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Hydrogen-Bond-Networked Robust Binder Enabling Long-Cycling Sulfide-Based All-Solid-State Lithium Batteries.

Wenjun Zhang1,2,3, Pengzhou Mu2,3, Chenghao Sun2,3

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A new polymer binder, PNO, enables scalable wet processing for sulfide all-solid-state lithium batteries (ASSBs). This binder enhances structural stability in thin electrolyte films and high-loading cathodes, improving battery cycling performance.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Polymer Chemistry

Background:

  • Scalable manufacturing of sulfide-based all-solid-state lithium batteries (ASSBs) via wet processing requires binders compatible with low-polarity solvents and sulfides.
  • Existing binders struggle to achieve thin sulfide solid electrolyte (SSE) films (≤ 30 µm) and high-loading composite cathodes (≥ 30 mg cm⁻²).

Purpose of the Study:

  • To develop a novel binder enabling efficient wet processing for practical ASSBs.
  • To improve the mechanical integrity and processability of SSE films and composite cathodes.

Main Methods:

  • Design of a dynamic hydrogen bonding-empowered robust polymer (PNO) binder utilizing soft-hard segment synergism.
  • Incorporation of polybutadiene soft segments for processability and carbamate-containing hard segments for mechanical strength via dynamic hydrogen bonding.
  • Fabrication and testing of ASSBs with PNO binder-based cathodes and SSE films.

Main Results:

  • The PNO binder facilitates the formation of thin SSE films and high-loading composite cathodes.
  • Dynamic hydrogen bonding in PNO enhances mechanical strength and stress dissipation, ensuring structural stability during processing and cycling.
  • ASSBs assembled with PNO binder demonstrated outstanding cycling stability, outperforming recently reported sulfide-based ASSBs.

Conclusions:

  • The soft-hard segment synergism binder design strategy overcomes key bottlenecks in wet processing of ASSBs.
  • PNO binder is conducive to accelerating the scale-up production of advanced sulfide-based ASSBs.
  • This approach offers a pathway for developing high-performance, manufacturable solid-state batteries.