Semi-alicyclic fluorinated polyimide with ultrahigh energy density enabled by bandgap-topology co-engineering

Semi-alicyclic fluorinated polyimide with ultrahigh energy density enabled by bandgap-topology co-engineering

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Shuoyan Liu^a^,^b, Jiufeng Dong^a^,^b^,^*, Liang Sun^a^,^b, Zizhao Pan^a^,^b, Yujuan Niu^a^,^b, Yani Lu^a^,^b, Yuqi Liu^a^,^b, Hong Wang^a^,^b^,^**

Journal of Materiomics | 2026, 12(2) : 101151

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Journal of Materiomics | 2026, 12(2): 101151

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Semi-alicyclic fluorinated polyimide with ultrahigh energy density enabled by bandgap-topology co-engineering

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Shuoyan Liu^a^,^b, Jiufeng Dong^a^,^b^,^*, Liang Sun^a^,^b, Zizhao Pan^a^,^b, Yujuan Niu^a^,^b, Yani Lu^a^,^b, Yuqi Liu^a^,^b, Hong Wang^a^,^b^,^**

Affiliations

^aState Key Laboratory of Quantum Functional Materials, Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, 518055, Guangdong, China

^bGuangdong Provincial Key Laboratory of Functional Oxide Materials and Devices & Shenzhen Engineering Research Center for Novel Electronic Information Materials and Devices, Southern University of Science and Technology, Shenzhen, 518055, Guangdong, China

Published: 2026-03-20 doi: 10.1016/j.jmat.2025.101151

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Abstract

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Aromatic polyimide (PI) with high glass transition temperature (T_g) shows promise as a polymer dielectric for energy storage, but its rigid aromatic structure and electron delocalization cause significant conduction loss, degrading energy storage performance and breakdown strength (E_b) under high temperatures. Herein, we introduce a novel semi-alicyclic fluorinated polyimide (H-FPI) designed via a molecular engineering strategy that synergistically integrates bandgap and topological conformation modulation. Specifically, the alicyclic group elevates the lowest unoccupied molecular orbital (LUMO) while strong electron-withdrawing trifluoromethyl (-CF₃) substitution depresses the highest occupied molecular orbital (HOMO), creating a wide bandgap (4.2 eV). Concurrently, the chair-conformation alicyclic backbone and sterically bulky -CF₃ groups synergistically disrupt molecular planarity, reducing π-orbital overlap to suppress charge transfer while restricting chain mobility to yield a high T_g of 272 ℃. Remarkably, H-FPI film delivers a high energy density of 6.02 J/cm³ with a superior breakdown strength of 626 MV/m at 200 ℃, surpassing commercial PI and fluorinated polyimide (FPI) by 1261% and 55%, respectively. Furthermore, H-FPI film exhibits exceptional capacitor charge-discharge cyclability, enhanced mechanical robustness, and excellent thermal stability. This work establishes a new molecular design paradigm for organic capacitors in electrffied transportation and smart grid systems requiring high-temperature working reliability.

Key words

Polymer capacitors / High-temperature / Semi-alicyclic fluorinated polyimide / Bandgap / Topological conformation

Cite this Article

Shuoyan Liu, Jiufeng Dong, Liang Sun, Zizhao Pan, Yujuan Niu, Yani Lu, Yuqi Liu, Hong Wang. Semi-alicyclic fluorinated polyimide with ultrahigh energy density enabled by bandgap-topology co-engineering[J]. Journal of Materiomics, 2026 , 12 (2) : 101151 - . DOI: 10.1016/j.jmat.2025.101151

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Funding

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National Natural Science Foundation of China(52361165625; 52407023)

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Year 2026 volume 12 Issue 2

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Article Info

doi: 10.1016/j.jmat.2025.101151

Receive Date：2025-07-27
Online Date：2026-08-13
Published：2026-03-20

Article Data

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History

Received：2025-07-27
Revised：2025-10-08
Accepted：2025-10-15

Funding

National Natural Science Foundation of China(52361165625; 52407023)

Affiliations

^aState Key Laboratory of Quantum Functional Materials, Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, 518055, Guangdong, China

Corresponding:

^* Southern University of Science and Technology, No. 1088 Xueyuan Avenue, Nanshan District, Shenzhen, 518055, China. E-mail addresses: dongjf@mail.sustech.edu.cn (J. Dong)

^** Southern University of Science and Technology, No. 1088 Xueyuan Avenue, Nanshan District, Shenzhen, 518055, China. wangh6@sustech.edu.cn (H. Wang).

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表12种不同金属材料的力学参数

科 Family	属数 Number of genus	种数 Number of species	占总种数比例 Percentage of total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
鹅膏菌科Amanitaceae	2	11	5.26	鹅膏菌属 Amanita	10	4.78
小菇科 Mycenaceae	2	12	5.74	丝盖伞属 Inocybe	5	2.39
多孔菌科 Polyporaceae	8	14	6.70	蜡蘑属 Laccaria	5	2.39
红菇科 Russulaceae	3	23	11.00	小皮伞属 Marasmius	6	2.87
				小菇属 Mycena	11	5.26
				光柄菇属 Pluteus	5	2.39
				红菇属 Russula	17	8.13
				栓菌属 Trametes	5	2.39

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