Robust Imidazole-Linked 2D Covalent Organic Frameworks for Efficient Electrochemical Sodium-Ion Storage
Yuzhao Guo
State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun, 130012 China
Both authors contributed equally to this work.
Search for more papers by this authorProf. Linqi Cheng
Key Laboratory of polyoxometalate and Reticular Material Chemistry of Ministry of Education and Faculty of Chemistry, Northeast Normal University, Changchun, 130024 China
Both authors contributed equally to this work.
Search for more papers by this authorXupeng Zhang
Key Laboratory of polyoxometalate and Reticular Material Chemistry of Ministry of Education and Faculty of Chemistry, Northeast Normal University, Changchun, 130024 China
Search for more papers by this authorMeiling Qi
State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun, 130012 China
Search for more papers by this authorYabo Wei
School of Chemical and Environmental Engineering, Shanghai Institute of Technology, Shanghai, 201418 China
Search for more papers by this authorCorresponding Author
Prof. Sheng Han
School of Chemical and Environmental Engineering, Shanghai Institute of Technology, Shanghai, 201418 China
E-mail: [email protected]; [email protected]; [email protected]
Search for more papers by this authorXi Su
State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun, 130012 China
Search for more papers by this authorCorresponding Author
Prof. Heng-Guo Wang
Key Laboratory of polyoxometalate and Reticular Material Chemistry of Ministry of Education and Faculty of Chemistry, Northeast Normal University, Changchun, 130024 China
E-mail: [email protected]; [email protected]; [email protected]
Search for more papers by this authorCorresponding Author
Long Chen
State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun, 130012 China
E-mail: [email protected]; [email protected]; [email protected]
Search for more papers by this authorYuzhao Guo
State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun, 130012 China
Both authors contributed equally to this work.
Search for more papers by this authorProf. Linqi Cheng
Key Laboratory of polyoxometalate and Reticular Material Chemistry of Ministry of Education and Faculty of Chemistry, Northeast Normal University, Changchun, 130024 China
Both authors contributed equally to this work.
Search for more papers by this authorXupeng Zhang
Key Laboratory of polyoxometalate and Reticular Material Chemistry of Ministry of Education and Faculty of Chemistry, Northeast Normal University, Changchun, 130024 China
Search for more papers by this authorMeiling Qi
State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun, 130012 China
Search for more papers by this authorYabo Wei
School of Chemical and Environmental Engineering, Shanghai Institute of Technology, Shanghai, 201418 China
Search for more papers by this authorCorresponding Author
Prof. Sheng Han
School of Chemical and Environmental Engineering, Shanghai Institute of Technology, Shanghai, 201418 China
E-mail: [email protected]; [email protected]; [email protected]
Search for more papers by this authorXi Su
State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun, 130012 China
Search for more papers by this authorCorresponding Author
Prof. Heng-Guo Wang
Key Laboratory of polyoxometalate and Reticular Material Chemistry of Ministry of Education and Faculty of Chemistry, Northeast Normal University, Changchun, 130024 China
E-mail: [email protected]; [email protected]; [email protected]
Search for more papers by this authorCorresponding Author
Long Chen
State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun, 130012 China
E-mail: [email protected]; [email protected]; [email protected]
Search for more papers by this authorAbstract
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.
Conflict of Interests
The authors declare no conflict of interest.
Open Research
Data Availability Statement
The data that support the findings of this study are available in the Supporting Information of this article.
Supporting Information
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|---|---|
| ange202510604-sup-0001-SupMat.docx6.3 MB | Supporting Information |
Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.
References
- 1Y. Zhong, W. Dong, S. Ren, L. Li, Adv. Mater. 2024, 36, 2308251.
- 2D. Chen, W. Chen, Y. Wu, L. Wang, X. Wu, H. Xu, L. Chen, Angew. Chem. Int. Ed. 2023, 62, e202217479.
- 3Z. Chen, J. Wang, M. Hao, Y. Xie, X. Liu, H. Yang, G. I. N. Waterhouse, X. Wang, S. Ma, Nat. Commun. 2023, 14, 1106.
- 4A. P. Côté, A. I. Benin, N. W. Ockwig, M. O'Keeffe, A. J. Matzger, O. M. Yaghi, Science 2005, 310, 1166–1170.
- 5W. Meng, Y. Li, Z. Zhao, X. Song, F. Lu, L. Chen, Chem. Res. Chin. Univ. 2022, 38, 440–445.
- 6Z. Tie, S. Deng, H. Cao, M. Yao, Z. Niu, J. Chen, Angew. Chem. Int. Ed. 2022, 61, e202115180.
- 7Q. Zhao, Y. Lu, J. Chen, Adv. Energy Mater. 2017, 7, 1601792.
- 8Y. Liu, X. Zhao, C. Fang, Z. Ye, Y.-B. He, D. Lei, J. Yang, Y. Zhang, Y. Li, Q. Liu, Y. Huang, R. Zeng, L. Kang, J. Liu, Y.-H. Huang, Chem 2018, 4, 2463–2478.
