Robust Imidazole‐Linked 2D Covalent Organic Frameworks for Efficient Electrochemical Sodium‐Ion Storage

Y Yuzhao Guo (State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry Jilin University Changchun China) L Linqi Cheng (Department of Chemistry, Rice University, 6100 Main Street, Houston, Texas 77005, United States) X Xupeng Zhang M Meiling Qi (State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry Jilin University Changchun 130012 China) Y Yabo Wei (School of Chemical and Environmental Engineering Shanghai Institute of Technology Shanghai 201418 China) S Sheng Han (Academy for Advanced Interdisciplinary Studies, Frontiers Science Center for New Organic Matter, State Key Laboratory and Institute of Elemento-Organic Chemistry, College of Chemistry, College of Outstanding Engineers) X Xi Su (State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry) H Heng‐Guo Wang (Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education and Faculty of Chemistry Northeast Normal University Changchun People's Republic of China) L Long Chen (Department of Chemistry, Frontiers Science Center for New Organic Matter and State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry)

Abstract

Abstract Exploring stable and functional linkages through facile one‐pot cyclocondensation reactions represents one of the frontiers in the development of covalent organic frameworks (COFs), which can enhance structural robustness and diversity while broadening their application potential. In this study, we report a facile synthetic strategy using p ‐toluenesulfonic acid (PTSA) as a proton mediator to construct two imidazole‐linked COFs (TABQ‐COF and TAPT‐COF) via one‐pot cyclocondensation of aromatic aldehydes with ortho ‐diamines. These two COFs not only possess good crystallinity but also exhibit excellent physicochemical stability and contain abundant redox‐active sites, which endows them with charming advantages for electrochemical energy storage. Remarkably, when employed as an anode material for sodium‐ion batteries (SIBs), TAPT‐COF delivered a reversible capacity of 517 mAh g −1 at 0.05 A g −1 while maintaining outstanding cycling stability with minimal capacity degradation (<0.035% per cycle) over 1000 cycles at 1.0 A g −1 . This superior performance stems from synergistic contributions of abundant redox‐active centers (C═O and C═N groups), which enable efficient Na + storage through multielectron redox mechanisms. This study highlights the strategic advantage of structurally stable COFs with precisely engineered redox‐active motifs via facile synthesis for advancing high‐performance electrochemical energy storage.

Article Details

Volume / Issue Vol. 64, Issue 36
Published September 01, 2025
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (9)

Y

Yuzhao Guo

State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry Jilin University Changchun China

L

Linqi Cheng

Department of Chemistry, Rice University, 6100 Main Street, Houston, Texas 77005, United States

X

Xupeng Zhang

M

Meiling Qi

State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry Jilin University Changchun 130012 China

Y

Yabo Wei

School of Chemical and Environmental Engineering Shanghai Institute of Technology Shanghai 201418 China

S

Sheng Han

Academy for Advanced Interdisciplinary Studies, Frontiers Science Center for New Organic Matter, State Key Laboratory and Institute of Elemento-Organic Chemistry, College of Chemistry, College of Outstanding Engineers

X

Xi Su

State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry

H

Heng‐Guo Wang

Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education and Faculty of Chemistry Northeast Normal University Changchun People's Republic of China

L

Long Chen

Department of Chemistry, Frontiers Science Center for New Organic Matter and State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry