Accelerated Single Li-Ion Transport in Solid Electrolytes for Lithium-Sulfur Batteries: Poly(Arylene Ether Sulfone) Grafted with Pyrrolidinium-Terminated Poly(Ethylene Glycol)

Polymeric solid electrolytes have attracted tremendous interest in high-safety and high-energy capacity lithium-sulfur (LiS) batteries. There is, however, still a dilemma to concurrently attain high Li-ion conductivity and high mechanical strength that effectively suppress the Li-dendrite growth. Accordingly, a rapidly Li-ion conducting solid electrolyte is prepared by grafting pyrrolidinium cation (PYR+)-functionalized poly(ethylene glycol) onto the poly(arylene ether sulfone) backbone (PAES-g-2PEGPYR). The PYR+ groups effectively immobilize anions of Li-salts in Li-conductive PEGPYR domains phase-separated from PAES matrix to enhance the single-ion conduction. The tailored PAES-g-2PEGPYR membrane shows a high Li-ion transference number of 0.601 and superior ionic conductivity of 1.38 mS cm-1 in the flexible solid state with the tensile strength of 1.0 MPa and Young's modulus of 1.5 MPa. Moreover, this PAES-g-2PEGPYR membrane exhibits a high oxidation potential (5.5 V) and high thermal stability up to 200 (C. The Li/PAES-g-2PEGPYR/Li cell stably operates for 1000 h without any short circuit, and the rechargeable Li/PAES-g-2PEGPYR/S cell discharges a capacity of 1004.7 mAh g-1 at C/5 with the excellent rate capability and the prominent cycling performance of 95.3% retention after 200 cycles. Self-assembled solid electrolyte prepared by grafting pyrrolidinium cation-functionalized poly(ethylene glycol) onto poly(arylene ether sulfone) backbone is beneficial for accelerating Li-ion transport in large conducting domains. This electrolyte membrane satisfying stimulation in improving ionic conductivity with high Li-ion selectivity and excellent mechanical/dimensional stability is expected to apply in lithium secondary battery with enhanced electrochemical performance and elimination of safety concerns.image