Hydrothermally Synthesized CoMn₂O₄/Graphite Composite as a High-Capacity Anode for Lithium-Ion Batteries
DOI:
https://doi.org/10.11113/jamst.v30n2.352Keywords:
CoMn2O4; Hydrothermal method; Anode materials; Graphite; Lithium-ion batteriesAbstract
The increasing demand for high-energy-density lithium-ion batteries (LIBs) drives the development of anode materials with capacities exceeding that of graphite (372 mAh g⁻¹). CoMn₂O₄, with a high theoretical capacity (921 mAh g⁻¹), is a promising candidate but suffers from low conductivity and severe volume expansion. In this work, a CoMn₂O₄/graphite (CMO/g) composite is developed to address these limitations through a synergistic effect. CoMn₂O₄ is synthesized via a hydrothermal method followed by calcination, and the sample treated at 700 °C exhibits the best crystallinity and morphology. Structural characterizations (XRD, FTIR, FESEM-EDX) confirm the successful formation of the composite and uniform distribution of CoMn₂O₄ on graphite. Electrochemical evaluations reveal that CMO/g-3 delivers a high initial discharge capacity of 2503 mAh g⁻¹ and maintains ~1000 mAh g⁻¹ after 100 cycles with nearly 100% coulombic efficiency and low charge-transfer resistance. A full cell assembled with CMO/g-3 and LiFePO₄ provides an initial discharge capacity of 146.5 mAh g⁻¹ at 0.2 A g-1, although capacity fading occurs upon prolonged cycling due to volume expansion effects. Overall, the CoMn₂O₄/graphite composite demonstrates enhanced electrochemical performance and promising potential as a high-capacity anode material for next-generation LIBs.
References
[1] Lin, S., & Zhang, T. (2024). Preparation of various Co/Cu and Co/Fe molar ratios and gel-modified nanomaterials as anodes for Li-ion batteries. Materials Chemistry and Physics, 311, 128547.
[2] International Energy Agency. (2022). World energy outlook 2022. International Energy Agency.
[3] Raimi, D., & Newell, R. G. (2024). Global energy outlook comparison methods: 2023 update.
[4] Cai, W., Yao, Y.-X., Zhu, G.-L., Yan, C., Jiang, L.-L., He, C., Huang, J.-Q., & Zhang, Q. (2020). A review on energy chemistry of fast-charging anodes. Chemical Society Reviews, 49(12), 3806–3833.
[5] Elalfy, D. A., Gouda, E., Kotb, M. F., Bureš, V., & Sedhom, B. E. (2024). Comprehensive review of energy storage systems technologies, objectives, challenges, and future trends. Energy Storage Research, 54, 101482.
[6] Li, M.-T., Liu, R.-R., Wang, L.-Y., Wang, H.-J., Sun, J.-W., & Yu, Y. (2025). Iron-based bimetallic oxide carbon composites with superior lithium storage capabilities serve as anode in lithium-ion batteries. Inorganic Chemistry Communications, 574, 122399.
[7] Cai, K.-X., Luo, S.-H., Jun, C., Kun, L., Yan, S.-X., Hou, P.-Q., Qing, W., Zhang, Y.-H., & Xin, L. (2023). Enhancement of lithium storage performance of ZnMn₂O₄ anode by optimizing hydrothermal synthesis. Transactions of Nonferrous Metals Society of China, 33(9), 2772–2783.
[8] Sanad, M., Yousef, A. K., Rashad, M., Naggar, A., & El-Sayed, A. (2020). Robust and facile strategy for tailoring CoMn₂O₄ and MnCo₂O₄ structures as high-capacity anodes for lithium-ion batteries. Polyhedron, 579, 411889.
[9] Shi, Y. J., Song, M. J., Zhang, Y., Zhang, C., Gao, H., Niu, J. Z., Ma, W. S., Qin, J. Y., & Zhang, Z. H. (2019). A self-healing CuGa₂ anode for high-performance Li-ion batteries. Journal of Power Sources, 437, 226916.
