Covalent Organic Frameworks-integrated Metal-Oxide-N-doped Catalysts: A Synergistic Approach to High Energy and Power Density
- School of New Energy and Intelligent Connected Vehicle, University of Sanya, Hainan, 572022, China
- Center for Energy and Environment, School of Advanced Sciences, KLE Technological University, Hubballi, 580 031, India
- Korea University, Seoul 02841, Republic of Korea
- School of Engineering, University of Petroleum and Energy Studies (UPES), Dehradun, Uttarakhand, India 248 007
- Department of Material Science, Hangzhou Dianzi University, Hangzhou, China
- The Quzhou Affiliated Hospital of Wenzhou Medical University, Quzhou People’s Hospital, Quzhou, 324000, China
- School of Chemistry, D amghan University, Damghan, 36716-45667, Iran
Received: 10-11-2025
Revised: 02-01-2026
Accepted: 15-02-2026
Published in Issue 30-04-2026
Copyright (c) 2026 Rozhin Darabi, P.M Anjana, Tejraj M. Aminabhavi, Li Fu, Hassan Karimi-Maleh (Author)

This work is licensed under a Creative Commons Attribution 4.0 International License.
How to Cite
PDF views: 15
Abstract
Supercapacitors have played an important role in electrochemical energy storage. The performance characteristics of supercapacitor devices greatly depend not only on the electrode design but also on the core materials used in the electrode. In this study, we synthesised a new class of ternary materials that require simple methods of synthesis, involving a covalent organic framework (COF)-NiCo2O4-N-doped nanocomposite using a cost-effective hydrothermal route of synthesis. Composite electrode of COF/NiCo₂O₄-N-doped was developed that exhibited a high specific capacitance of 1,283.3 F g-1 at a discharge current density of 2 A g-1 when measured using a three-electrode setup. To show the potential of using COF/NiCo₂O₄-N-doped electroactive materials to create a practical and functional device, we fabricated an asymmetric supercapacitor (ASC) out of the COF/NiCo₂O₄-N-doped composite as the positrode and activated carbon (AC) as the negatrode in an electrolyte of 3 M KOH. The fabricated ASC device, COF/NiCo₂O₄-N-doped//AC exhibited impressive 34.59 Wh kg-1 and 1235.75 W kg-1 energy and power density ratings, respectively at a 2 A g-1 discharge current density, which maintained 90% rate of performance after 10,000 cycles of operation. Thus, the current study presents an efficient electrode material for deployment in energy storage devices of the future.
Keywords
- COFs,
- Electrochemical stability,
- Pseudocapacitive,
- Supercapacitors,
- Transition metal oxide
References
- Zhang, Z., Xu, X., Xing, X., Tang, X., Zhang, X., Chen, J., Xu, Y., Jiang, H., Exquisitely functionalized porphyrin-COF self-supporting nanofilm for high-performance in-plane micro-supercapacitor. Appl Surf Sci 680, 161327 (2025).
- Shanavaz, H., Alharethy, F., Jeon, B.H., Exploring the potential of metal tailored imine based covalent organic framework for asymmetric supercapacitor applications. J Mol Struct 1321, 139983 (2025).
- Devendran, A., Nagai, A., Covalent Organic Framework-Derived Highly Defective Carbon-Integrated Polymer Composite Electrode for Supercapacitor Applications. ACS Appl Energy Mater 8, 2597–2611 (2025).
- Aribou, Z., Mzioud, K., Ouakki, M., Ferraa, N., Bakkali, S., Touhami, M.E., Recent Advances in Supercapacitor Materials: A Review on Performance Enhancement, Flexibility, and Scalability for Next-Generation Energy Storage. Advancements and Innovations in Electrochemical Conversion and Energy Storage. (2026) 163-236.
- R. Darabi, M. Shabani-Nooshabadi, ZIF-8/Co-C3N4-GNR/MXene nanocomposites: A novel electrode material with excellent electrochemical properties for supercapacitors, Alex Eng J 129 (2025) 803-810.
- Darabi, R., Zare, N., Karimi-Maleh, H., Karimi, F. Novel ternary nanocomposites as a powerful catalyst for high-performance all-solid-state asymmetric supercapacitors. Adv Compos Hybrid Mater 7, 184 (2024).
- Anakha, D., Nithyadas, K., Vyshnavi, T., Ananthkumar, M., Menon, P.R., Yamuna, R., Fabrication of CuO-βCD/Co-Al LDH nanocomposite for supercapacitor applications. Carbon Lett 35, 2791-2807 (2025).
- Oladele, I., Adelani, S., Taiwo, A., Akinbamiyorin, I., Olanrewaju, O., Orisawayi, A., Polymer-based nanocomposites for supercapacitor applications: a review on principles, production and products. RSC Adv 15, 7509-7534 (2025).