- 9N. Wang, Z. Guo, Z. Ni, J. Xu, X. Qiu, J. Ma, P. Wei, Y. Wang, Angew. Chem. Int. Ed. 2021, 60, 20826–20832.
- 10C. S. Diercks, O. M. Yaghi, Science 2017, 355, eaal1585.
- 11D. Rodríguez-San-Miguel, F. Zamora, Chem. Soc. Rev. 2019, 48, 4375–4386.
- 12Y. Lin, H. Cui, C. Liu, R. Li, S. Wang, G. Qu, Z. Wei, Y. Yang, Y. Wang, Z. Tang, H. Li, H. Zhang, C. Zhi, H. Lv, Angew. Chem. Int. Ed. 2023, 62, e202218745.
- 13F. Kang, L. Yan, Z. Chen, Y. Zhang, Q. Gu, J. Yang, S. Xu, X. Wang, C.-S. Lee, Y. Wang, Q. Zhang, Angew. Chem. Int. Ed. 2025, 64, e202417779.
- 14X. Hu, N. Mao, X. Yan, L. Huang, X. Liu, H. Yang, Q. Sun, X. Liu, H. Jia, Chem. Res. Chin. Univ. 2024, 40, 824–841.
- 15J. Liu, K. Guo, W. Guo, J. Chang, Y. Li, F. Bao, Angew. Chem. Int. Ed. 2025, 64, e202424494.
- 16C. Wang, Y. Ni, C. Zhu, Y. Li, Z. Yan, Y. Lu, J. Chen, Angew. Chem. Int. Ed. 2025, 64, e202423992.
- 17M. Wu, Y. Zhao, R. Zhao, J. Zhu, J. Liu, Y. Zhang, C. Li, Y. Ma, H. Zhang, Y. Chen, Adv. Funct. Mater. 2022, 32, 2107703.
- 18X. Li, S. Cai, B. Sun, C. Yang, J. Zhang, Y. Liu, Matter 2020, 3, 1507–1540.
- 19S. Xu, T. Naren, Y. Zhao, Q. Gu, T. W. Lau, C.-S. Lee, F.-R. Chen, J. Yin, L. Chen, Q. Zhang, Angew. Chem. Int. Ed. 2025, 64, e202422040.
- 20C. Li, D.-D. Wang, G. S. H. Poon Ho, Z. Zhang, J. Huang, K.-T. Bang, C. Y. Lau, S.-Y. Leu, Y. Wang, Y. Kim, J. Am. Chem. Soc. 2023, 145, 24603–24614.
- 21C. Qian, L. Feng, W. L. Teo, J. Liu, W. Zhou, D. Wang, Y. Zhao, Nat. Rev. Chem. 2022, 6, 881–898.
- 22K.-H. Xie, G.-B. Wang, F. Huang, F. Zhao, J.-L. Kan, Z.-Z. Chen, L. Cai, S.-L. Han, Y. Geng, Y.-B. Dong, Nat. Commun. 2025, 16, 3493.
- 23X. Yang, D.-H. Si, H.-F. Li, R. Cao, Y.-B. Huang, Mater. Chem. Front. 2024, 8, 1611–1618.
- 24S.-Y. Ding, W. Wang, Chem. Soc. Rev. 2013, 42, 548–568.
- 25J. L. Segura, M. J. Mancheño, F. Zamora, Chem. Soc. Rev. 2016, 45, 5635–5671.
- 26P.-L. Wang, S.-Y. Ding, Z.-C. Zhang, Z.-P. Wang, W. Wang, J. Am. Chem. Soc. 2019, 141, 18004–18008.
- 27Z.-C. Zhang, P.-L. Wang, Y.-F. Sun, T. Yang, S.-Y. Ding, W. Wang, J. Am. Chem. Soc. 2024, 146, 4822–4829.
- 28a) M. Torabi, M. Yarie, A. Tavassoli, N. Zarei, L. Vatannavaz, M. A. Zolfigol, S. Azizian, S. Khazalpour, Coord. Chem. Rev. 2025, 527, 216359; b) Q. Zhang, Z. Zhu, L. Liu, H. Huang, X. Chen, Y. Bian, M. Shao, X. Wei, C. Wang, D. Wang, J. Dong, Y. Guo, Y. Zhu, Y. Liu, Angew. Chem. Int. Ed. 2024, 63, e202319027; c) Q. Zhang, F. Zhang, J. Dong, M. Shao, M. Zhu, D. Wang, Y. Guo, J. Zhang, Y. Liu, Chem. Mater. 2022, 34, 6977–6984.
- 29X. Wang, M. Liu, Y. Liu, S. Shang, C. Du, J. Hong, W. Gao, C. Hua, H. Xu, Z. You, J. Chen, Y. Liu, J. Am. Chem. Soc. 2023, 145, 26900–26907.
