Carbon supported Fe₇₀Co₂₀Ni₁₀ trimetallic catalyst for enhanced cathode performance in Dual-chamber microbial fuel cells for wastewater treatment
Article Main
Abstract
Scalable microbial fuel cells (MFCs) for simultaneous wastewater treatment and electricity generation require cost-effective, high-performance cathode catalysts that operate efficiently at neutral pH. Herein, the present study reports a trimetallic Fe₇₀Co₂₀Ni₁₀ alloy nanoparticle catalyst supported on carbon (Fe₇₀Co₂₀Ni₁₀/C) as a highly active and durable oxygen reduction reaction (ORR) electrocatalyst. The catalyst was synthesized via a facile thermal-activation route using sodium borohydride (NaBH4), yielding homogeneous alloy nanoparticles (8–12 nm) with pronounced electron transfer from Fe to Ni, thereby optimizing oxygen adsorption energy and enhancing ORR kinetics. When deployed as a cathode in a dual-chamber MFC at 1.0 mg cm⁻² loading, Fe₇₀Co₂₀Ni₁₀/C delivered a maximum power density of 1532 mW m⁻² and an open-circuit voltage of 0.936 V, and operational stability for over 1100 hours. This configuration also achieved high wastewater treatment efficiency, with 89.7% chemical oxygen demand (COD) removal and 9.7% coulombic efficiency. These findings highlight the superior catalytic and operational performance of Fe₇₀Co₂₀Ni₁₀/C compared with the synthesized mono- and bimetallic Fe, Co, and Ni-based catalysts, suggesting its potential as a cost-effective alternative to precious-metal catalysts for MFC applications for wastewater treatment
Article Details
Article Details
Keywords
Coulombic efficiency, Dual-chamber microbial fuel cell reactor, Fe₇₀Co₂₀Ni₁₀/C cathode catalyst, Oxygen reduction reaction (ORR), Power density
References
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Mercado, R., Zhang, J. Z., En Lu, J., Allen, A., Zhang, P., Zhang, T., Lu, J. Q., Wahl, C., Lu, B. & Chen, S. (2020). Nitrogen‐doped porous carbon cages for electrocatalytic reduction of oxygen: Enhanced performance with iron and cobalt dual metal centers. ChemCatChem, 12(12), 3230–3239. https://doi.org/10.1002/cctc.201902324
Mohammadi, F., Vakili-Nezhaad, G. R., Al-Rawahi, N. & Gholipour, S. (2023). Microbial electrochemical systems for bioelectricity generation: Current state and future directions. Results in Engineering, 20, 101619. https://doi.org/10.1016/j.rineng.2023.101619
Muthusamy, S., Billo, T., Chen, K., Sabhapathy, P., Sabbah, A., Chang, Y., Syum, Z. & Chen, L. (2023). Modification of conductive carbon with N‐Coordinated Fe−Co dual‐metal sites for oxygen reduction reaction. ChemElectroChem, 10(19). https://doi.org/10.1002/celc.202300272
Nandikes, G., Singh, L. & Gouse Peera, S. (2021). Perovskite-based nanocomposite electrocatalysts: An alternative to platinum ORR catalyst in microbial fuel cell cathodes. Energies, 15(1), 272. https://doi.org/10.3390/en15010272
Pan, P. & Bhattacharyya, N. (2023). Bioelectricity production from microbial fuel cell (MFC) using Lysinibacillus xylanilyticus strain nbpp1 as a biocatalyst. Current Microbiology, 80(8). https://doi.org/10.1007/s00284-023-03338-5
Pan, Q.-R., Li, N., Liu, Z.-Q., Lai, B.-L., Huang, L.-J. & Feng, Y.-N. (2022). Regulating the electronic structure of Cu-Nx active sites for efficient and durable oxygen reduction catalysis to improve microbial fuel cell performance. ACS Applied Materials & Interfaces, 15(1), 1234–1246. https://doi.org/10.1021/acsami.2c18876
