Achieving High Energy Density at 200 °C in All-organic Polyimide Dielectrics Enabled by an Ultra-low Loading Multifunctional Porphyrin Crosslinker

Nan Hai; Peng Wu; Kang-Yan Chen; Qiang-Qiang Hai; Hong-Qiang Xia; Jun Zhang; Jie Mao

doi:10.1007/s10118-026-3706-6

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Achieving High Energy Density at 200 °C in All-organic Polyimide Dielectrics Enabled by an Ultra-low Loading Multifunctional Porphyrin Crosslinker

RESEARCH ARTICLE | Updated：2026-09-23

- Achieving High Energy Density at 200 °C in All-organic Polyimide Dielectrics Enabled by an Ultra-low Loading Multifunctional Porphyrin Crosslinker
- Chinese Journal of Polymer Science Vol. 44, Issue 10, Pages: 3610-3620(2026)
- Affiliations：
  
  School of Chemistry and Chemical Engineering, Ningxia University, Yinchuan 750021, China
- Author bio：
  
  ws1003m@163.com (J.Z.)
  maojie@nxu.edu.cn (J.M.)
- Funds：
- DOI：10.1007/s10118-026-3706-6
  CLC：
- Received：12 March 2026，
  
  Revised：2026-04-02，
  
  Accepted：07 April 2026，
  
  Online First：09 July 2026，
  
  Published：05 October 2026
- Accepted：
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Hai, N.; Wu, P.; Chen, K. Y.; Hai, Q. Q.; Xia, H. Q.; Zhang, J.; Mao, J. Achieving high energy density at 200 °C in all-organic polyimide dielectrics enabled by an ultra-low loading multifunctional porphyrin crosslinker. Chinese J. Polym. Sci. 2026, 44, 3610–3620

Nan Hai, Peng Wu, Kang-Yan Chen, et al. Achieving High Energy Density at 200 °C in All-organic Polyimide Dielectrics Enabled by an Ultra-low Loading Multifunctional Porphyrin Crosslinker[J]. Chinese Journal of Polymer Science, 2026, 44(10): 3610-3620.
Hai, N.; Wu, P.; Chen, K. Y.; Hai, Q. Q.; Xia, H. Q.; Zhang, J.; Mao, J. Achieving high energy density at 200 °C in all-organic polyimide dielectrics enabled by an ultra-low loading multifunctional porphyrin crosslinker. Chinese J. Polym. Sci. 2026, 44, 3610–3620 DOI： 10.1007/s10118-026-3706-6.

Nan Hai, Peng Wu, Kang-Yan Chen, et al. Achieving High Energy Density at 200 °C in All-organic Polyimide Dielectrics Enabled by an Ultra-low Loading Multifunctional Porphyrin Crosslinker[J]. Chinese Journal of Polymer Science, 2026, 44(10): 3610-3620. DOI： 10.1007/s10118-026-3706-6.

摘要

Ultra-low-loading 5

20-tetra(4-aminophenyl) porphyrin (TAPP) crosslinks polyimide (PI) and provides deep traps

boosting 200 °C energy density with high efficiency.

Abstract

High-temperature polymer dielectrics are critically needed for advanced power electronics; however

their performance is often compromised by charge-transfer complexes (CTC) in aromatic polyimides. To overcome this limitation

we introduced an ultra-low loading of 5

20-tetra(4-aminophenyl) porphyrin (TAPP) as

a multifunctional crosslinker into a polyimide (PI) matrix. TAPP simultaneously establishes covalent crosslinking and trap engineering

and its amino groups form a robust network with PI chains

whereas the porphyrin cycle acts as an efficient deep-level charge trap

effectively suppressing CTC formation and charge migration. The optimized PCPI films exhibited a tunable non-monotonic dielectric constant while maintaining a low loss. The PCPI-0.1 sample shows a significantly enhanced breakdown strength and achieves high discharge energy densities of 8.78

6.09

and 4.97 J·cm

−3

at 25

150

200 °C

respectively

while maintaining an efficiency above 85%. Remarkably

PCPI-0.1 delivered superior energy density compared to most high-temperature polymer dielectrics reported in the literature

coupled with excellent cycling stability and aging resistance. This work presents a strategy based on ultra-low-loading crosslinking that integrates structural modulation with deep-trap engineering

offering a viable pathway to high-performance all-organic dielectrics for extreme-condition applications.