[10] Shen, M., & Ma, H. (2022). Metal-organic frameworks (MOFs) and their derivatives as electrode materials for lithium-ion batteries. Coordination Chemistry Reviews, 470, 214715.
[11] Zhang, D., Zhang, C. Y., Xu, H. S., Huo, Z., Shi, X. Y., Luo, B. M., Liu, G. Y., Liu, X. D., Li, L. P., & Yu, C. (2024). Ultrafast synthesis of spinel AMn₂O₄ (A = Co, Mn, Zn) nanopolyhedras and their composites applied to lithium-ion battery anode. Journal of Alloys and Compounds, 987, 174040.
[12] Pan, X., Ma, J., Yuan, R., & Yang, X. (2017). Layered double hydroxides for preparing CoMn₂O₄ nanoparticles as anodes of lithium-ion batteries. Materials Chemistry and Physics, 194, 137–141.
[13] Abdah, M. A. A. M., Azlan, F. N. M., Wong, W. P., Mustafa, M. N., Walvekar, R., & Khalid, M. (2024). Microwave-assisted upcycling of plastic waste to high-performance carbon anode for lithium-ion batteries. Chemosphere, 349, 140973.
[14] Yao, B., Wang, Z., Ding, C., Feng, M., Li, Z., & Huang, Y. (2023). ZnFe₂O₄/Graphite composite with high performance as anode material for lithium-ion batteries. Energy Materials Letters, 19(1), 29–37.
[15] Murugesan, M., Nallamuthu, N., Ranjithkumar, R., Krishnakumar, M., Devendran, P., & Ramesh, K. (2023). Synthesis and electrochemical investigation of hetero-bimetallic CoMn₂O₄ microrods for novel supercapacitor electrodes. Energy Materials Letters, 19(1), 108–118.
[16] Azad, A. K., Abdalla, A. M., Kumarasinghe, P. I. I., Nourean, S., Azad, A. T., Ma, J., Jiang, C., Dawood, M. M. K., Wei, B., & Patabendige, C. N. K. (2024). Developments and key challenges in micro/nanostructured binary transition metal oxides for lithium-ion battery anodes. Journal of Energy Storage, 84, 110850.
[17] Wang, W., Zhang, P., Jiang, X., Zhou, J.-J., Xu, L., Chen, F., & Chen, L. (2022). Constructing N-doped carbon beads-encapsulated CoMn₂O₄ microboxes with pyramidal walls for enhanced Li storage. Materials Today Energy, 30, 101149.
[18] Nakhodchari, M. M., Seifi, M., & Moghadam, M. T. (2023). Ternary MnCo₂O₄/MWCNT/rGO nanocomposites as high-performance supercapacitor electrode materials. Journal of Physics and Chemistry of Solids, 174, 111170.
[19] Rong, T., Yuan, Y., Yu, H., Zuo, H., & Xue, Q. (2023). Research on anthracite-derived graphite flakes prepared by molten salt electrolysis as anode materials for high-performance lithium-ion batteries. Fuel Processing Technology, 252, 107992.
[20] Feng, J., Zhang, B., Du, P., Yuan, Y., Li, M., Chen, X., Guo, Y., Xie, H., & Yin, H. (2023). Recovery of LiCoO₂ and graphite from spent lithium-ion batteries by molten-salt electrolysis. iScience, 26(11), 108097.
[21] Abdah, M. A. A. M., Mokhtar, M., Khoon, L. T., Sopian, K., Dzulkurnain, N. A., Ahmad, A., Sulaiman, Y., Bella, F., & Su’ait, M. S. (2021). Synthesis and electrochemical characterizations of poly(3,4-ethylenedioxythiophene)/manganese oxide coated on porous carbon nanofibers as a potential anode for lithium-ion batteries. Energy Reports, 7, 8677–8687.
[22] Saidi, N. M., Khairudin, A., Mustafa, M. N., Omar, F. S., Gerard, O., Tan, Y. S., Khalid, M., & Numan, A. (2024). Highly amorphous cobalt phosphate synthesized via microwave route as a superior positive electrode material for asymmetric supercapatteries. Journal of Energy Storage, 97, 112647.