Sawant, S. Y., Han, T. H. & Cho, M. H. (2016). Metal-free carbon-based materials: Promising electrocatalysts for oxygen reduction reaction in microbial fuel cells. International Journal of Molecular Sciences, 18(1), 25. https://doi.org/10.3390/ijms18010025
Scharf, J., Wallace, W. D. Z., Kübler, M., Paul, S. D., Ni, L., Gridin, V. & Kramm, U. I. (2022). Relation between half‐cell and fuel cell activity and stability of FeNC catalysts for the oxygen reduction reaction. SusMat, 2(5), 630–645. https://doi.org/10.1002/sus2.84
Soleimani, A., Heidari, M., Luo, Y., Khorrami, B. M. & Hosseini Dolatabadi, S. H. (2023). Hydrogen: An integral player in the future of sustainable transportation. A survey of fuel cell vehicle technologies, adoption patterns, and challenges. mdpi ag. https://doi.org/10.20944/preprints202310.0415.v1
Subhadarshini, S., Venkata Mohan, S., Sarkar, O., Jana, T., Roy, T. K. & Sravan, J. S. (2023). Sulfonated polybenzimidazole as a PEM in a microbial fuel cell: An efficient strategy for green energy generation and wastewater cleaning. ACS Applied Energy Materials, 6(3), 1422–1438. https://doi.org/10.1021/acsaem.2c03238
Tan, S.-M., Wong, Y.-S., Ong, S.-A., Teoh, T.-P., Thung, W.-E. & Ho, L.-N. (2020). The reaction of wastewater treatment and power generation of single chamber microbial fuel cell against substrate concentration and anode distributions. Journal of Environmental Health Science and Engineering, 18(2), 793–807. https://doi.org/10.1007/s40201-020-00504-w
Theofanidis, S. A., Detavernier, C., Longo, A., Galvita, V. V., Meledina, M., Poelman, H., Van Tendeloo, G., Marin, G. B. & Dharanipragada, N. V. R. A. (2018). Fe-containing magnesium aluminate support for stability and carbon control during methane reforming. ACS Catalysis, 8(7), 5983–5995. https://doi.org/10.1021/acscatal.8b01039
Tornheim, A. & O’Hanlon, D. C. (2020). What do coulombic efficiency and capacity retention truly measure? A deep dive into cyclable lithium inventory, limitation type, and redox side reactions. Journal of The Electrochemical Society, 167(11), 110520. https://doi.org/10.1149/1945-7111/ab9ee8
Wang, Y., Xing, J., Qian, J., Liu, L. & Li, J. (2023). Facile fabrication of nickel supported on reduced graphene oxide composite for oxygen reduction reaction. Nanomaterials, 13(24), 3087. https://doi.org/10.3390/nano13243087
Xie, H., Zhou, G., Jiao, Z., Du, Q., Li, H., Ren, J. & Chen, S. (2017). Catalytic combustion of volatile aromatic compounds over CuO-CeO2 catalyst. Korean Journal of Chemical Engineering, 34(7), 1944–1951. https://doi.org/10.1007/s11814-017-0111-4
Zhang, J., Li, F., Liu, W., Wang, Q., Li, X., Hung, S.-F., Yang, H. & Liu, B. (2024). Modulating spin of atomic manganese center for high-performance oxygen reduction reaction. Angewandte Chemie (International Ed. in English), 63(51). https://doi.org/10.1002/anie.202412245
Zhao, Y., Liu, J., Yu, G., Liao, L. & Wei, P. (2019). B‐Doped Fe/N/C Porous catalyst for high‐performance oxygen reduction in anion‐exchange membrane fuel cells. ChemElectroChem, 6(6), 1754–1760. https://doi.org/10.1002/celc.201801688
Zhong, G., Fu, X., Wang, F., Liu, L., Xu, S., Wang, H., Dou, J., Zheng, C. Z. & Liao, W. (2020). Effect of experimental operations on the limiting current density of oxygen reduction reaction evaluated by rotating‐disk electrode. ChemElectroChem, 7(5), 1107–1114. https://doi.org/10.1002/celc.201902085
