Volume 21, Issue 24 2412698
Research Article

Highly Crystalline and Robust Donor-Acceptor Type Covalent Organic Frameworks for Long-life Sodium-Ion Battery Cathodes

Kun Kang

Kun Kang

School of Materials Science and Engineering, Shaanxi Normal University, Xi'an, 710119 P. R. China

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Ying Liu

Ying Liu

College of Chemistry and Environmental Engineering, Anyang Institute of Technology, Anyang, 455000 P. R. China

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Jiaqi Duan

Jiaqi Duan

School of Materials Science and Engineering, Shaanxi Normal University, Xi'an, 710119 P. R. China

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Xue Tang

Xue Tang

School of Materials Science and Engineering, Shaanxi Normal University, Xi'an, 710119 P. R. China

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Yan Wang

Yan Wang

School of Materials Science and Engineering, Tongji University, Shanghai, 200092 P. R. China

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Shiqi Zhang

Shiqi Zhang

School of Mechanical Engineering, Nantong University, Nantong, 226019 P. R. China

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Heng Wang

Heng Wang

School of Mechanical Engineering, Nantong University, Nantong, 226019 P. R. China

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Jincan Cui

Jincan Cui

School of Mechanical Engineering, Nantong University, Nantong, 226019 P. R. China

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Xiaolei Yuan

Xiaolei Yuan

School of Mechanical Engineering, Nantong University, Nantong, 226019 P. R. China

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Xu Deng

Xu Deng

College of Chemistry and Environmental Engineering, Anyang Institute of Technology, Anyang, 455000 P. R. China

College of Chemistry and Chemical Engineering, Henan Polytechnic University, Jiaozuo, 454003 P. R. China

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Ning Fu

Corresponding Author

Ning Fu

College of Chemistry and Environmental Engineering, Anyang Institute of Technology, Anyang, 455000 P. R. China

College of Chemistry and Chemical Engineering, Henan Polytechnic University, Jiaozuo, 454003 P. R. China

E-mail: [email protected]; [email protected]; [email protected]

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Ben Yang

Corresponding Author

Ben Yang

School of Materials Science and Engineering, Shaanxi Normal University, Xi'an, 710119 P. R. China

E-mail: [email protected]; [email protected]; [email protected]

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Jian-Yong Hu

Corresponding Author

Jian-Yong Hu

School of Materials Science and Engineering, Shaanxi Normal University, Xi'an, 710119 P. R. China

E-mail: [email protected]; [email protected]; [email protected]

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First published: 25 April 2025

Abstract

Covalent organic frameworks (COFs) hold great potential in sodium-ion battery cathodes. However, most reported COF-based electrodes show unsatisfying capacity and rate performance due to their limited redox site density, low crystallinity, and poor conductivity. Herein, a highly crystalline and robust donor-acceptor type COF with abundant redox active sites is developed by the polymerization of donor unit benzo[1,2-b:3,4-b″:5,6-b″']trithiophene-2,5,8-tricarbaldehyde) (BTT) and acceptor unit s-indacene-1,3,5,7(2H,6H)-tetrone (ICTO) (denoted as BTT-ICTO) for cathodic Na+ storage. The BTT-ICTO-graphene composites (BTT-ICTO@G) synthesized by in situ growth have a loose sheet structure with rough surfaces, contributing to the improved conductivity and active site utilization of BTT-ICTO. Benefiting from the robustness of BTT-ICTO linked by ethylene bonds, the BTT-ICTO@G cathodes exhibit a high capacity of 325 mAh g−1 at 0.1 A g−1 with a high active site utilization of 80%, excellent rate performance of 190 mAh g−1 at 5.0 A g−1, and exceptional cycle performances of 196 mAh g−1 over 10 000 cycles at 2.0 A g−1 with only 0.0015% decay per cycle. These properties make the BTT-ICTO@G cathodes among the best-reported COF-based sodium-ion battery cathodes. In addition, in situ Raman, ex situ Fourier transform infrared, and theoretical calculations disclose the reaction pathway of Na+ storage.

Conflict of Interest

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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