π‐Conjugated Microporous Hydrocarbon Electrodes for High‐Capacity and High‐Voltage Lithium‐Ion Capacitors

C Chenyu Wei (State Key Laboratory of Metal Matrix Composites,School of Materials Science and Engineering, Zhangjiang Institute for Advanced Study (ZIAS) Shanghai Jiao Tong University Shanghai 200240 P.R. China) S Shicong Zhang (State Key Laboratory of Metal Matrix Composites,School of Materials Science and Engineering, Zhangjiang Institute for Advanced Study (ZIAS) Shanghai Jiao Tong University Shanghai 200240 P.R. China) M Mei Xu Y Yang Xu T Tao Li Y Yi Shen (College of Chemistry, Chemical Engineering and Materials Science, and State Key Laboratory of Radiation Medicine and Protection) J Jinghua Cai (State Key Laboratory of Metal Matrix Composites,School of Materials Science and Engineering, Zhangjiang Institute for Advanced Study (ZIAS) Shanghai Jiao Tong University Shanghai 200240 P.R. China) X Xinji Dong (State Key Laboratory of Metal Matrix Composites,School of Materials Science and Engineering, Zhangjiang Institute for Advanced Study (ZIAS) Shanghai Jiao Tong University Shanghai 200240 P.R. China) H Hexian Ma (State Key Laboratory of Metal Matrix Composites,School of Materials Science and Engineering, Zhangjiang Institute for Advanced Study (ZIAS) Shanghai Jiao Tong University Shanghai 200240 P.R. China) T Tao Zhang F Fengtao Yu (National Key Laboratory of Uranium Resources Exploration‐Mining and Nuclear Remote Sensing East China University of Technology Nanchang 330013 China) F Fuqiang Huang (Key Laboratory of Intelligent Creation for Extreme Energy Materials of Ministry of Education, School of Materials Science and Engineering and Zhang Jiang Institute for Advanced Study) T Tianquan Lin (State Key Laboratory of Metal Matrix Composites,School of Materials Science and Engineering, Zhangjiang Institute for Advanced Study (ZIAS) Shanghai Jiao Tong University Shanghai 200240 P.R. China)

Abstract

AbstractCarbon‐based cathodes are widely utilized in lithium‐ion capacitors due to their superior cycle stability, safety, and tolerance to overcharging compared to oxide‐based cathodes. However, the limited capacity of carbon cathodes, primarily governed by the electric double‐layer capacitance mechanism, constrains their energy storage potential. Conventional strategies like increasing surface area and pore volume have provided marginal improvements, while heteroatom doping has been restricted by low working voltage and compromised conductivity. To overcome these limitations, a novel class of π‐conjugated microporous hydrocarbons (CMHs) is developed using sub‐graphitic polycyclic aromatic hydrocarbons (PAH) as building blocks. These materials PPe, PPy, and PAn feature carbon‐like large π‐conjugated surfaces, abundant oxygen‐free edge C(sp2)–H sites, and well‐defined microporous structures, facilitating anion adsorption and ion transport. Among them, PPe demonstrates exceptional performance with a high voltage of 3.13 V vs Li+/Li, a remarkable capacity of 241 mAh g−1 2.5 times of commercial activated carbon (YP50), and exceptional rate performance (up to 50 A g−1), far surpassing all other reported LIC cathode materials. These findings provide a fundamental design strategy for carbon‐based cathodes in LICs that highlighting the role of π‐conjugation and edge chemistry in electrochemical performance, paving the way for next‐generation high‐capacity, high‐voltage energy storage devices.

Article Details

Volume / Issue Vol. 37, Issue 30
Published July 01, 2025
ISSN 0935-9648
Publisher Unknown Publisher

Journal Info

Advanced Materials

Unknown Publisher

ISSN: 0935-9648 Physical Sciences

Authors (13)

C

Chenyu Wei

State Key Laboratory of Metal Matrix Composites,School of Materials Science and Engineering, Zhangjiang Institute for Advanced Study (ZIAS) Shanghai Jiao Tong University Shanghai 200240 P.R. China

S

Shicong Zhang

State Key Laboratory of Metal Matrix Composites,School of Materials Science and Engineering, Zhangjiang Institute for Advanced Study (ZIAS) Shanghai Jiao Tong University Shanghai 200240 P.R. China

M

Mei Xu

Y

Yang Xu

T

Tao Li

Y

Yi Shen

College of Chemistry, Chemical Engineering and Materials Science, and State Key Laboratory of Radiation Medicine and Protection

J

Jinghua Cai

State Key Laboratory of Metal Matrix Composites,School of Materials Science and Engineering, Zhangjiang Institute for Advanced Study (ZIAS) Shanghai Jiao Tong University Shanghai 200240 P.R. China

X

Xinji Dong

State Key Laboratory of Metal Matrix Composites,School of Materials Science and Engineering, Zhangjiang Institute for Advanced Study (ZIAS) Shanghai Jiao Tong University Shanghai 200240 P.R. China

H

Hexian Ma

State Key Laboratory of Metal Matrix Composites,School of Materials Science and Engineering, Zhangjiang Institute for Advanced Study (ZIAS) Shanghai Jiao Tong University Shanghai 200240 P.R. China

T

Tao Zhang

F

Fengtao Yu

National Key Laboratory of Uranium Resources Exploration‐Mining and Nuclear Remote Sensing East China University of Technology Nanchang 330013 China

F

Fuqiang Huang

Key Laboratory of Intelligent Creation for Extreme Energy Materials of Ministry of Education, School of Materials Science and Engineering and Zhang Jiang Institute for Advanced Study

T

Tianquan Lin

State Key Laboratory of Metal Matrix Composites,School of Materials Science and Engineering, Zhangjiang Institute for Advanced Study (ZIAS) Shanghai Jiao Tong University Shanghai 200240 P.R. China