Zhou, D., Sun, X., Xu, W., Kuang, Y., Mohammed‐Ibrahim, J., Jawaid, S., Liu, W. & Li, P. (2020). Recent advances in non-precious metal‐based electrodes for alkaline water electrolysis. ChemNanoMat, 6(3), 336–355. https://doi.org/10.1002/cnma.202000010
Bhat, A. Y., Bashir, A. U., Jain, P., Bhat, M. A. & Ingole, P. P. (2024). Unraveling the active sites on mesoporous CuFe2O4@N-carbon catalysts with abundant oxygen vacancies and M-N-C content for boosted nitrogen reduction toward electrosynthesis of ammonia. Small (Weinheim an Der Bergstrasse, Germany), 20(45). https://doi.org/10.1002/smll.202403319
Dessie, Y. & Tadesse, S. (2022). Advancements in bioelectricity generation through nanomaterial-modified anode electrodes in microbial fuel cells. Frontiers in Nanotechnology, 4. https://doi.org/10.3389/fnano.2022.876014
Dey, S., Dhal, G. C., Mohan, D. & Prasad, R. (2020). Structural and catalytic properties of Fe and Ni doping on CuMnOx catalyst for CO oxidation. Advanced Composites and Hybrid Materials, 3(1), 84–97. https://doi.org/10.1007/s42114-020-00139-3
Fantauzzi, M., Passiu, C., Rossi, A., Secci, F., Cannas, C. & Sanna Angotzi, M. (2019). Nanostructured spinel cobalt ferrites: Fe and Co chemical state, cation distribution and size effects by X-ray photoelectron spectroscopy. RSC Advances, 9(33), 19171–19179. https://doi.org/10.1039/c9ra03488a
Gangadharan, P. K., Kurungot, S. & Pandikassala, A. (2021). Toward pH independent oxygen reduction reaction by polydopamine derived 3D interconnected, iron carbide embedded graphitic carbon. ACS Applied Materials & Interfaces, 13(7), 8147–8158. https://doi.org/10.1021/acsami.0c18036
Gayathri, A., Kiruthika, S., Selvarani, V., Alsalhi, M.S., Devanesan, S., Kim, W. & Muthukumaran, B. (2022). Evaluation of iron-based alloy nanocatalysts for the electrooxidation of ethylene glycol in membraneless fuel cells. Fuel, 321: 124059, https://doi.org/10.1016/j.fuel.2022.124059.
Gilanizadeh, M. & Zeynizadeh, B. (2018). Synthesis of magnetic Fe3O4@SiO2@Cu–Ni–Fe–Cr LDH: an efficient and reusable mesoporous catalyst for reduction and one-pot reductive-acetylation of nitroarenes. Journal of the Iranian Chemical Society, 15(12), 2821–2837. https://doi.org/10.1007/s13738-018-1469-x
Guadarrama-Pérez, O., Bustos-Terrones, V., Guadarrama-Pérez, V. H., Guillén-Garcés, R. A., Hernández-Romano, J., Treviño-Quintanilla, L. G., Estrada-Arriaga, E. B. & Moeller-Chávez, G. E. (2023). Variation of graphene/titanium dioxide concentration as electrocatalyst for an oxygen reduction reaction in constructed wetland-microbial fuel cells. Electrochemistry Communications, 157, 107618. https://doi.org/10.1016/j.elecom.2023.10 7618
Ishaq, A., Azman, S. B., Said, M. I. M., Bello, A. D., Abubakar, U. A., Jagun, Z. T., Houmsi, M. R., Isah, A. S. & Mohammad, S. J. (2024). The influence of various chemical oxygen demands on microbial fuel cells performance using leachate as a substrate. Environmental Science and Pollution Research, https://doi.org/10.1007/s11356-024-32090-x
Jadhav, G. S., Mehta, A. K., Tripathi, A. & Ghangrekar, M. M. (2024). Multi-metal ferrite as a promising catalyst for oxygen reduction reaction in microbial fuel cell. Environmental Science and Pollution Research International, 31(42), 54402–54416. https://doi.org/10.1007/s11356-024-34220-x
