Scalable High‐Permittivity Polyimide Copolymer with Ultrahigh High‐Temperature Capacitive Performance Enabled by Molecular Engineering

Jiufeng,Dong1,2; Li,Li1,2; Yujuan,Niu1,2; Zizhao,Pan1,2; Yupeng,Pan3; Liang,Sun1,2; Li,Tan1,2; Yuqi,Liu1,2; Xinwei,Xu1,2; Xugang,Guo1,2; Qing,Wang4; Hong,Wang1,2

2023-12-31

10.1002/aenm.202303732

Advanced Energy Materials   影响因子和分区

1614-6832

1614-6840

["Polymer capacitors are essential components of advanced electronic and power systems. However, the deficient high-temperature capacitive performance of polymer dielectrics fails to meet the demand for harsh condition applications, due to the mutually restrictive relationships in permittivity (epsilon r), glass transition temperature (Tg), and bandgap (Eg). Here, a modularized molecular engineering strategy is reported to enhance the high-temperature capacitive performance of polymer dielectrics. First, the potential influences of multiple structural units on epsilon r, Tg, and Eg of polymers are elucidated by comparing a set of polyimides (PIs). After screening out an excellent sulfonated PI with concurrently high epsilon r (4.2), Eg (3.4 eV), and Tg (311.2 degrees C), a semi-alicyclic sulfonyl-containing PI copolymer is further synthesized that exhibits a superior discharged energy density of 4.3 J cm-3 above 90% efficiency at 200 degrees C and 485 MV m-1. Density functional theory calculations demonstrate that the combination of polar sulfonyl group, ether linkage, and alicyclic group in the backbones of the copolymer decouples the dipole orientation and the segmental motion of backbones, and reduces conjugation effects of aromatic groups, thereby minimizing the polarization relaxation loss and the conduction loss while retaining excellent thermal stability and high permittivity.","An original semi-alicyclic sulfonyl-containing polyimide copolymer that exhibits superior high-temperature capacitive performance, excellent charge-discharge stability, and ultrahigh power density is designed. The sulfonyl group, ether linkage, and alicyclic group in the backbones of the copolymer decouple the conjugation effects of the aromatic structure, while retaining excellent thermal stability, high permittivity, and wide bandgap.image"]

bandgap high temperature molecular engineering permittivity polymer capacitors

SCI ; EI

英语

第一 ; 共同第一 ; 通讯

National Natural Science Foundation of China[92066208] ; Shenzhen Science and Technology Program[KQTD20180411143514543] ; China Postdoctoral Science Foundation[2023M731498] ; Guangdong Provincial Key Laboratory Program[2021B1212040001] ; null[2021YFB3800603]

Chemistry ; Energy & Fuels ; Materials Science ; Physics

Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:001133235900001

Wiley

20240115313105

Density functional theory ; Dielectric materials ; Glass transition ; High temperature applications ; Permittivity ; Polyimides

Dielectric Materials:708.1 ; Chemical Operations:802.3 ; Organic Polymers:815.1.1 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

人工提交

1.Department of Materials Science and Engineering Southern University of Science and Technology Shenzhen, Guangdong 518055, China
2.Shenzhen Engineering ResearchCenter for Novel Electronic Information Materials andDevices&Guangdong Provincial Key Laboratory of Functional Oxide Materials andDevices Southern University of Science and Technology Shenzhen,Guangdong 518055, China
3.Shenzhen Grubbs Institute andDepartment ofChemistry Southern University of Science and Technology Shenzhen,Guangdong 518055, China
4.Department of Materials Science and Engineering The Pennsylvania StateUniversity University Park, PA 16802,USA

Jiufeng,Dong,Li,Li,Yujuan,Niu,等. Scalable High‐Permittivity Polyimide Copolymer with Ultrahigh High‐Temperature Capacitive Performance Enabled by Molecular Engineering[J]. Advanced Energy Materials,2023,14(9):2303732 (1 of 8).

Jiufeng,Dong.,Li,Li.,Yujuan,Niu.,Zizhao,Pan.,Yupeng,Pan.,...&Hong,Wang.(2023).Scalable High‐Permittivity Polyimide Copolymer with Ultrahigh High‐Temperature Capacitive Performance Enabled by Molecular Engineering.Advanced Energy Materials,14(9),2303732 (1 of 8).

Jiufeng,Dong,et al."Scalable High‐Permittivity Polyimide Copolymer with Ultrahigh High‐Temperature Capacitive Performance Enabled by Molecular Engineering".Advanced Energy Materials 14.9(2023):2303732 (1 of 8).