Coal fly ash is converted into a MnFe2O4/NaA composite for sustainable wastewater treatment.
The material removes ammonium (NH4+-N) and degrades tetracycline simultaneously.
Adsorption and photocatalysis work together to enhance pollutant removal efficiency.
The composite shows strong stability and can be reused multiple times.
This approach supports circular economy by turning waste into high-value materials.
| [1] | Li C., Awasthi M.K., Liu J., et al. (2025). Veterinary tetracycline residues: Environmental occurrence, ecotoxicity, and degradation mechanism. Environ. Res. 266:120417. DOI:10.1016/j.envres.2024.120417 |
| [2] | Yang K., Yue Q., Kong J., et al. (2016). Microbial diversity in combined UAF–UBAF system with novel sludge and coal cinder ceramic fillers for tetracycline wastewater treatment. Chem. Eng. J. 285:319. DOI:10.1016/j.cej.2015.10.019 |
| [3] | Zhang H., Cheng S., Li B., et al. (2018). Fabrication of magnetic Co/BiFeO3 composite and its advanced treatment of pharmaceutical wastewater by activation of peroxysulphate. Sep. Purif. Technol. 202:242. DOI:10.1016/j.seppur.2018.03.072 |
| [4] | Daghrir R. and Drogui P. (2013). Tetracycline antibiotics in the environment: a review. Environ. Chem. Lett. 11:209−227. DOI:10.1007/s10311-013-0404-8 |
| [5] | Liu H., Yang L., Chen H., et al. (2023). Preparation of floating BiOCl0.6I0.4/ZnO photocatalyst and its inactivation of Microcystis aeruginosa under visible light. J. Environ. Sci. 125:362. DOI:10.1016/j.jes.2021.12.044. |
| [6] | Zhang X., Li C., Chen T., et al. (2021). Enhanced visible-light-assisted peroxymonosulfate activation over MnFe2O4 modified g-C3N4/diatomite composite for bisphenol A degradation. Int. J. Min. Sci. Technol. 31:1169. DOI:10.1016/j.ijmst.2021.11.008 |
| [7] | Verraes C., Van Boxstael S., Van Meervenne E., et al. (2013). Antimicrobial resistance in the food chain: A review. Int. J. Environ. Res. Public Health 10:2643−2670. DOI:10.3390/ijerph10072643 |
| [8] | Kazmi R. and Chakraborty M. (2025). Use of coal mining wastes in the construction industry to promote a circular economy: a systematic literature review. Circ. Econ. Sustain. 5:3593. DOI:10.1007/s43615-025-00551-1 |
| [9] | Fernández-Pereira C., Leiva C., Luna-Galiano Y., et al. (2024). Improved recycling of a gasification fly ash: An integrated waste management approach within the framework of a circular economy. Waste Manag. 187:31. DOI:10.1016/j.wasman.2024.06.029 |
| [10] | Tang D., Pal M., Meng T., et al. (2025). Synthesis and applications of magnetic zeolites: A comprehensive review. J. Supercond. Nov. Magn. 38. DOI:10.1007/s10948-025-06986-9. |
| [11] | Liu G., Lin Y., Zhang L., et al. (2024). Preparation of NaA zeolite molecular sieve based on solid waste fly ash by high-speed dispersion homogenization-assisted alkali fusion-hydrothermal method and its performance of ammonia-nitrogen adsorption. J. Sci.: Adv. Mater. Devices 9:100673. DOI:10.1016/j.jsamd.2024.100673 |
| [12] | Jankowska A., Panek R., Franus W., et al. (2024). Tailoring natural and fly ash-based zeolites surfaces for efficient 2,4-D herbicide adsorption: The role of hexadecyltrimethylammonium bromide modification. Molecules 29. DOI:10.3390/molecules29225244. |