Khater, D., Hazaa, M., Hassan, R. Y. A. & El-Khatib, K. M. (2024). Electricity generation using Glucose as substrate in microbial fuel cell. Journal of Basic and Environmental Sciences, 2(3), 84–98. https://doi.org/10.21608/jbes.2024.369589
Liu, X., Li, Y., Liu, H., Yang, H., Yang, B., Zhang, Q., Zou, L., Zou, Z. & Chen, C. (2019). Fe2N nanoparticles boosting FeNx moieties for highly efficient oxygen reduction reaction in Fe-N-C porous catalyst. Nano Research, 12(7), 1651–1657. https://doi.org/10.1007/s12274-019-2415-7
Luo, S., Yao, J., Wang, R., Wang, L., Chen, X., Yu, D. & Elfalleh, W. (2021). Effect of nickel modification on Ru–Ni/NaY catalyst structure and linoleic acid isomerization selectivity. Journal of Food Measurement and Characterization, 15(6), 5584-5598. https://doi.org/10.1007/s11694-021-01101-7
Ma, Q., Li, Z., Ma, J., Jin, H., Zhang, Z., Liu, B., Xu, H., Zhu, J. & Mu, S. (2021). Stabilizing Fe-N-C catalysts as model for oxygen reduction reaction. Advanced Science, 8(23), 2102209. https://doi.org/10.1002/advs.202102209
Mercado, R., Zhang, J. Z., En Lu, J., Allen, A., Zhang, P., Zhang, T., Lu, J. Q., Wahl, C., Lu, B. & Chen, S. (2020). Nitrogen‐doped porous carbon cages for electrocatalytic reduction of oxygen: Enhanced performance with iron and cobalt dual metal centers. ChemCatChem, 12(12), 3230–3239. https://doi.org/10.1002/cctc.201902324
Mohammadi, F., Vakili-Nezhaad, G. R., Al-Rawahi, N. & Gholipour, S. (2023). Microbial electrochemical systems for bioelectricity generation: Current state and future directions. Results in Engineering, 20, 101619. https://doi.org/10.1016/j.rineng.2023.101619
Muthusamy, S., Billo, T., Chen, K., Sabhapathy, P., Sabbah, A., Chang, Y., Syum, Z. & Chen, L. (2023). Modification of conductive carbon with N‐Coordinated Fe−Co dual‐metal sites for oxygen reduction reaction. ChemElectroChem, 10(19). https://doi.org/10.1002/celc.202300272
Nandikes, G., Singh, L. & Gouse Peera, S. (2021). Perovskite-based nanocomposite electrocatalysts: An alternative to platinum ORR catalyst in microbial fuel cell cathodes. Energies, 15(1), 272. https://doi.org/10.3390/en15010272
Pan, P. & Bhattacharyya, N. (2023). Bioelectricity production from microbial fuel cell (MFC) using Lysinibacillus xylanilyticus strain nbpp1 as a biocatalyst. Current Microbiology, 80(8). https://doi.org/10.1007/s00284-023-03338-5
Pan, Q.-R., Li, N., Liu, Z.-Q., Lai, B.-L., Huang, L.-J. & Feng, Y.-N. (2022). Regulating the electronic structure of Cu-Nx active sites for efficient and durable oxygen reduction catalysis to improve microbial fuel cell performance. ACS Applied Materials & Interfaces, 15(1), 1234–1246. https://doi.org/10.1021/acsami.2c18876
Sawant, S. Y., Han, T. H. & Cho, M. H. (2016). Metal-free carbon-based materials: Promising electrocatalysts for oxygen reduction reaction in microbial fuel cells. International Journal of Molecular Sciences, 18(1), 25. https://doi.org/10.3390/ijms18010025
Scharf, J., Wallace, W. D. Z., Kübler, M., Paul, S. D., Ni, L., Gridin, V. & Kramm, U. I. (2022). Relation between half‐cell and fuel cell activity and stability of FeNC catalysts for the oxygen reduction reaction. SusMat, 2(5), 630–645. https://doi.org/10.1002/sus2.84