- Shariq, M., Alshehri, K., Bouzgarrou, S.M., Ali, S.K., Alqurashi, Y., Hassan, K., Azooz, R., Progress in development of MXene-based nanocomposites for supercapacitor application-A review. FlatChem 44, 100609 (2024).
- Sharma, S., Chand, P., Supercapacitor and electrochemical techniques: A brief review. Results Chem 5, 100885 (2023).
- Kumar, N., Kim, S.B., Lee, S.Y., Park, S.J., Recent advanced supercapacitor: a review of storage mechanisms, electrode materials, modification, and perspectives. Nanomaterials 12, 3708 (2022).
- Attia, S.Y., Mohamed, S.G., Barakat, Y.F., Hassan, H.H., Zoubi, W.A., Supercapacitor electrode materials: addressing challenges in mechanism and charge storage. Rev Inorg Chem 42, 53-88 (2022).
- Forouzandeh, P., Kumaravel, V., Pillai, S.C., Electrode materials for supercapacitors: a review of recent advances. Catalysts 10, 969 (2020).
- He, Y., Liu, X., He, K., Kamyab, H., Gnanasekaran, L., Anjana, P.M., Aminabhavi, T.M., Vasseghian, Y., Hojjati-Najafabadi, A., High-performance supercapacitors based on NiMn layered double hydroxides/Ni3S2 nanocomposite. J Power Sources 634, 236465 (2025).
- Wang, R., Gao, J., Vijayalakshmi, M., Tang, H., Chen, K., Reddy, C.V., Kakarla, R.R., Anjana, P.M., Rezakazemi, M., Cheolho, B., Shim, J., Aminabhavi, T.M., Metal–organic frameworks and their composites: Design, synthesis, properties, and energy storage applications. Chem Eng J 496, 154294 (2024).
- Bashir, T., Ghasali, E., Raza, S., Orooji, Y., Two-Dimensionally Aligned Vermiculite Nanoflakes with Built-In Diatomite Filler for Reversible Lithium-Ion Storage Performance. J Nanostructure Chem 15, 152506 (2025).
- Wang, M., Guo, H., Xue, R., Li, Q., Liu, H., Wu, N., Yao, W., Yang, W., Covalent organic frameworks: A new class of porous organic frameworks for supercapacitor electrodes. ChemElectroChem 6, 2984-2997 (2019).
- Sajjad, M., Lu, W., Covalent organic frameworks based nanomaterials: Design, synthesis, and current status for supercapacitor applications: A review. J Energy Storage 39, 102618 (2021).
- Waller, PJ., Gándar, F., Yaghi, OM., Chemistry of covalent organic frameworks. Acc Chem Res 48, 3053–3063 (2015)."[20]
- Hu, D., Jia, Y., Yang, S., Lin, C., Huang, F., Wu, R., Guo, S., Xie, K., Du, P., Hierarchical nanocomposites of redox covalent organic frameworks nanowires anchored on graphene sheets for super stability supercapacitor. Chem Eng J 488, 151160 (2024)."
- Li, R., Li, J., Liu, Q., Li, T., Lan, D., Ma, Y., Recent progress on covalent organic frameworks and their composites as electrode materials for supercapacitors. Adv Compos Mater 8 (2025) 86.
- Darabi, R., Karimi-Maleh, H., Zhong, N., Karimi-Harandi, M.H., Preparation of Fe-MOF/CuO/C3N4 as novel assemblies nanocomposites for high performance asymmetric supercapacitors. Electrochim Acta 480, 143871 (2024).
- Yang, Y., Xu, D., Sun, Q., Li, Y., Zhang, W., Li, Z., Hu, Z., Anthraquinone-based covalent organic framework/reduced graphene oxide composites for supercapacitors. J Energy Storage 114, 115881 (2025)
- Jameel, Y., Firdaus, A.H.M., Salit, M.S., Nanocomposites in energy conversion. Phys Sci Rev (2025) https://doi.org/10.1515/psr-2024-0028
- Wang, C., Zhou, E., He, W., Deng, X., Huang, J., Ding, M., Wei, X., Liu, X., Xu, X., NiCo2O4-Based Supercapacitor Nanomaterials, Nanomaterials 7(2), 41 2017.
- Li, Y., Han, X., Yi, T., He, Y., Li, X., Review and prospect of NiCo2O4-based composite materials for supercapacitor electrodes. J Energy Chem 31, 54-78 (2019).
- [27] Abouali, S., Garakani, MA., Xu, ZL., Kim, JK., NiCo2O4/CNT nanocomposites as bi-functional electrodes for Li ion batteries and supercapacitors. Carbon 102, 262-272 (2016).
