amorphous poly(ionic liquid) based biomass chitosan derivative, as a modifier for PEO-based solid polymer electrolytes (SPEs) to address these deficiencies. Hybrid SPEs with HACC-TFSI display enlarged amorphous regions with enhanced ionic conductivity. Interactions between quaternary ammonium cations and TFSI⁻ anions in hybrid SPEs are also found to promote dissociation between Li⁺ and TFSI⁻, which further increases ionic mobility. Moreover, the electrochemical stability, mechanical strength, and thermal stability of hybrid SPEs are collectively superior to blank SPEs without HACC-TFSI. LiFePO₄/SPEs/Li full-cells assembled using 10wt% HACC-TFSI in PEO (10%HACC-TFSI/SPEs) electrolyte provide a capacity of 161.3 mAh g⁻¹ and operate with excellent cycle performances at 0.2 C and 60 °C. Even when the temperature is increased to 150 °C, LiFePO₄/SPEs/Li cells with 10%HACC-TFSI/SPEs still display remarkable cycle performance with 73% capacity retention after 100 cycles at 1 C rate.

聚环氧乙烷（PEO）基聚合物电解质是更安全的下一代锂金属电池中固态电解质的有希望的候选者。尽管有它们的优点，但是基于PEO的电解质仍显示出高结晶的环氧乙烷链，其提供差的离子电导率，因此严重限制了其实际应用。在这里，我们报告使用羟丙基三甲基铵双（三氟甲烷）磺酰亚胺壳聚糖盐（HACC-TFSI），它是一种基于无定形聚（离子液体）的生物质壳聚糖衍生物，作为基于PEO的固体聚合物电解质（SPEs）的改性剂解决这些缺陷。具有HACC-TFSI的混合SPE显示出具有增强的离子电导率的扩大的无定形区域。季铵阳离子与TFSI之间的相互作用^-在混合的SPE阴离子还发现，以促进锂之间的解离⁺和TFSI ^- ，这进一步增加了离子迁移率。此外，混合SPE的电化学稳定性，机械强度和热稳定性总体上优于不含HACC-TFSI的空白SPE。使用在PEO中的10wt％HACC-TFSI（10％HACC-TFSI / SPEs）电解质组装的LiFePO ₄ / SPEs / Li全电池可提供161.3 mAh g ^-1的容量，并在0.2 C和60°C下具有出色的循环性能。即使当温度升至150°C时，具有10％HACC-TFSI / SPEs的LiFePO ₄ / SPEs / Li电池在1 C速率100次循环后仍显示出卓越的循环性能，容量保持率达到73％。