Soleimani, A., Heidari, M., Luo, Y., Khorrami, B. M. & Hosseini Dolatabadi, S. H. (2023). Hydrogen: An integral player in the future of sustainable transportation. A survey of fuel cell vehicle technologies, adoption patterns, and challenges. mdpi ag. https://doi.org/10.20944/preprints202310.0415.v1
Subhadarshini, S., Venkata Mohan, S., Sarkar, O., Jana, T., Roy, T. K. & Sravan, J. S. (2023). Sulfonated polybenzimidazole as a PEM in a microbial fuel cell: An efficient strategy for green energy generation and wastewater cleaning. ACS Applied Energy Materials, 6(3), 1422–1438. https://doi.org/10.1021/acsaem.2c03238
Tan, S.-M., Wong, Y.-S., Ong, S.-A., Teoh, T.-P., Thung, W.-E. & Ho, L.-N. (2020). The reaction of wastewater treatment and power generation of single chamber microbial fuel cell against substrate concentration and anode distributions. Journal of Environmental Health Science and Engineering, 18(2), 793–807. https://doi.org/10.1007/s40201-020-00504-w
Theofanidis, S. A., Detavernier, C., Longo, A., Galvita, V. V., Meledina, M., Poelman, H., Van Tendeloo, G., Marin, G. B. & Dharanipragada, N. V. R. A. (2018). Fe-containing magnesium aluminate support for stability and carbon control during methane reforming. ACS Catalysis, 8(7), 5983–5995. https://doi.org/10.1021/acscatal.8b01039
Tornheim, A. & O’Hanlon, D. C. (2020). What do coulombic efficiency and capacity retention truly measure? A deep dive into cyclable lithium inventory, limitation type, and redox side reactions. Journal of The Electrochemical Society, 167(11), 110520. https://doi.org/10.1149/1945-7111/ab9ee8
Wang, Y., Xing, J., Qian, J., Liu, L. & Li, J. (2023). Facile fabrication of nickel supported on reduced graphene oxide composite for oxygen reduction reaction. Nanomaterials, 13(24), 3087. https://doi.org/10.3390/nano13243087
Xie, H., Zhou, G., Jiao, Z., Du, Q., Li, H., Ren, J. & Chen, S. (2017). Catalytic combustion of volatile aromatic compounds over CuO-CeO2 catalyst. Korean Journal of Chemical Engineering, 34(7), 1944–1951. https://doi.org/10.1007/s11814-017-0111-4
Zhang, J., Li, F., Liu, W., Wang, Q., Li, X., Hung, S.-F., Yang, H. & Liu, B. (2024). Modulating spin of atomic manganese center for high-performance oxygen reduction reaction. Angewandte Chemie (International Ed. in English), 63(51). https://doi.org/10.1002/anie.202412245
Zhao, Y., Liu, J., Yu, G., Liao, L. & Wei, P. (2019). B‐Doped Fe/N/C Porous catalyst for high‐performance oxygen reduction in anion‐exchange membrane fuel cells. ChemElectroChem, 6(6), 1754–1760. https://doi.org/10.1002/celc.201801688
Zhong, G., Fu, X., Wang, F., Liu, L., Xu, S., Wang, H., Dou, J., Zheng, C. Z. & Liao, W. (2020). Effect of experimental operations on the limiting current density of oxygen reduction reaction evaluated by rotating‐disk electrode. ChemElectroChem, 7(5), 1107–1114. https://doi.org/10.1002/celc.201902085
Zhou, D., Sun, X., Xu, W., Kuang, Y., Mohammed‐Ibrahim, J., Jawaid, S., Liu, W. & Li, P. (2020). Recent advances in non-precious metal‐based electrodes for alkaline water electrolysis. ChemNanoMat, 6(3), 336–355. https://doi.org/10.1002/cnma.202000010
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Carbon supported Fe₇₀Co₂₀Ni₁₀ trimetallic catalyst for enhanced cathode performance in Dual-chamber microbial fuel cells for wastewater treatment. (2026). Journal of Applied and Natural Science, 18(1), 279-292. https://doi.org/10.31018/jans.v18i1.7091
