An Optimization of the Adsorption Method for Methylene Blue Using Faujasite Zeolite-X Synthesized from Coal-Fly Ash Utilizing RSM Coupled with Central Composite Design Approach

https://doi.org/10.22146/ijc.107596

Divya Tirva(1*), Dharmesh Sur(2)

(1) Department of Chemical Engineering, Faculty of Technology, Marwadi University, Rajkot, Gujarat 360003, India
(2) Department of Chemical Engineering, Faculty of Technology, Marwadi University, Rajkot, Gujarat 360003, India
(*) Corresponding Author

Abstract


The objective of the research was to evaluate the effectiveness of Faujasite zeolite-X, produced from coal fly ash, in removing methylene blue dye. The zeolite was synthesized using hydrothermal treatment, and its properties were analyzed using X-ray diffraction (XRD), scanning electron microscopy with energy-dispersive X-ray spectroscopy (SEM+EDAX), and Fourier-transform infrared spectroscopy (FTIR). Response surface methodology (RSM), employing a central composite design (CCD) was used to optimize the adsorption parameters. High-resolution XRD confirmed phase-pure, highly crystalline Faujasite zeolite-X, responsible for its superior adsorption ability. SEM shows conversion of amorphous coal fly ash to strongly crystalline Faujasite-type zeolite-X with sharp angular morphologies, confirming the process’s efficacy and its suitability for industrial use. Elimination of MB onto the synthesized adsorbent reached 99.23% at pH 9, contact time of 40 min at 55 °C, sorbent mass of 2.5 g/L, and an original dye concentration of 125 ppm. Unlike previous studies, this work integrates waste valorization with advanced statistical optimization to achieve superior dye removal efficiency. The optimized process not only develops the dye removal efficiency but also offers a green, scalable solution for coal fly ash utilization and textile sewage treatment, thereby addressing serious environmental issues and encouraging cleaner industrial performance.


Keywords


Faujasite zeolite-X; adsorption optimization; central composite design; response surface methodology; methylene blue dye



References

[1] Liu, Q., Zhao, Y., Wang, J., Zhou, Y., Liu, X., Hao, M., Chen, Z., Wang, S., Yang, H., and Wang, X., 2024, Application of single-atom-based photocatalysts in environmental pollutant removal and renewable energy production, Crit. Rev. Environ. Sci. Technol., 54 (12), 909–930.

[2] Mondal, P., Baksi, S., and Bose, D., 2017, Study of environmental issues in textile industries and recent wastewater treatment technology, World Sci. News, 61 (2), 98–109.

[3] Liu, X., Li, Y., Chen, Z., Yang, H., Wang, S., Tang, Z., and Wang, X., 2023, Recent progress of covalent organic frameworks membranes: Design, synthesis, and application in water treatment, Eco-Environ. Health, 2 (3), 117–130.

[4] Vezentsev, A.I., Thuy, D.M., Goldovskaya-Peristaya, L.F., and Glukhareva, N.A., 2018, Adsorption of methylene blue on the composite sorbent based on bentonite-like clay and hydroxyapatite, Indones. J. Chem., 18 (4), 733–741.

[5] Astuti, W., Chafidz, A., Wahyuni, E.T., Prasetya, A., Bendiyasa, I.M., and Abasaeed, A.E., 2019, Methyl violet dye removal using coal fly ash (CFA) as a dual sites adsorbent, J. Environ. Chem. Eng., 7 (5), 103262.

[6] Wang, S., Chen, Z., Cai, Y., Wu, X.L., Wang, S., Tang, Z., Hu, B., Li, Z., and Wang, X., 2023, Application of COFs in capture/conversion of CO2 and elimination of organic/inorganic pollutants, Environ. Funct. Mater., 2 (1), 76–92.

[7] Mustikaningrum, M., Cahyono, R.B., and Yuliansyah, A.T., 2022, Adsorption of methylene blue on nano-crystal cellulose of oil palm trunk: Kinetic and thermodynamic studies, Indones. J. Chem., 22 (4), 953–964.