| [13] | Reed J.L.A., James A., Carey T., et al. (2024). Engineered species-selective ion-exchange in tuneable dual-phase zeolite composites. Chem. Sci. 15:13699. DOI:10.1039/d4sc02664k |
| [14] | Munir N., Javaid A., Abideen Z., et al. (2023). The potential of zeolite nanocomposites in removing microplastics, ammonia, and trace metals from wastewater and their role in phytoremediation. Environ. Sci. Pollut. Res. 31:1695. DOI:10.1007/s11356-023-31185-1 |
| [15] | Wahba M.A. and Khaled R.K. (2025). V/Zn incorporated-MCM-41: Synthesis, characterization and visible light photocatalytic activity for tetracycline degradation. J. Inorg. Organomet. Polym. Mater. 35:4445. DOI:10.1007/s10904-024-03533-2 |
| [16] | Huang Kong E.D., Lai C.W., Juan J.C., et al. (2025). Recent advances in titanium dioxide bio-derived carbon photocatalysts for organic pollutant degradation in wastewater. iScience 28. DOI:10.1016/j.isci.2025.112368. |
| [17] | Li J., Li Y., Xiong Z., et al. (2019). The electrochemical advanced oxidation processes coupling of oxidants for organic pollutants degradation: a mini-review. Chin. Chem. Lett. 30:2139. DOI:10.1016/j.cclet.2019.04.057 |
| [18] | Sawunyama L., Oyewo O.A., Makgato S.S., et al. (2025). TiO2–ZnO functionalized low-cost ceramic membranes from coal fly ash for the removal of tetracycline from water under visible light. Discover Nano 20. DOI:10.1186/s11671-024-04178-3. |
| [19] | Shi J., Zhang M., Zhu L., et al. (2025). Recent advances in sustainable synthesis of zeolites. Mater. Today Sustain. 29:101065. DOI:10.1016/j.mtsust.2024.101065 |
| [20] | Zhou X., Liu S., Hu Y., et al. (2024). Green synthesis of porous bamboo-based activated carbon with high VOCs adsorption performance via steam activation method. J. Porous Mater. 31:737. DOI:10.1007/s10934-024-01557-0 |
| [21] | Bissenova M., Idrissov N., Kuspanov Z., et al. (2025). Hybrid adsorption–photocatalysis composites: a sustainable route for efficient water purification. Mater. Renew. Sustain. Energy 14:44. DOI:10.1007/s40243-025-00319-5 |
| [22] | Jiang Q., He J., Wang Y., et al. (2024). Efficient removal of ammonia–nitrogen in wastewater by zeolite molecular sieves prepared from coal fly ash. Sci. Rep. 14. DOI:10.1038/s41598-024-72067-x. |
| [23] | Jalloul G., Hijazi N., Boyadjian C., et al. (2024). Titania-zeolite composite for tetracycline photocatalytic degradation under visible light: A comparison between doping and ion exchange. Heliyon 10:e31854. DOI:10.1016/j.heliyon.2024.e31854 |
| [24] | Bissenova M., Idrissov N., Kuspanov Z., et al. (2025). Hybrid adsorption–photocatalysis composites: a sustainable route for efficient water purification. Mater. Renew. Sustain. Energy 14. DOI:10.1007/s40243-025-00319-5. |
| [25] | Liu Y., Wang L., Dai X., et al. (2024). Research on the adsorption-photocatalytic synergistic degradation of tetracycline by Au nanoparticles/TiO2 nanorods/biochar. J. Alloys Compd. 976:172985. DOI:10.1016/j.jallcom.2023.172985 |
| [26] | Ramu S., Kainthla I., Chandrappa L., et al. (2023). Recent advances in metal organic frameworks–based magnetic nanomaterials for waste water treatment. Environ. Sci. Pollut. Res. 31:167. DOI:10.1007/s11356-023-31162-8 |