[23] Mustafa, M. N., Abdah, M. A. A. M., Numan, A., Sulaiman, Y., Walvekar, R., & Khalid, M. (2023). Effect of precursor concentration on the electrochemical properties of nickel cobalt phosphate for high-performance electrochromic supercapacitors. Journal of Energy Storage, 74, 109321.
[24] Mundinamani, S., & Rabinal, M. K. (2014). Cyclic voltammetric studies on the role of electrode, electrode surface modification and electrolyte solution of an electrochemical cell. IOSR Journal of Applied Chemistry, 7, 45–52.
[25] Saidi, N. M., Khairudin, A., Li, L., Abdah, M. A. A. M., Gerard, O., Tan, Y. S., Khalid, M., Khan, F., Mustafa, M. N., & Numan, A. (2023). Performance comparison of 2D nickel phosphate nanoparticles prepared via sonochemical and microwave-assisted hydrothermal routes for supercapattery. Journal of Energy Storage, 73, 108846.
[26] Gerard, O., Ramesh, S., Ramesh, K., Numan, A., Mustafa, M. N., Khalid, M., Ramesh, S., & Tiong, S. K. (2024). Evaluation of the effect of precursor ratios on the electrochemical performances of binder-free NiMn-phosphate electrodes for supercapattery. Journal of Colloid and Interface Science, 667, 585–596.
[27] Mijailović, D. M., Radmilović, V. V., Lačnjevac, U. Č., Stojanović, D. B., Bustillo, K. C., Jović, V. D., Radmilović, V. R., & Uskoković, P. S. (2021). Tetragonal CoMn₂O₄ nanocrystals on electrospun carbon fibers as high-performance battery-type supercapacitor electrode materials. Dalton Transactions, 50(43), 15669–15678.
[28] Deng, J., Liu, C., Chen, X., & Madou, M. (2026). Mechanically strong and highly conductive graphitized carbon nanowire arrays for nano-fabrication of carbon-based chips. Microsystems & Nanoengineering, 12(1), 30.
[29] Kanagambal, P., Ahamed, A. J., & Rajeswaran, P. (2023). A novel mesoporous CoMn₂O₄@rGO composite as an electrode material for hybrid supercapacitor energy storage device applications. Diamond and Related Materials, 137, 110098.
[30] Mohd Abdah, M. A. A., Mohammad Azlan, F. N., Wong, W. P., Mustafa, M. N., Walvekar, R., & Khalid, M. (2024). Microwave-assisted upcycling of plastic waste to high-performance carbon anode for lithium-ion batteries. Chemosphere, 349, 140973.
[31] Mohd Abdah, M. A. A., Mohammad Azlan, F. N., Wong, W. P., Mustafa, M. N., Numan, A., Walvekar, R., & Khalid, M. (2025). Enhancing sustainable lithium-ion battery anode using activated carbon-derived polypropylene plastic waste/MXene hybrid composite. Journal of Electroanalytical Chemistry, 997, 119472.
[32] Sunjaya, N. B. P., Yulianti, R. T., Hanifah, A., Fadila, S., Indriyati, I., Priyono, S., Indayaningsih, N., Setiawan, J., Effendi, M., & Yudianti, R. (2026). Structural and synergistic effect of SnO₂–carbon interfaces for improved lithium-ion battery anode performance. Surfaces and Interfaces, 83, 108502.
[33] Min, K., Kim, K., An, H., Go, Y., Lee, Y., Lim, D., & Baeck, S.-H. (2022). Yolk-shell-structured SiO₂@N,P co-doped carbon spheres as highly stable anode materials for lithium-ion batteries. Journal of Power Sources, 543, 231849.
[34] Cifre-Herrando, M., Roselló-Márquez, G., & García-Antón, J. (2025). Structural and electrochemical characterization of modified WO₃ nanostructures for lithium-ion battery anodes. Separation and Purification Technology, 373, 133673.
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