[8] Ferreira, B.C.S., Teodoro, F.S., Mageste, A.B., Gil, L.F., de Freitas, R.P., and Gurgel, L.V.A., 2015, Application of a new carboxylate-functionalized sugarcane bagasse for adsorptive removal of crystal violet from aqueous solution: Kinetic, equilibrium and thermodynamic studies, Ind. Crops Prod., 65, 521–534.

[9] Musthofa, A.M.H., Syafila, M., and Helmy, Q., 2023, Effect of activated carbon particle size on methylene blue adsorption process in textile wastewater, Indones. J. Chem., 23 (2), 461–474.

[10] Iryani, A., Nur, H., Santoso, M., and Hartanto, D., 2020, Adsorption study of rhodamine B and methylene blue dyes with ZSM-5 directly synthesized from Bangka kaolin without organic template, Indones. J. Chem., 20 (1), 130–140.

[11] Yousuf, A., Manzoor, S.O., Youssouf, M., Malik, Z.A., and Khawaja, K.S., 2020, Fly ash: Production and utilization in India-an overview, J. Mater. Environ. Sci., 11 (6), 911–921.

[12] Ahmed, S., Saurikhia, A., Haleem, A., and Gangopadhyay, S., 2016, Geographical spread of fly ash generation and residual potential for its utilization in India, Int. J. Innovative Res. Rev., 4 (1), 8–19.

[13] Alam, J., and Akhtar, M., 2011, Fly ash utilization in different sectors in Indian scenario, Int. J. Emerg. Trends Eng. Dev., 1 (1), 1–14.

[14] Lin, C.F., and Hsi, H.C., 1995, Resource recovery of waste fly ash: Synthesis of zeolite-like materials, Environ. Sci. Technol., 29 (4), 1109–1117.

[15] Ojha, K., Pradhan, N.C., and Samanta, A.N., 2004, Zeolite from fly ash: Synthesis and characterization, Bull. Mater. Sci., 27 (6), 555–564.

[16] Iqbal, A., Sattar, H., Haider, R., and Munir, S., 2019, Synthesis and characterization of pure phase zeolite 4A from coal fly ash, J. Cleaner Prod., 219, 258–267.

[17] Xie, J., Wang, Z., Wu, D., and Kong, H., 2014, Synthesis and properties of zeolite/hydrated iron oxide composite from coal fly ash as efficient adsorbent to simultaneously retain cationic and anionic pollutants from water, Fuel, 116, 71–76.

[18] Sivalingam, S., and Sen, S., 2018, Optimization of synthesis parameters and characterization of coal fly ash derived microporous zeolite X, Appl. Surf. Sci., 455, 903–910.

[19] Phuong, N.T.T., Minh, C.H., Lam, H.H., Duong, N.T.H., and Nguyen, L.Q., 2023, An ultrafast and green synthesis of mesoporous zeolite X for great enhancement in methylene blue adsorption, Adv. Sci. Technol., 122, 49–55.

[20] Hadda Aya, H., Djamel, N., Samira, A., Otero, M., and Ali Khan, M., 2024, Optimizing methylene blue adsorption conditions on hydrothermally synthesized NaX zeolite through a full two-level factorial design, RSC Adv., 14 (33), 23816–23827.

[21] Bonetti, B., Waldow, E.C., Trapp, G., Hammercshmitt, M.E., Ferrarini, S.F., Pires, M.J., Estevam, S.T., and Aquino, T.F.D., 2021, Production of zeolitic materials in pilot scale based on coal ash for phosphate and potassium adsorption in order to obtain fertilizer, Environ. Sci. Pollut. Res., 28 (3), 2638–2654.

[22] Zhou, C., Gao, Q., Luo, W., Zhou, Q., Wang, H., Yan, C., and Duan, P., 2015, Preparation, characterization and adsorption evaluation of spherical mesoporous Al-MCM-41 from coal fly ash, J. Taiwan Inst. Chem. Eng., 52, 147–157.

[23] Sudha, G., Subramanian, E., and Murugan, C., 2015, Development of iron oxide/zeo-NaX nano photocatalyst from coal fly ash and its activity assessment by methylene blue dye degradation, Int. Res. J. Nat. Appl. Sci., 2 (2), 114–128.