- 30H. J. Kim, C. H. Heo, H. M. Kim, J. Am. Chem. Soc. 2013, 135, 17969–17977.
- 31Y. Hu, N. Dunlap, S. Wan, S. Lu, S. Huang, I. Sellinger, M. Ortiz, Y. Jin, S.-h. Lee, W. Zhang, J. Am. Chem. Soc. 2019, 141, 7518–7525.
- 32C. Guo, M. Liu, G.-K. Gao, X. Tian, J. Zhou, L.-Z. Dong, Q. Li, Y. Chen, S.-L. Li, Y.-Q. Lan, Angew. Chem. Int. Ed. 2022, 61, e202113315.
- 33G. Zhao, Y. Zhang, Z. Gao, H. Li, S. Liu, S. Cai, X. Yang, H. Guo, X. Sun, ACS Energy Lett. 2020, 5, 1022–1031.
- 34Y.-W. Song, P. Shi, B.-Q. Li, X. Chen, C.-X. Zhao, W.-J. Chen, X.-Q. Zhang, X. Chen, Q. Zhang, Matter 2021, 4, 253–264.
- 35H. Ye, C. Zhang, Y. Li, W. Zhang, K. Zhang, B. Li, W. Hua, K. Wang, K. Xu, Prog. Nat. Sci. Mater. Int. 2023, 33, 754–766.
- 36S. Haldar, A. Schneemann, S. Kaskel, J. Am. Chem. Soc. 2023, 145, 13494–13513.
- 37Z. Li, Q. Jia, Y. Chen, K. Fan, C. Zhang, G. Zhang, M. Xu, M. Mao, J. Ma, W. Hu, C. Wang, Angew. Chem. Int. Ed. 2022, 61, e202207221.
- 38Z. Luo, L. Liu, J. Ning, K. Lei, Y. Lu, F. Li, J. Chen, Angew. Chem. Int. Ed. 2018, 57, 9443–9446.
- 39S. Saha, S. Khamrui, K. Biradha, J. Am. Chem. Soc. 2024, 146, 26556–26566.
- 40Y. Zhang, Z. Qiao, R. Zhang, Z. Wang, H.-J. Wang, J. Zhao, D. Cao, S. Wang, Angew. Chem. Int. Ed. 2023, 62, e202314539.
- 41Y. Liu, Z. Li, C. Li, Y. Wei, S. Yan, Z. Ji, S. Zou, H. Li, Y. Liu, C. Chen, X. He, M. Wu, Chem. Eng. J. 2024, 488, 150778.
- 42Z. Wang, Y. Yang, Z. Zhao, P. Zhang, Y. Zhang, J. Liu, S. Ma, P. Cheng, Y. Chen, Z. Zhang, Nat. Commun. 2021, 12, 1982.
- 43K. Fan, J. Li, Y. Xu, C. Fu, Y. Chen, C. Zhang, G. Zhang, J. Ma, T. Zhai, C. Wang, J. Am. Chem. Soc. 2023, 145, 12682–12690.
- 44Q. Zhao, Y. Ni, Y. Lu, W. Xie, H. Li, Z. Yan, K. Zhang, Y. Li, J. Chen, Angew. Chem. Int. Ed. 2025, 64, e202424025.
- 45T.-X. Luan, L. Du, J.-R. Wang, K. Li, Q. Zhang, P.-Z. Li, Y. Zhao, ACS Nano 2022, 16, 21565–21575.
- 46L. Sporrer, Q. Guo, X. Li, A. Wrzesinska-Lashkova, F. Reichmayr, S. Fu, H. I. Wang, M. Bonn, X. Li, P.-A. Laval-Schmidt, M. Wang, Y. Lu, Y. Vaynzof, M. Yu, X. Feng, R. Dong, Angew. Chem. Int. Ed. 2025, 64, e202418390.
- 47L. Zheng, J. Ren, H. Ma, M. Yang, X. Yan, R. Li, Q. Zhao, J. Zhang, H. Fu, X. Pu, M. Hu, J. Yang, J. Mater. Chem. A 2023, 11, 108–117.
- 48X. Yan, S. Lyu, X.-Q. Xu, W. Chen, P. Shang, Z. Yang, G. Zhang, W. Chen, Y. Wang, L. Chen, Angew. Chem. Int. Ed. 2022, 61, e202201900.
- 49J. Klein, L. Kampermann, B. Mockenhaupt, M. Behrens, J. Strunk, G. Bacher, Adv. Funct. Mater. 2023, 33, 2304523.
- 50W. Yuan, J. Weng, Y. Sun, P. Zhang, M. Ding, S. Chen, P. Zhou, J. Zhou, Adv. Funct. Mater. 2025, 35, 2415402.
- 51H. Li, M. Tang, Y. Wu, Y. Chen, S. Zhu, B. Wang, C. Jiang, E. Wang, C. Wang, J. Phys. Chem. Lett. 2018, 9, 3205–3211.
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