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references

Feng, Q. K.; Zhong, S. L.; Pei, J. Y.; Zhao, Y.; Zhang, D. L.; Liu, D. F.; Dang, Z. M. Recent progress and future pros pects on all-organic polymer dielectrics for energy storage capacitors. Chem. Rev. 2022 , 122 , 3820−3878..

Zhang, X.; Jiang, J.; Shen, Z.; Dan, Z.; Li, M.; Lin, Y.; Shen, Y. Polymer nanocomposites with ultrahigh energy density and high discharge efficiency by modulating their nanostructures in three dimensions. Adv. Mater. 2018 , 30 , 1707269..

Li, L.; Cheng, J.; Cheng, Y.; Han, T.; Liu, Y.; Zhou, Y.; Wang, Q. Significant improvements in dielectric constant and energy density of ferroelectric polymer nanocomposites enabled by ultralow contents of nanofillers. Adv Mater. 2021 , 33 , 2102392..

Liu, X. J.; Zheng, M. S.; Chen, G.; Dang, Z. M.; Zha, J. W. High-temperature polyimide dielectric materials for energy storage: theory, design, preparation and properties. Energ. Environ. Sci. 2022 , 15 , 56−81..

Dong, J.; Li, L.; Niu, Y.; Pan, Z.; Pan, Y.; Sun, L.; Wang, H. Scalable high-permittivity polyimide copolymer with ultrahigh high-temperature capacitive performance enabled by molecular engineering. Adv. Energy. Mater. 2024 , 14 , 2303732..

[H. Li, Y. Zhou, Y. Liu, L. Li, Y. Liu, Q. Wang, CHEM SOC REV 2021 , 50 , 6369. Li, H.; Zhou, Y.; Liu, Y.; Li, L.; Liu, Y.; Wang, Q. Dielectric polymers for high-temperature capacitive energy storage. Chem. Soc. Rev. 2021 , 50 , 6369−6400..

Zha, J. W.; Xiao, M.; Wan, B.; Wang, X.; Dang, Z. M.; Chen, G. Polymer dielectrics for high-temperature energy storage: constructing carrier traps. Prog. Mater. Sci. 2023 , 140 , 101208..

Hasegawa, M.; Horie, K. Photophysics, photochemistry, and optical properties of polyimides. Prog. Polym. Sci. 2001 , 26 , 259−335..

Zhuang, Y.; Seong, J. G.; Lee, Y. M. Polyimides containing aliphatic/alicyclic segments in the main chains. Prog. Polym. Sci. 2019 , 92 , 35−88..

[Zhou, L.; Zhao, S.; Xie, P.; Miao, X.; Liu, S.; Sun, N.; Shen, Y. Research progress and prospect of polymer dielectrics. Appl. Phys. Rev . 2023 , 10 , 031310..

Li, L.; Dong, J.; Hu, R.; Chen, X.; Niu, Y.; Wang, H. Wide-bandgap fluorides/polyimide composites with enhanced energy storage properties at high temperatures. Chem. Eng. J. 2022 , 435 , 135059..

Yuan, C.; Zhou, Y.; Zhu, Y.; Liang, J.; Wang, S.; Peng, S.; Li, Q. Polymer/molecular semiconductor all-organic composites for high-temperature dielectric energy storage. Nat. Commun. 2020 , 11 , 3919..

Li, H.; Yang, T.; Zhou, Y.; Ai, D.; Yao, B.; Liu, Y.; Wang, Q. Enabling high-energy-density high-efficiency ferroelectric polymer nanocomposites with rationally designed nanofillers. Adv. Funct. Mater. 2021 , 31 , 2006739..

