<p>Polymer composite dielectrics are key materials for high-temperature film capacitors, yet their energy storage capability is severely constrained at elevated temperatures. Molecular fillers that simultaneously integrate deep-level trapping (high electron affinity, <i>E</i><sub>a</sub>), strong insulation (large bandgap, <i>E</i><sub>g</sub>), and high thermal stability are rarely available, posing a major challenge for improving high-temperature energy storage performance. To address this challenge, here we screen and identify hexaazatriphenylene hexacarbonitrile (HAT-CN) as a promising candidate that fulfills the above critical requirements from numerous commercial organic molecules. When incorporated into a high glass transition temperature (<i>T</i><sub>g</sub>) polymer fluorene polyester (FPE), the resulting all-organic composite exhibits simultaneously suppressed high-temperature conduction loss and preserved mechanical robustness. Consequently, the optimized composite achieves record-high discharged energy densities of 7.31 J cm<sup>−3</sup> at 150 °C and 6.14 J cm<sup>−3</sup> at 200 °C (<i>η</i>⩾90%) with a low cost and scalable process. This work demonstrates that the filler design based on synergistic key properties provides a potent pathway to break the longstanding high-temperature performance bottleneck in polymer dielectrics.</p>

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Integrated molecular engineering strategy in all-organic dielectrics for ultrahigh-temperature capacitive energy storage

  • Yuanqi Wang,
  • Hangyao Wu,
  • Lan Chen,
  • Sinan Lin,
  • Chenyi Li,
  • Yun Zhang,
  • Yang Li,
  • Huamin Zhou,
  • Yang Liu

摘要

Polymer composite dielectrics are key materials for high-temperature film capacitors, yet their energy storage capability is severely constrained at elevated temperatures. Molecular fillers that simultaneously integrate deep-level trapping (high electron affinity, Ea), strong insulation (large bandgap, Eg), and high thermal stability are rarely available, posing a major challenge for improving high-temperature energy storage performance. To address this challenge, here we screen and identify hexaazatriphenylene hexacarbonitrile (HAT-CN) as a promising candidate that fulfills the above critical requirements from numerous commercial organic molecules. When incorporated into a high glass transition temperature (Tg) polymer fluorene polyester (FPE), the resulting all-organic composite exhibits simultaneously suppressed high-temperature conduction loss and preserved mechanical robustness. Consequently, the optimized composite achieves record-high discharged energy densities of 7.31 J cm−3 at 150 °C and 6.14 J cm−3 at 200 °C (η⩾90%) with a low cost and scalable process. This work demonstrates that the filler design based on synergistic key properties provides a potent pathway to break the longstanding high-temperature performance bottleneck in polymer dielectrics.