Dynamic Migration‐Pulling Polymer Electrolyte Design Strategy for Low‐Temperature Lithium–Sulfur Batteries

W Wenkai Song B Borui Li (School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)) Y Yunpeng Qu (School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)) W Wanyuan Jiang (State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, School of Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)) M Mengfan Pei (School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)) N Naiwen Hu (School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)) S Shuo Zhuo (School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)) C Chang Su (School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)) X Xin Jin R Runyue Mao (School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)) D Dongming Liu (School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)) X Xigao Jian (School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)) F Fangyuan Hu (School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province))

Abstract

Abstract Quasi‐solid‐state lithium–sulfur batteries exhibit significant promise as safe, high‐energy electrochemical storage technology, yet their performance remains constrained by polysulfide accumulation and exacerbated shuttle effects due to sluggish redox kinetics and inefficient charge transport. Here, a dynamic migration‐pulling strategy is proposed to accelerate polysulfide redox kinetics by dynamically restructuring the solvated structure of Li + , which is validated on a GPE incorporating boronic ester dynamic covalent bonds and polar side chains (BE‐GPE). Theoretical calculations and experiments revealed that the desolvation barrier for Li + is significantly reduced, while the ligand groups were pulled out from the solvated shell assisted by the migration of dynamic covalent bonds. Rapid charge transfer kinetics are attainable via designed electrolyte. Consequently, BE‐GPE based lithium–sulfur batteries delivered high reversible capacity of 1446 mAh g −1 at 0.1 C and long‐term cycling stability with an average capacity decay of 0.04% during 1000 cycles at 0.5 C. The initial capacity at 0.5 C is up to 920 mAh g −1 and remains stable for 200 cycles at 0 °C. Successfully realized the energy storage of quasi‐solid‐state Li–S batteries under low‐temperature conditions.

Article Details

Volume / Issue Vol. 64, Issue 29
Published July 14, 2025
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (13)

W

Wenkai Song

B

Borui Li

School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)

Y

Yunpeng Qu

School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)

W

Wanyuan Jiang

State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, School of Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)

M

Mengfan Pei

School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)

N

Naiwen Hu

School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)

S

Shuo Zhuo

School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)

C

Chang Su

School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)

X

Xin Jin

R

Runyue Mao

School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)

D

Dongming Liu

School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)

X

Xigao Jian

School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)

F

Fangyuan Hu

School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province)