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<p>Flexible dielectrics are urgently needed in advanced electrical systems and modern power electronics. Nevertheless, conventional polymer dielectrics suffer from low discharged energy density and charge-discharge efficiency at elevated temperatures due to severe conduction loss. Here, we report a perpendicular gradient structured polymer composite dielectric with an inorganic hybrid crosslinking network of Si-O-Ti. Driven by surface energy difference, SiO<sub>2</sub> accumulates on the film surface to block the charge injection, while bulk TiO<sub>2</sub> boosts the dielectric constant. The hybrid crosslinking network of Si-O-Ti also enhances the thermal stability, mechanical modulus and insulation strength by reducing free volume. Ultimately, the obtained composite delivers a discharged energy density of 6.04 J/cm<sup>3</sup> above 90% efficiency at 200 °C, exhibiting a 364.62% enhancement over the pristine polymer. This strategy effectively modulates surface and bulk properties, accordingly contributing to improving high-temperature capacitive energy storage performance.</p>

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Surface energy-driven perpendicular gradient structure in flexible composite dielectrics for high-temperature capacitive energy storage

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年6月25日

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  • Minhao Yang,
  • Huarui Yan,
  • Shiang Zhao,
  • Yanlong Zhao,
  • Haoran Sun,
  • Zhongjun Zhou,
  • Jiajun Qu,
  • Zhenyu Jia,
  • Zhenzhong Yang,
  • Jun Liu,
  • Bobo Tian,
  • Zhi-Min Dang

摘要

Flexible dielectrics are urgently needed in advanced electrical systems and modern power electronics. Nevertheless, conventional polymer dielectrics suffer from low discharged energy density and charge-discharge efficiency at elevated temperatures due to severe conduction loss. Here, we report a perpendicular gradient structured polymer composite dielectric with an inorganic hybrid crosslinking network of Si-O-Ti. Driven by surface energy difference, SiO2 accumulates on the film surface to block the charge injection, while bulk TiO2 boosts the dielectric constant. The hybrid crosslinking network of Si-O-Ti also enhances the thermal stability, mechanical modulus and insulation strength by reducing free volume. Ultimately, the obtained composite delivers a discharged energy density of 6.04 J/cm3 above 90% efficiency at 200 °C, exhibiting a 364.62% enhancement over the pristine polymer. This strategy effectively modulates surface and bulk properties, accordingly contributing to improving high-temperature capacitive energy storage performance.