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Mechanically Adaptive Polyrotaxane Interlayers for Low-Pressure High Energy Density Sulfide-Based All-Solid-State

Jihoon Oh1,2, Leonie Braks3, Ali Coskun3

  • 1School of Chemical and Biological Engineering, Institute of Chemical Process, Seoul National University, Seoul, Republic of Korea.

Angewandte Chemie (International Ed. in English)
|May 15, 2026
PubMed
Summary

A novel mechanically adaptive anode interface using polyrotaxane (PR) and indium fluoride (InF3) enhances all-solid-state battery (ASSB) performance. This breakthrough ensures stable operation under low pressure, crucial for high-energy-density applications.

Keywords:
all‐solid‐state batterieslithium metal anodeslow‐pressure operationpolyrotaxaneself‐healing

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Polymer Science

Background:

  • All-solid-state batteries (ASSBs) offer high energy density but struggle with performance under low stack pressure, especially with lithium metal or anode-less designs.
  • Mechanical instability and void formation at interfaces lead to battery degradation, limiting practical applications.

Purpose of the Study:

  • To develop a mechanically adaptive anode interface for ASSBs that maintains performance under low stack pressure.
  • To enable stable and reliable operation of high-energy-density ASSBs in commercially relevant conditions.

Main Methods:

  • Design of an elastic polymer interface incorporating mechanically interlocked polyrotaxane (PR).
  • Integration of indium fluoride (InF3) for spontaneous chemical interface stabilization.
  • Testing of the interface under low stack pressure (0.8 MPa) at 25°C, including anode-less configurations.

Main Results:

  • The PR-based interface demonstrated robust cycling stability and reliable performance.
  • The synergistic combination of PR's elastic resilience and InF3's chemical stability prevented void formation.
  • Successful operation was achieved even in anode-less configurations (N/P = 0) under low-pressure conditions.

Conclusions:

  • Mechanically interlocked molecular architectures offer a promising strategy for void-free interfaces in low-pressure ASSBs.
  • The developed adaptive interface significantly enhances the practical applicability of high-energy-density ASSBs.
  • This approach paves the way for more stable and efficient solid-state battery technologies.