[24] Kim, H.J., Joshi, M.K., Pant, H.R., Kim, J.H., Lee, E., and Kim, C.S., 2015, One-pot hydrothermal synthesis of multifunctional Ag/ZnO/fly ash nanocomposite, Colloids Surf., A, 469, 256–262.

[25] Lin, L., Lin, Y., Li, C., Wu, D., and Kong, H., 2016, Synthesis of zeolite/hydrous metal oxide composites from coal fly ash as efficient adsorbents for removal of methylene blue from water, Int. J. Miner. Process., 148, 32–40.

[26] Fungaro, D.A., Grosche, L.C., Pinheiro, A., Izidoro, J.C., and Borrely, S.I., 2011, Adsorption of methylene blue from aqueous solution on zeolitic material for color and toxicity removal, Orbital: Electron. J. Chem., 2 (3), 235–47.

[27] Borhade, A.V., Kshirsagar, T.A., and Dholi, A.G., 2017, Eco-friendly synthesis of aluminosilicate bromo sodalite from waste coal fly ash for the removal of copper and methylene blue dye, Arabian J. Sci. Eng., 42 (10), 4479–4491.

[28] Saud, P.S., Pant, B., Park, M., Chae, S.H., Park, S.J., Ei-Newehy, M., Al-Deyab, S.S., and Kim, H.Y., 2015, Preparation and photocatalytic activity of fly ash incorporated TiO2 nanofibers for effective removal of organic pollutants, Ceram. Int., 41 (1, Pt. B), 1771–1777.

[29] Al-dahri, T., AbdulRazak, A.A., and Rohani, S., 2022, Preparation and characterization of Linde-type A zeolite (LTA) from coal fly ash by microwave-assisted synthesis method: Its application as adsorbent for removal of anionic dyes, Int. J. Coal Prep. Util., 42 (7), 2064–2077.

[30] Cunico, P., Kumar, A., and Fungaro, D.A., 2015, Adsorption of dyes from simulated textile wastewater onto modified nanozeolite from coal fly ash, J. Nanosci. Nanoeng., 1 (3), 148–161.

[31] Sivalingam, S., and Sen, S., 2019, Efficient removal of textile dye using nanosized fly ash derived zeolite-X: Kinetics and process optimization study, J. Taiwan Inst. Chem. Eng., 96, 305–314.

[32] Gross-Lorgouilloux, M., Soulard, M., Caullet, P., Patarin, J., Moleiro, E., and Saude, I., 2010, Conversion of coal fly ashes into Faujasite under soft temperature and pressure conditions: Influence of additional silica, Microporous Mesoporous Mater., 127 (1-2), 41–49.

[33] Narimani, M., Gonbadi, M., and Zerafat, M.M., 2025, Methylene blue adsorption on Y-zeolite as a nano-porous adsorbent: Equilibrium and kinetic studies, Int. J. Environ. Anal. Chem., 17 (105, 5369–5389.

[34] Kunecki, P., Panek, R., Wdowin, M., and Franus, W., 2017, Synthesis of faujasite (FAU) and tschernichite (LTA) type zeolites as a potential direction of the development of lime Class C fly ash, Int. J. Miner. Process, 166, 69–78.

[35] Parra-Huertas, R.A., Calderón-Carvajal, C.O., Gómez-Cuaspud, J.A., and Vera-López, E., 2023, Synthesis and characterization of Faujasite-Na from fly ash by the fusion-hydrothermal method, Bol. Soc. Esp. Ceram. Vidrio, 62 (6), 527–542.

[36] Shi, L., Wang, Q., Zhao, X., Che, Y., Liu, H., Zuo, W., and Zhang, Y., 2023, The methyl blue adsorption performance and mechanism of NaX zeolite synthesized from Huadian oil shale ash, J. Taiwan Inst. Chem. Eng., 147, 104904.

[37] Ramezani, H., Azizi, S.N., and Cravotto, G., 2019, Improved removal of methylene blue on modified hierarchical zeolite Y: Achieved by a “destructive-constructive” method, Green Process. Synth., 8 (1), 730–741.

