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Solid-state Graft Copolymer Electrolytes for Lithium Battery Applications
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Regulating Interface Dipole Interaction between Ethers and Active Species Toward Highly Stable Li-SPAN Batteries.

Xinyi Liu1, Shuang Wu1, Zhimeng Hao1

  • 1Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071, China.

Angewandte Chemie (International Ed. in English)
|November 6, 2024
PubMed
Summary

A new dipropyl ether electrolyte enhances sulfurized polyacrylonitrile (SPAN) cathodes in lithium metal batteries. This innovation improves cycle stability and extreme-temperature performance, addressing capacity fading and shuttle effects for longer battery life.

Keywords:
Li-SPAN batteriesdipole interactionelectrode electrolyte interphasesolvation structurewide temperature range

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Sulfurized polyacrylonitrile (SPAN) is a promising organic cathode material for long-lifespan lithium metal batteries.
  • Conventional ether-based electrolytes lead to irreversible sulfur-sulfur bond cleavage, causing capacity fading and shuttle effects in SPAN batteries.
  • Stable electrolyte-electrode interfaces (EEI) are crucial for high-performance lithium-organic batteries.

Purpose of the Study:

  • To develop a novel electrolyte for lithium-sulfurized polyacrylonitrile (Li-SPAN) batteries to overcome limitations of conventional electrolytes.
  • To investigate the impact of a dipropyl ether (PE) based electrolyte on battery performance, particularly cycle stability and extreme-temperature operation.
  • To demonstrate a strategy for modulating electrolyte-electrode interactions for enhanced Li-organic battery longevity.

Main Methods:

  • A new electrolyte solvent, dipropyl ether (PE), was formulated for Li-SPAN batteries.
  • Electrolyte properties such as desolvation energy barrier and Li+ transference number were evaluated.
  • Electrolyte-electrode interface (EEI) stability was assessed.
  • Full cells and an Ah-scale pouch cell were assembled and tested for cyclability, capacity retention, and performance at extreme temperatures (-50°C to 50°C).

Main Results:

  • The PE-based electrolyte exhibited a low desolvation energy barrier and a high Li+ transference number.
  • A stable electrolyte-electrode interface (EEI) was achieved, mitigating irreversible S-S bond cleavage.
  • Full cells demonstrated good cyclability, high capacity retention, and superior performance across a wide temperature range.
  • An Ah-scale pouch cell achieved 96.5% capacity retention after 75 cycles with lean electrolyte, delivering an initial specific energy density of 150 Wh/kg.
  • The PE-based electrolyte strategy proved effective for various organic electrodes.

Conclusions:

  • The dipropyl ether electrolyte effectively suppresses irreversible S-S bond cleavage and shuttle effects in SPAN cathodes.
  • This electrolyte enables long-cycle stability, high capacity retention, and excellent extreme-temperature performance for Li-SPAN batteries.
  • The strategy of modulating dipole interactions at the EEI using PE-based electrolytes offers a universal approach for developing long-lasting Li-organic batteries under demanding conditions.