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Design of Intrinsic Polyimides via a Restricted Dihedral-Rotation Structural Strategy for Superior High-Temperature

Bingyu Zou1,2, Shuo Zhao3, Yang Zhao3

  • 1School of Emergent Soft Matter, State Key Laboratory of Advanced Papermaking and Paper-based Materials, South China University of Technology, Guangzhou, China.

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Summary

This study enhances polyimide (PI) dielectrics for high-temperature applications by modifying their structure to suppress charge-transfer complexes (CTC) and improve energy density. The new materials offer superior performance in harsh environments.

Keywords:
Charge‐transfer complexesEnergy‐storage capacityIntrinsic polymer dielectricPolyimidesRestricted dihedral‐rotation structure

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Area of Science:

  • Materials Science
  • Polymer Chemistry
  • Electrical Engineering

Background:

  • Intrinsic polyimide (PI) dielectrics have limited energy-storage capacity due to structural constraints hindering optimization of charge-transfer complexes (CTC), high glass-transition temperature (Tg), and dielectric constant (εr).
  • This limitation restricts their application in high-temperature and harsh environments.

Purpose of the Study:

  • To develop intrinsically modified PI dielectrics with enhanced energy-storage capacity for high-temperature applications.
  • To achieve synergistic optimization of CTC suppression, Tg, and εr through chemical modification.

Main Methods:

  • Constructed intrinsic PI dielectrics with restricted dihedral-rotation structure using ─Cl, ─CH3, and ─CF3 substituents.
  • Investigated the effect of these substituents on molecular chain rigidity, CTC formation, Tg, and εr.
  • Fabricated and tested high-temperature-resistant stacked-film capacitor devices.

Main Results:

  • Restricted dihedral-rotation structure maintained high Tg and prevented film failure from internal stress.
  • Highly electronegative substituents and restricted structure synergistically suppressed CTC, enhancing breakdown strength (Eb).
  • The ─Cl substituent compensated for εr reduction, leading to outstanding discharged energy density (Ud) of 11.47 J/cm3 @150°C and 9.46 J/cm3 @200°C.
  • Fabricated devices showed excellent capacitance stability and power density.

Conclusions:

  • Chemical modification strategy effectively achieved synergistic optimization of CTC suppression, Tg, and εr in PI dielectrics.
  • This approach provides valuable guidance for developing scalable, high-performance polymer capacitors for demanding applications.