- Li, Q., Lu, C., Chen, C., Xie, L., Liu, Y., Li, Y., Kong, Q., Wang, H., Layered NiCo2O4/reduced graphene oxide composite as an advanced electrode for supercapacitor. Energy Storage Mater 8, 59-67 (2017)
- Wu, P., Cheng, S., Yao, M., Yang, L., Zhu, Y., Liu, P., Xing, O., Zhou, J., Wang, M., Luo, H., Liu, M., A Low-Cost, Self-Standing NiCo2O4@CNT/CNT Multilayer Electrode for Flexible Asymmetric Solid-State Supercapacitors. Adv Funct Mater 27, 1702160 (2017).
- Zhong, X., Shu, C., Su, X., Wang, W., Gong, J., Insight into improved oxygen evolution reaction on electronic modulation of phosphorus doped NiCo2O4. Mater Today Commun 31, 103708 (2022).
- Zhang, H., Li, H., Wang, H., He, K., Wang, S., Tang, Y., Chen, J., NiCo2O4/N-doped graphene as an advanced electrocatalyst for oxygen reduction reaction. J Power Sources 280, 640-648 (2015)
- Feng, X., Huang, Y., Li, C., Chen, X., Zhou, S., Gao, X., Chen, C., Controllable synthesis of porous NiCo2O4/NiO/Co3O4 nanoflowers for asymmetric all-solid-state supercapacitors. Chem Eng J 368, 51-60 (2019).
- Wang, Z., Su, H., Liu, F., Chu, X., Yan, C., Gu, B., Huang, H., Yang, T., Chen, N., Han, Y., Establishing highly-efficient surface faradaic reaction in flower-like NiCo O nano-/micro-structures Porous Carbon Framework with B-Doped NiCo2O4 Nanoclusters for Enhancing the Performance of Carbon Fiber-Based Flexible Supercapacitors. ACS Appl Nano Mater 7, 11816-11826 (2024).
- Yuvaraja, R., Sarathkumar, S., Gowsalya, V., Anitha Juliet, S.P., Veeralakshmi, S., Kalaiselvam, S., Hussain, S., Nehru, S., In situ synthesis of NiCo2O4/carbon nanocomposites: effect of carbon content and symmetric/asymmetric device configuration on supercapacitor performance. New J Chem 48, 15556-15566 (2024).
- Zhou, Y., Li, C., Li, X., Huo, P., Wang, H., Construction of high-performance electrode materials of NiCo2O4 nanoparticles encapsulated in ultrathin N-doped carbon nanosheets for supercapacitors. Dalton Trans 50, (2021) 1097-1105
- Mulik, S.V., Koyale, P.A., Soni, S.S., Maske, S.M., Dongale, T.D., Sutar, S.S., Parale, V.G., Park, H.H., Delekar, S.D., Optimized Fabrication of Supercapacitor Using MOF-Derived NiCo2O4 with Porous Carbon as Cathode: Electrochemical Characterization and Stability Analysis using Time Series Analysis Technique. ACS Appl Electron 6, 4369-4380 (2024).
- Bhatti, M.A., Kumar, S., Tahira, A., Bhatti, A.L., Ujjan, Z.A., Jakhrani, M.A., Aftab, U., Alshammari, R.H., Nafady, A., Dawi, E., Emo, M., Vigolo, B., Infantes-Molina, A., Ibupoto, Z.H., Advanced NiCo2O4/ZnO-CuO/NF composite for high-performance asymmetric supercapacitor and efficient oxygen evolution reaction applications, Adv Compos Hybrid Mat 8, 148 (2025).
- Chen, S., Gao, P., Zhang, D., Lin, L., Huang, L., Li, Z., Lan, Z., Jiang, Y., Ru, Q., Zhou, G., Liu, J.M., Kempa, K., Gao,V., Flexible asymmetric supercapacitors based on NiCo2O4 in a neutral electrolyte achieving 2.4 V voltage window. J Alloys Compd 860, 158346 (2021).
- Choi, K., Moon, I.K., Oh, J., An efficient amplification strategy for N-doped NiCo 2 O 4 with oxygen vacancies and partial Ni/Co-nitrides as a dual-function electrode for both supercapatteries and hydrogen electrocatalysis. J Mater Chem A 7, 1468-1478 (2019).
- Wang, Z., Li, H., Guo, Z., Liang, H., Jin, L., Li, M., Ao, Y., Compd 860, 158346 (2021).
- Wang, W., Qi, J., Sui, Y., He, Y., Meng, Q., Wei, F., Jin, Y., An Asymmetric Supercapacitor Based on Activated Porous Carbon Derived from Walnut Shells and NiCo₂O₄ Nanoneedle Arrays Electrodes, J Nanosci Nanotechnol 18, 5600-5608 (2018).
10.57647/jnsc.2026.1602.09