Ai, D.; Li, H.; Zhou, Y.; Ren, L.; Han, Z.; Yao, B.; Wang, Q. Tuning nanofillers in situ prepared polyimide nanocomposites for high-temperature capacitive energy storage. Adv. Energy. Mater. 2020 , 10 , 1903881..

Sun, B.; Hu, P.; Ji, X.; Fan, M.; Zhou, L.;Guo, M.; Shen, Y. Excellent stability in polyetherimide/SiO2 nanocomposites with ultrahigh energy density and discharge efficiency at high temperature. Small 2022 , 18 , 2202421..

Xiang, D.; Wang, X.; Jia, C.; Lee, T.; Guo, X. Molecular-scale electronics: from concept to function. Chem. Rev. 2016 , 116 , 4318−4440..

Wang, Q.; Wang, T.; Chi, H.; Zhao, D.; Yu, L.; Jiang, Z.; Zhang, Y. Scalable all-organic polymer dielectrics for high-temperature film capacitors with construction of deep-trap level and cross-linking network. Chem. Eng. J. 2025 , 506 , 160204..

Zhou, Y.; Zhang, Z.; Tang, Q.; Ma, X.; Hou, X. Enhancing the high-temperature energy storage properties of PEI dielectrics by constructing trap-rich covalently cross-linked networks via POSS-functionalized BNNS. Mater. Horiz. 2024 , 11 , 4348−4358..

Meng, Z.; Zhang, T.; Zhang, C.; Shang, Y.; Lei, Q.; Chi, Q. Advances in polymer dielectrics with high energy storage performance by designing electric charge trap structures. Adv. Mater. 2024 , 36 , 2310272..

Wu, C.; Deshmukh, A. A.; Li, Z.; Chen, L.; Alamri, A.; Wang, Y.; Cao, Y. Flexible temperature-invariant polymer dielectrics with large bandgap. Adv. Mater. 2020 , 32 , 2000499..

Sharma, V.; Wang, C.; Lorenzini, R. G.; Ma, R.; Zhu, Q.; Sinkovits, D. W.; Kumar, S. G Sotzing, GA; Boggs, SA; Ramprasad, R. Nat. Commun. 2014 , 5 , 4845..

[Sun, Y.; Boggs, S. A.; Ramprasad, R. The intrinsic electrical breakdown strength of insulators from first principles. Appl. Phys. Lett. 2012 , 101 ..

Yu, S.; Zhou, J.; Xu, A.; Lao, J.; Luo, H.; Chen, S. The scalable and high performance polyimide dielectrics containing alicyclic structures for high-temperature capacitive energy storage. Chem. Eng. J. 2023 , 469 , 143803..

Cheng, Y.; Zhang, X.; Qin, Y.; Dong, P.; Yao, W.; Matz, J.; Ye, M. Super-elasticity at 4 K of covalently crosslinked polyimide aerogels with negative Poisson’s ratio. Nat. Commun. 2021 , 12 , 4092..

Landi Jr, S.; Segundo, I. R.; Freitas, E.; Vasilevskiy, M.; Carneiro, J.; Tavares, C. J. Use and misuse of the Kubelka-Munk function to obtain the band gap energy from diffuse reflectance measurements. Solid. State. Commun. 2022 , 341 , 114573..

Pan, Y.; Guo, Y.; Liu, J.; Zhu, H.; Chen, G.; Liu, Q.; Jin, W. PDMS with tunable side group mobility and its highly permeable membrane for removal of aromatic compounds. Angew. Chem. Int. Edit. 2022 , 61 , e202111810..

Ambegaokar, V.; Halperin, B. I.; Langer, J. S. Hopping conductivity in disordered systems. Phys. Rev. B 1971 , 4 , 2612..

Chiu, F. C. A review on conduction mechanisms in dielectric films. Adv. Mater. Sci. Eng. 2014 , 2014 , 578168..

