A Dipole‐Confined Charge Transport Paradigm for Ultrahigh‐Temperature Dielectric Polymers
Abstract
ABSTRACT A pervasive challenge in materials science, the incompatible trade‐off among breakdown strength ( E b ), thermal stability ( T g ), and dielectric constant ( ε r ), has limited the development of polymer dielectrics for extreme‐environment film capacitors. Here, this trilemma is overcome via a dipole‐regulation strategy, confining polar methyl‐sulfonyl groups within a rigid semi‐aromatic polyimide framework using flexible methylene linkers. This dipole confinement domain structure of sulfonyl‐methylene‐benzene decouples dipolar response from charge transport: the flexible linkers enable polarization, while the rigid semi‐aromatic framework localizes charges and suppresses conduction. It results in a stable dipole network, yielding a material (STPCB‐PI) with a wide bandgap (4.38 eV) and a record T g (>400°C). It achieves a high ε r of 5.8, a modulus of 6.7 GPa, and exceptional energy storage, delivering 12.00 J cm −3 with 97% efficiency at 25°C, 9.98 J cm −3 with 94% efficiency at 150°C, and retaining 8.62 J cm −3 with 90% efficiency at 200°C, 293% improvement over the state‐of‐the‐art commercial polyetherimide. Even at 250°C, it maintains 4.24 J cm −3 with 93% efficiency. It also exhibits excellent self‐healing and cyclic endurance. This work sets a new performance benchmark and establishes a generalizable design paradigm that reconciles the intrinsic conflict between polarization and insulation in high‐temperature dielectric polymers.
Article Details
Authors (11)
Zunchu Liu
PCFM Lab, GD HPPC Lab, Guangdong Engineering Technology Research Centre For High‐Performance Organic and Polymer Photoelectric Functional Films, GBRCE For Functional Molecular Engineering, State Key Laboratory of Optoelectronic Materials and Technologies, School of Chemistry, IGCME Sun Yat‐Sen University Guangzhou China
Kaijin Chen
PCFM Lab, GD HPPC Lab, Guangdong Engineering Technology Research Centre For High‐Performance Organic and Polymer Photoelectric Functional Films, GBRCE For Functional Molecular Engineering, State Key Laboratory of Optoelectronic Materials and Technologies, School of Chemistry, IGCME Sun Yat‐Sen University Guangzhou China
Xueyi Yu
PCFM Lab, GD HPPC Lab, Guangdong Engineering Technology Research Centre For High‐Performance Organic and Polymer Photoelectric Functional Films, GBRCE For Functional Molecular Engineering, State Key Laboratory of Optoelectronic Materials and Technologies, School of Chemistry, IGCME Sun Yat‐Sen University Guangzhou China
Jinkun Bian
PCFM Lab, GD HPPC Lab, Guangdong Engineering Technology Research Centre For High‐Performance Organic and Polymer Photoelectric Functional Films, GBRCE For Functional Molecular Engineering, State Key Laboratory of Optoelectronic Materials and Technologies, School of Chemistry, IGCME Sun Yat‐Sen University Guangzhou China
Weiwen Zheng
PCFM Lab, GD HPPC Lab, Guangdong Engineering Technology Research Centre For High‐Performance Organic and Polymer Photoelectric Functional Films, GBRCE For Functional Molecular Engineering, State Key Laboratory of Optoelectronic Materials and Technologies, School of Chemistry, IGCME Sun Yat‐Sen University Guangzhou China
Xueqi Zhao
Jilin Province Research Center for Engineering and Technology of Spectral Analytical Instruments, College of Chemistry, Jilin University
Zihao Huang
State Key Laboratory of Bioinspired Interfacial Materials Science, School of Chemistry
Runxin Bei
PCFM Lab, GD HPPC Lab, Guangdong Engineering Technology Research Centre For High‐Performance Organic and Polymer Photoelectric Functional Films, GBRCE For Functional Molecular Engineering, State Key Laboratory of Optoelectronic Materials and Technologies, School of Chemistry, IGCME Sun Yat‐Sen University Guangzhou China
Siwei Liu
Jiarui Xu
Yi Zhang