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The interionic forces of the strong electrolytes depend on the solvent's dielectric constant, which is the ability of a solvent to store electrical energy, based on its polarizability. and the solution's concentration. In high-dielectric solvents and in dilute solutions, weak electrostatic forces keep ions apart. However, in low-dielectric solvents or concentrated solutions, stronger interionic forces may cause ions to pair up as ionic doublets despite being fully ionized. The theory of strong...
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Solid-state Graft Copolymer Electrolytes for Lithium Battery Applications
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Interface Engineered Electrolyte Design Strategy for Ultralong-Cycle Solid-State Lithium Batteries Over Wide

Yunpeng Qu1, Chang Su1, Lin Wang1

  • 1School 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.

Angewandte Chemie (International Ed. in English)
|April 23, 2025
PubMed
Summary

A novel fluoropolymer-containing plastic-crystal electrolyte (FPCE) enables stable solid-state lithium battery operation across wide temperatures. This electrolyte optimizes the solid electrolyte interface, preventing dendrite growth and enhancing cycle life.

Keywords:
In situ SEI formationLong cycle lifeSolid polymer electrolytesWide temperature range

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Polymer Science

Background:

  • Solid-state lithium batteries require stable operation over wide temperature ranges for practical applications.
  • Suboptimal ionic conductivity, lithium dendrite growth, and unstable interfaces limit battery cycle life at extreme temperatures.

Purpose of the Study:

  • To develop a fluoropolymer-containing plastic-crystal-based electrolyte (FPCE) for solid-state lithium batteries.
  • To optimize the solid electrolyte interface (SEI) for enhanced performance and stability.

Main Methods:

  • Structural engineering of a fluoropolymer-containing plastic-crystal-based electrolyte (FPCE).
  • Integration of solvent structure simulation and experimental validation.
  • Electrochemical testing of lithium iron phosphate (LFP)|FPCE|Li cells and Ah-level pouch cells.

Main Results:

  • FPCE effectively regulates Li+ transport and promotes the in-situ formation of a LiF-rich inorganic-organic hybrid SEI.
  • LFP|FPCE|Li cells demonstrated stable cycling for 5000 cycles at 10 C with minimal capacity decay (0.00448% per cycle).
  • Ah-level pouch cells operated stably between -10 °C and 80 °C.

Conclusions:

  • The developed FPCE enhances the overall stability of solid-state lithium batteries.
  • FPCE offers a valuable strategy for designing wide-temperature solid-state polymer electrolytes.
  • This work addresses key challenges for the practical application of solid-state lithium batteries at extreme temperatures.