Tian, F.; Bu, W.; Shi, L.; Yang, C.; Wang, Y.; Lei, Q. Theory of modified thermally stimulated current and direct determination of trap level distribution. J. Electrostat. 2011 , 69 , 7−10..

Wu, Y.; He, Y.; Zhou, T.; Chen, C.; Zhong, F.; Xia, Y.; Zhang, C. Synergistic functionalization of h-BN by mechanical exfoliation and PEI chemical modification for enhancing the corrosion resistance of waterborne epoxy coating. Prog. Org. Coat. 2020 , 142 , 105541..

Dong, X.; Wang, Y.; Cao, Y.; Li, N.; Fu, J.; Yu, J.; Hu, Z. Enhanced high-temperature energy storage performance in all-organic dielectric films through synergistic crosslinking of chemical and physical interaction. Chem. Eng. J. 2024 , 500 , 157312..

Wei, Y.; Yang, L.; Wang, C.; Zhu, Z.; Dai, Y.; Qin, H.; Xiong, C. Enhanced high-temperature capacitive energy storage in polyetherimide dielectrics through dense crosslinked network structures. Chem. Eng. J. 2025 , 507 , 160793..

Dhanumalayan, E.; Joshi, G. M. Performance properties and applications of polytetrafluoroethylene (PTFE)-a review. Adv. Compos. Hybrid. Ma. 2018 , 1 , 247−268..

Niu, Y.; Dong, J.; He, Y.; Xu, X.; Li, S.; Wu, K.; Wang, H. Significantly enhancing the discharge efficiency of sandwich-structured polymer dielectrics at elevated temperature by building carrier blocking interface. Nano. Energy. 2022 , 97 , 107215..

Deshmukh, A. A.; Wu, C.; Yassin, O.; Mishra, A.; Chen, L.; Alamri, A.; Sotzing, G. Flexible polyolefin dielectric by strategic design of organic modules for harsh condition electrification. Energ. Environ. Sci. 2022 , 15 , 130−1314..

Qin, S.; Song, J.; Qin, H.; Fu, Y.; Liu, M.; Yu, S.; Wang, S. Fluorinated aromatic polyimide with large bandgap exhibiting superior capacitive performance at elevated temperatures. J. Energy. Storage. 2024 , 87 , 111458..

Zhou, S.; Zhao, H.; Zhang, N.; Yin, L.; Bai, J. Improved high-temperature energy storage performance of sandwich PEI-based composites via introducing charge traps by differential functional fillers. Chem. Eng. J. 2025 , 504 , 158941..

Dong, J.; Li, L.; Qiu, P.; Pan, Y.; Niu, Y.; Sun, L.; Wang, H. Scalable polyimide-organosilicate hybrid films for high-temperature capacitive energy storage. Adv. Mater. 2023 , 35 , 2211487..

[Baghban, A.; Ezedin Nejadian, H.; Habibzadeh S.; Zokaee Ashtiani F.; Sci. Rep-UK. 2022 , 12 , 19428..

Choi, H.; An, J.; Lee, K.; Kwon, K. Y. Polyethyleneimine incorporated hydroxyapatite for improved colloidal stability. Bull. Korean. Chem. Soc. 2024 , 45 , 614−619..

Li, X.; Luo, H.; Zhai, D.; Wan, Y.; He, G.; Hu, D.; Zhang, S. Enhanced capacitive energy storage of polyetherimide at high temperatures by integration of electrical insulation and thermal conductivity. Adv. Powder Mater. 2025 , 4 , 100286..

Yang, M.; Li, H.; Wang, J.; Shi, W.; Zhang, Q.; Xing, H.; Shen, Y. Roll-to-roll fabricated polymer composites filled with subnanosheets exhibiting high energy density and cyclic stability at 200° C. Nat. Energy. 2024 , 9 , 143−153..

Zhao, S.; Peng, W.; Zhou, L.; Dai, S.; Ren, W.; Xu, E.; Nan, C. W. Metal-organic cage crosslinked nanocomposites with enhanced high-temperature capacitive energy storage performance. Nat. Commun. 2025 , 16 , 769..

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