[38] Amodu, O.S., Ojumu, T.V., Ntwampe, S.K., and Ayanda, O.S., 2015, Rapid adsorption of crystal violet onto magnetic zeolite synthesized from fly ash and magnetite nanoparticles, J. Encapsulation Adsorpt. Sci., 5 (4), 191–203.

[39] Pal, D., and Sen, S., 2024 Optimal synthesis of dolochar derived faujasite zeolite X for highly effective Cd(II) removal, Environ. Res., 240, 117494.

[40] Naskar, J., and Sharma, A.K., 2025 Resource and recycling: A comprehensive review of India’s coal landscape, characterization, and the current to future potential of fly ash from thermal power plants, Int. J. Coal Prep. Util., 45 (11), 2472–2522.

[41] Yoldi, M., Fuentes-Ordoñez, E.G., Korili, S.A., and Gil, A., 2019 Zeolite synthesis from industrial wastes, Microporous Mesoporous Mater., 287, 183–191.

[42] Tirva, D., Palkar, R.R., and Agheda, K., 2023, An optimization of synthesis technique for Na-X zeolite from coal-fly ash using Taguchi experimental design, Chem. Pap., 77 (9), 5143–5153.

[43] Makgabutlane, B., Nthunya, L.N., Nxumalo, E.N., Musyoka, N.M., and Mhlanga, S.D., 2020, Microwave irradiation-assisted synthesis of zeolites from coal fly ash: An optimization study for a sustainable and efficient production process, ACS Omega, 5 (39), 25000–25008.

[44] Park S., 1996, Robust Design and Analysis for Quality Engineering, Springer New York, NY, US.

[45] Boycheva, S., Marinov, I., Miteva, S., and Zgureva, D., 2020, Conversion of coal fly ash into nanozeolite Na-X by applying ultrasound assisted hydrothermal and fusion-hydrothermal alkaline activation, Sustainable Chem. Pharm., 15, 100217.

[46] Xiao, M., Hu, X., Gong, Y., Gao, D., Zhang, P., Liu, Q., Liu, Y., and Wang, M., 2015, Solid transformation synthesis of zeolites from fly ash, RSC Adv., 5 (122), 100743–100749.

[47] Wang, Y., Lv, T., Ma, Y., Tian, F., Shi, L., Liu, X., and Meng, C., 2016, Synthesis and characterization of zeolite L prepared from hydrothermal conversion of magadiite, Microporous Mesoporous Mater., 228, 86–93.

[48] Deng, L., Xu, Q., and Wu, H., 2016, Synthesis of zeolite-like material by hydrothermal and fusion methods using municipal solid waste fly ash, Procedia Environ. Sci., 31, 662–667.

[49] Pathak, C.Y., Roy, D., and Das, S., 2014, Utilization of fly ash byproduct in synthetic zeolites, World J. Civ. Eng. Constr. Technol., 1 (1), 2–11.

[50] Nawagamuwa, U.P., and Wijesooriya, N., 2018, Use of flyash to improve soil properties of drinking water treatment sludge, Int. J. Geo-Eng., 9 (1), 1–8.

[51] Ghaedi, M., Ansari, A., Habibi, M.H., and Asghari, A.R., 2014, Removal of malachite green from aqueous solution by zinc oxide nanoparticle loaded on activated carbon: Kinetics and isotherm study, J. Ind. Eng. Chem., 20 (1), 17–28.

[52] Gollakota, A.R.K., Volli, V., Munagapati, V.S., Wen J.C., and Shu C.M., 2020, Synthesis of novel ZSM-22 zeolite from Taiwanese coal fly ash for the selective separation of rhodamine 6G, J. Mater. Res. Technol., 9 (6), 15381–15393.

[53] Sun, Z., Li, C., and Wu, D., 2010, Removal of methylene blue from aqueous solution by adsorption onto zeolite synthesized from coal fly ash and its thermal regeneration, J. Chem. Technol. Biotechnol., 85 (6), 845–850.

[54] Ho, K.Y., McKay, G., and Yeung, K.L., 2003, Selective adsorbents from ordered mesoporous silica, Langmuir, 19 (7), 3019–3024.

