Interface Engineered Electrolyte Design Strategy for Ultralong‐Cycle Solid‐State Lithium Batteries Over Wide Temperature Range

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)) 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)) L Lin Wang 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)) 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)) R Runyang 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) Dalian University of Technology Dalian 116024 China) 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)) W Wenkai Song 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)) X Xin Jin 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 Achieving stable operation under a wide temperature range is the direction of development for the practical application of solid‐state lithium batteries. However, the suboptimal ionic conductive properties exhibited by the electrolyte, the uncontrolled growth of lithium dendrites due to the deposition of inhomogeneous Li + and the potential safety hazards caused by unstable interfaces have seriously affected the cycle life of the battery at extreme temperatures. Herein, a fluoropolymer‐containing plastic‐crystal‐based electrolyte (FPCE) has been developed by means of a structural engineering process, with the objective of optimizing the solid electrolyte interface (SEI). The integration of solvent structure simulation and experimental results demonstrates that FPCE regulates Li + transport, promotes the in‐situ formation of the LiF‐rich inorganic–organic hybrid SEI, and enhances the overall stability of the battery. Consequently, FPCE assists in preserving stable LFP|FPCE|Li cells cycling, with 5000 cycles at a high current density of 10 C and an average capacity decay rate of merely 0.00448% per cycle. Furthermore, the Ah‐level pouch cells demonstrate the capacity to operate stably within the temperature range of −10 to 80 °C. This study provides a valuable strategy for the design of wide‐temperature solid‐state polymer electrolytes.

Article Details

Volume / Issue Vol. 64, Issue 27
Published July 01, 2025
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (13)

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)

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)

L

Lin Wang

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)

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)

R

Runyang 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) Dalian University of Technology Dalian 116024 China

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)

W

Wenkai Song

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)

X

Xin Jin

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)