Effect of LiTFSI Solvation on Ionic Conductivity of Polyester-Based Solid Electrolytes

溶剂化 离子电导率 结晶度 电解质 聚酯纤维 聚合物 离子键合 电导率 材料科学 高分子化学 化学 化学工程 物理化学 有机化学 离子 结晶学 电极 工程类
作者
Zhenzhen Yang,Jiahui Cai,Zitong Shen,Bian Jing,Jiashang Chen,Yao Xu,Zecheng Fang,Cuicui Du,Xing Xiang,Juan Wang,Peng Yu,Ruiyao Cui,Siwen Bi
出处
期刊:Macromolecules [American Chemical Society]
卷期号:57 (9): 4460-4470
标识
DOI:10.1021/acs.macromol.4c00045
摘要

Carbonyl-containing polymers have been considered promising candidates as hosts in solid polymer electrolytes (SPEs) due to the reasonable chelating coordination with Li+, better antioxidation for high-voltage cathodes, and higher ion transference number compared with polyether SPEs. In this work, four polyesters of poly(octamethylene succinate), poly(hexmethylene succinate) (PHS), poly(butylene succinate), and polycaprolactone were investigated. In these SPEs with different −C═O/–CH2– ratios, PHS had the highest conductivity (σ) of 1.24 × 10–4 S/cm because of the excellent ability to deionize bis(trifluoromethane)sulfonimide (LiTFSI) up to 88.3 ± 3.2% at 70 °C and the lowest activation energy of Li+ ionic conduction. The effect of Li+/–C═O ratios (r) on the ionic conductivity can be clarified into low-, middle-, and high-concentrated regions. The decrease of PHS crystallinity due to LiTFSI solvation provided ion transport paths and mainly contributed to the improvement of ionic conductivity in the middle-concentrated region, while the solvation degree dominantly facilitated ionic conduction in the high-concentrated region and at higher temperatures. By combining the DFT simulation and polymer thermal analysis, we found the transition of Li+ coordination from multichain to single-chain bindings provided more flexible segment movement. It also proved that the sequence design of active groups in a polymer chain would be a promising strategy for stable and high-performance SPEs.
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