[55] Lin, J.X., Zhan, S.L., Fang, M.H., Qian, X.Q., and Yang, H., 2008, Adsorption of basic dye from aqueous solution onto fly ash, J. Environ. Manage., 87 (1), 193–200.

[56] Angaru, G.K.R., Choi, Y.L., Lingamdinne, L.P., Koduru, J.R., Yang, J.K., Chang, Y.Y., and Karri, R.R., 2022, Portable SA/CMC entrapped bimetallic magnetic fly ash zeolite spheres for heavy metals contaminated industrial effluents treatment via batch and column studies, Sci. Rep., 12 (1), 3430.

[57] de Klerk, A., 2018, Zeolites as catalysts for fuels refining after indirect liquefaction processes, Molecules, 23 (1), 115.

[58] Yuan, N., Gong, X., Sun, W., and Yu, C., 2021, Advanced applications of Zr-based MOFs in the removal of water pollutants, Chemosphere, 267, 128863.

[59] Grozdov, D., and Zinicovscaia, I., 2023, Mesoporous materials for metal-laden wastewater treatment, Materials, 16 (17), 5864.

[60] Hölderich, W., Hesse, M., and Näumann, F., 1988, Zeolites: Catalysts for organic syntheses, Angew. Chem., Int. Ed. Engl., 27 (2), 226–246.

[61] Zhang, Z., Zhang, Z., Fernández, Y., Menéndez, J.A., Niu, H., Peng, J., Zhang, L., and Guo, S., 2010, Adsorption isotherms and kinetics of methylene blue on a low-cost adsorbent recovered from a spent catalyst of vinyl acetate synthesis, Appl. Surf. Sci., 256 (8), 2569–2576.

[62] Kumar, S., Upadhyay, S.N., and Upadhya, Y.D., 1987, Removal of phenols by adsorption on fly ash, J. Chem. Technol. Biotechnol., 37 (4), 281–290.

[63] Kumar, V., Anandakumar, R., and Mathur, M., 2003, Management of fly ash in India: A perspective, The 3rd International Conference, Fly Ash Utilisation and Disposal, New Delhi, India, 19–12 February 2003, I.1–I.26.

[64] Ndlovu, N.Z.N., Missengue, R.N.M., Petrik, L.F., and Ojumu, T., 2017, Synthesis and characterization of Faujasite zeolite and geopolymer from South African coal fly ash, J. Environ. Eng., 143 (9), 04017042.

[65] Ndlovu, N.Z.N., Ameh, A.E., Petrik, L.F., and Ojumu, T.V., 2023, Synthesis and characterisation of pure phase ZSM-5 and sodalite zeolites from coal fly ash, Mater. Today Commun., 34, 105436.

[66] Daulay, A., Astuti, W., Sumardi, S., Mufakhir, F.R., Supriyatna, Y.I., Haryono, T., and Samada, L.H., 2025, Synthesis and characteristics of Na-A zeolite from coal fly ash and application for adsorption of cerium(III), J. Rare Earths, 43 (1), 171–179.

[67] Mohd Nasir, M.Z., Indiran, G., and Ahmad Zaini, M.A., 2021 Assessment of thermal regeneration of spent commercial activated carbon for methylene blue dye removal, Part. Sci. Technol., 39 (4), 504–510.

[68] Wang, S., and Zhu, Z.H., 2006, Characterisation and environmental application of an Australian natural zeolite for basic dye removal from aqueous solution, J. Hazard. Mater., 136 (3), 946–952.

[69] Cui, M., Mu, Y., Zhang, S., Wang, L., and Meng, C., 2018, Mechanistic study on the synthesis of ZSM-5 from a layered silicate magadiite, Microporous Mesoporous Mater., 265, 63–69.



DOI: https://doi.org/10.22146/ijc.107596

Article Metrics

Abstract views : 115 | views : 53 | views : 22


Copyright (c) 2025 Indonesian Journal of Chemistry

Creative Commons License
This work is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License.

 


Indonesian Journal of Chemistry (ISSN 1411-9420 /e-ISSN 2460-1578) - Chemistry Department, Universitas Gadjah Mada, Indonesia.

Web
Analytics View The Statistics of Indones. J. Chem.