| [27] | Derkaoui K., Bencherifa I., Elfiad A., et al. (2025). Unveiling the optical and dielectric properties of MnFe2O4: A high-performance visible-light photocatalyst for sustainable Rhodamine B degradation. J. Electron. Mater. 54:5271. DOI:10.1007/s11664-025-11991-8 |
| [28] | Tang D., Pal M., Meng T., et al. (2025). Synthesis and applications of magnetic zeolites: A comprehensive review. J. Supercond. Nov. Magn. 38:146. DOI:10.1007/s10948-025-06986-9 |
| [29] | Zhang T., Zhou T., He L., et al. (2020). Oxidative degradation of Rhodamine B by Ag@CuO nanocomposite activated persulfate. Synth. Met. 267:116479. DOI:10.1016/j.synthmet.2020.116479 |
| [30] | Wang Z., Lai C., Qin L., et al. (2020). ZIF-8-modified MnFe2O4 with high crystallinity and superior photo-Fenton catalytic activity by Zn-O-Fe structure for TC degradation. Chem. Eng. J. 392:124851. DOI:10.1016/j.cej.2020.124851 |
| [31] | Zhao W. and Yang B. (2024). Fabrication of magnetic MnFe2O4@HL composites with an in situ Fenton-like reaction for enhancing tetracycline degradation. J. Colloid Interface Sci. 658:997. DOI:10.1016/j.jcis.2023.12.067 |
| [32] | Jun B.-M., Elanchezhiyan S.S., Yoon Y., et al. (2020). Accelerated photocatalytic degradation of organic pollutants over carbonate-rich lanthanum-substituted zinc spinel ferrite assembled reduced graphene oxide by ultraviolet (UV)-activated persulfate. Chem. Eng. J. 393:124733. DOI:10.1016/j.cej.2020.124733 |
| [33] | Ghosh M., Akbar A. and Lakshmi M.B. (2024). Harnessing spinel ferrites: A comprehensive review of their role in water treatment. ChemRxiv. DOI:10.26434/chemrxiv-2024-hq04v. |
| [34] | Richard A.M., Tao D., Leclair C.A., et al. (2024). Analytical quality evaluation of the Tox21 compound library. Chem. Res. Toxicol. 38:15. DOI:10.1021/acs.chemrestox.4c00330 |
| [35] | Zheng A.L.T., Teo E.Y.L., Seenivasagam S., et al. (2024). Recent review on porous adsorbents for water decontamination: strategies for enhanced removal of tetracycline. J. Porous Mater. 32:1. DOI:10.1007/s10934-024-01699-1 |
| [36] | Liu G., Lin Y., Zhang L., et al. (2024). Preparation of NaA zeolite molecular sieve based on solid waste fly ash by high-speed dispersion homogenization-assisted alkali fusion-hydrothermal method and its performance of ammonia-nitrogen adsorption. J. Sci. Adv. Mater. Devices 9:100673. DOI:10.1016/j.jsamd.2024.100673 |
| [37] | Jiang X., Zhou Q. and Lian Y. (2023). Efficient photocatalytic degradation of tetracycline on the MnFe2O4/BGA composite under visible light. Int. J. Mol. Sci. 24. DOI:10.3390/ijms24119378. |
| [38] | Shi J., Zhang M., Zhu L., et al. (2025). Recent advances in sustainable synthesis of zeolites. Mater. Today Sustain. 29:101065. DOI:10.1016/j.mtsust.2024.101065 |
| [39] | Jiang Q., He J., Wang Y., et al. (2024). Efficient removal of ammonia–nitrogen in wastewater by zeolite molecular sieves prepared from coal fly ash. Sci. Rep. 14:21064. DOI:10.1038/s41598-024-72067-x |
| [40] | Lu A.-H., Salabas E.L. and Schüth F. (2007). Magnetic nanoparticles: Synthesis, protection, functionalization, and application. Angew. Chem. Int. Ed. 46:1222−1244. DOI:10.1002/anie.200602866 |
| [41] | Reddy L.H., Arias J.L., Nicolas J., et al. (2012). Magnetic nanoparticles: Design and characterization, toxicity and biocompatibility, pharmaceutical and biomedical applications. Chem. Rev. 112:5818−5878. DOI:10.1021/cr300068p |
