Rational Design of F-Modified Polyester Electrolytes for Sustainable All-Solid-State Lithium Metal Batteries

• DOI: 10.1021/jacs.3c12094
• Publication Date: 2024-02-22T16:59:51Z
• Authors: Xiaoxin Xie; Peng Zhang; Xihui Li; Zhaoxu Wang; Xuan Qin; Minhua Shao; Liqun Zhang; Weidong Zhou
• Keywords: Adipate

Solid polymer electrolytes (SPEs) are one of the most practical candidates for solid-state batteries owing to their high flexibility and low production cost, but application is limited by Li+ conductivity a narrow electrochemical window. To improve performance, it necessary reveal structure–property relationship SPEs. Here, 23 fluorinated linear polyesters were prepared editing coordination units, flexible linkage segments, interface passivating groups. Besides traditionally demonstrated coordinating capability chains, molecular asymmetry resulting interchain aggregation observed critical conductivity. By tailoring ability polyesters, can be raised 10 times. Among these solvent-free poly(pentanediol adipate) delivers highest room-temperature 0.59 × 10–4 S cm–1. The chelating oxalate leads an electron delocalization alkoxy oxygen, enhancing antioxidation lower high-value LiTFSI in SPEs recycled at 90%, regenerated 86%. This work elucidates polyester-based SPEs, displays design principles provides way development sustainable batteries.