| [42] | Mohapatra J., Mitra A., Bahadur D., et al. (2013). Surface controlled synthesis of MFe2O4 (M = Mn, Fe, Co, Ni and Zn) nanoparticles and their magnetic characteristics. Cryst. Eng. Comm. 15:524−532. DOI:10.1039/c2ce25957e |
| [43] | Cao K.L.A., Rahmatika A.M., Kitamoto Y., et al. (2021). Controllable synthesis of spherical carbon particles transition from dense to hollow structure derived from Kraft lignin. J. Colloid Interface Sci. 589:252. DOI:10.1016/j.jcis.2020.12.077 |
| [44] | Wang Z., Chen Q., Zhang J., et al. (2019). Characterization and source identification of tetracycline antibiotics in the drinking water sources of the lower Yangtze River. J. Environ. Manage. 244:13. DOI:10.1016/j.jenvman.2019.04.070 |
| [45] | Subasi B.S., Hayri-Senel T., Kahraman E., et al. (2025). Photocatalytic degradation of tetracycline from aqueous solution with graphene oxide and hydroxyapatite composites. Sci. Rep. 15. DOI:10.1038/s41598-025-11502-z. |
| [46] | Zolekafeli Z., Sateria S.F., Mohamed A.H., et al. (2024). Removal of tetracycline using tungsten disulfide/graphene oxide as photocatalyst: Effect of light irradiation and kinetic studies. Bull. Chem. React. Eng. Catal. 19:512. DOI:10.9767/bcrec.20204 |
| [47] | Kong Y., Zhuang Y., Han K., et al. (2020). Enhanced tetracycline adsorption using alginate-graphene-ZIF67 aerogel. Colloids Surf. A Physicochem. Eng. Asp. 588:124360. DOI:10.1016/j.colsurfa.2019.124360 |
| [48] | Sawunyama L., Oyewo O.A., Makgato S.S., et al. (2025). TiO2–ZnO functionalized low-cost ceramic membranes from coal fly ash for the removal of tetracycline from water under visible light. Discover Nano 20:1. DOI:10.1186/s11671-024-04178-3 |
| [49] | Nguyen H.A., Phuong N.T.T., Tran N.B., et al. (2025). Nano-enhanced Fenton/Fenton-like chemistry: integrating peroxidase nanozymes, MOFs, and MXenes for next-generation colorimetric biosensors. Nanoscale Adv. 7:4763. DOI:10.1039/d5na00387c |
| [50] | Singh A., Pratap S.G. and Raj A. (2024). Occurrence and dissemination of antibiotics and antibiotic resistance in aquatic environment and its ecological implications: a review. Environ. Sci. Pollut. Res. 31:47505. DOI:10.1007/s11356-024-34355-x |
| Song Y., Xu B., Bao X., et al. (2026). Sustainable synthesis of NaA zeolite-modified MnFe2O4 for synergistic removal of NH4+ and tetracycline. The Innovation Energy 3:100151. https://doi.org/10.59717/j.xinn-energy.2026.100151 |
To request copyright permission to republish or share portions of our works, please visit Copyright Clearance Center's (CCC) Marketplace website at marketplace.copyright.com.
Flow chart for the preparation of MnFe2O4/NaA molecular sieves
(A) XRD patterns of NaA, MnFe2O4 and 8% MnFe2O4/NaA; (B) VSM spectrum of 8% MnFe2O4/NaA
(A) SEM images of MnFe2O4; (B) NaA; (C) 8% MnFe2O4/NaA; (D) 8% MnFe2O4/NaA (used after 4 cycles )
XPS analysis of MnFe2O4 and 8% MnFe2O4/NaA
Curves of MnFe2O4, NaA and 8% MnFe2O4
8%MnFe2O4/NaA on the performance of photocatalytic degradation of TC
(A) ROS quenching tests and (B) Removal performance of ammonia nitrogen and TC by 8% MnFe2O4/NaA after chemical regeneration (25 °C, pH=7.00, 75min, 50 mM H2O2, 20 mg·L−1 MnFe2O4/NaA)