Surface Hydrophobization Via CTAB Functionalization as a Strategy for Enhancing Geopolymer Adsorption Capacity: Synthesis, Characterization, and Carbamazepine Removal Performance in Simulated Pharmaceutical Effluent"
Authors
Department of Environmental Science and Engineering, Guangdong Technion -Israel Institute of Technology, 214 Daxue Road, Shantou (China)
Article Information
Publication Timeline
Submitted: 2026-06-18
Accepted: 2026-06-23
Published: 2026-07-10
Abstract
Pharmaceutical active compounds (PACs) in wastewater pose a persistent environmental and public health threat due to their resistance to conventional treatment processes. Among these, carbamazepine (CBZ), a widely prescribed anticonvulsant, is frequently detected in effluents and surface waters at concentrations that disrupt aquatic ecosystems and potentiate antibiotic resistance. This study reports the synthesis, characterization, and adsorption performance of a cetyltrimethylammonium bromide (CTAB)-modified clay geopolymer composite (CTAB-BclayGeo) designed for targeted CBZ removal from aqueous media compared to an unmodified Clay Geopolymer (B-clayGeo). The composite was synthesized by alkaline activation of clay in the presence of a set CTAB concentration, followed by curing under controlled conditions. Physicochemical characterization was conducted using X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), scanning electron microscopy with energy-dispersive X-ray analysis (SEM/EDS) and Brunauer–Emmett–Teller (BET) surface area analysis. CTAB modification significantly increased the specific surface area from 27.28 m²/g (unmodified) to 67.16 m²/g, introduced hydrophobic organo-functional sites on the geopolymer surface, and enhanced mesopore accessibility for organic contaminant uptake. Batch adsorption experiments demonstrated that CTAB-ClayGeo achieved a maximum CBZ removal efficiency of 69.16% under optimized conditions (pH 8, contact time 24hrs, adsorbent dose 0.1 g/L). Adsorption kinetics followed the pseudo-second-order model, and equilibrium data were best described by the Langmuir isotherm, with a maximum monolayer adsorption capacity (qmax) of 58.2 mg/g. The adsorption mechanism is attributed to hydrophobic partitioning, π–π electron donor–acceptor interactions, and electrostatic attraction between CBZ and the organo-modified geopolymer surface.
Keywords
geopolymer; CTAB; surface modification; carbamazepine adsorption; wastewater treatment
Downloads
References
1. Abbou, B., Lebkiri, I., Ouaddari, H., El Amri, A., Achibat, F. E., Kadiri, L., . . . Rifi, E. H. (2023). Improved removal of methyl orange dye by adsorption using modified clay: combined experimental study using surface response methodology. Inorganic Chemistry Communications, 155, 111127. [Google Scholar] [Crossref]
2. Açışlı, Ö., Acar, İ., & Khataee, A. (2022). Preparation of a surface-modified fly ash-based geopolymer for the removal of an anionic dye: Parameters and adsorption mechanism. Chemosphere, 295, 133870. [Google Scholar] [Crossref]
3. Aghababaei, A., Azargohar, R., Dalai, A. K., Soltan, J., & Niu, C. H. (2022). Adsorption of carbamazepine from water by hydrothermally and steam-activated agricultural by-products: equilibrium, site energy, and thermodynamic studies. Chemical Engineering Communications, 209(6), 852-867. [Google Scholar] [Crossref]
4. Ahmad, F. A. (2023). The use of agro-waste-based adsorbents as sustainable, renewable, and low-cost alternatives for the removal of ibuprofen and carbamazepine from water. Heliyon, 9(6). [Google Scholar] [Crossref]
5. Al Qarni, H., Collier, P., O’Keeffe, J., & Akunna, J. (2016). Investigating the removal of some pharmaceutical compounds in hospital wastewater treatment plants operating in Saudi Arabia. Environmental Science and Pollution Research, 23(13), 13003-13014. [Google Scholar] [Crossref]
6. Alsubih, M., El Morabet, R., Khan, R. A., Khan, N. A., Khan, A. R., Khan, S., . . . Yousefi, M. (2022). Performance evaluation of constructed wetland for removal of pharmaceutical compounds from hospital wastewater: Seasonal perspective. Arabian Journal of Chemistry, 15(12), 104344. [Google Scholar] [Crossref]
7. Alver, A., Yılmaz, B. A., Bilican, B. K., Baştürk, E., Kaya, M., & Işık, M. (2024). Carbamazepine adsorption onto giant macroporous silica and adaptive neuro-fuzzy inference system modeling. Arabian Journal for Science and Engineering, 49(6), 8509-8524. [Google Scholar] [Crossref]
8. Carrio, J. A., Donato, R. K., Carvalho, A., Koon, G. K., Donato, K. Z., Yau, X. H., . . . Joy, J. (2025). From 2D kaolinite to 3D amorphous cement. Scientific reports, 15(1), 1669. [Google Scholar] [Crossref]
9. Davidovits, J. (2015). False values on CO2 emission for geopolymer cement/concrete published in scientific papers. Technical paper, 24, 1-9. [Google Scholar] [Crossref]
10. Duan, J., Chen, B., Zhang, Y., Cai, P., & Wang, F. (2024). Enhanced adsorption of Cr (VI) from aqueous solutions by CTAB-modified schwertmannite: Adsorption performance and mechanism. Chemical Engineering Research and Design, 208, 464-474. [Google Scholar] [Crossref]
11. Ekpeghere, K. I., Sim, W.-J., Lee, H.-J., & Oh, J.-E. (2018). Occurrence and distribution of carbamazepine, nicotine, estrogenic compounds, and their transformation products in wastewater from various treatment plants and the aquatic environment. Science of the total environment, 640, 1015-1023. [Google Scholar] [Crossref]
12. El-Bery, H. M., Saleh, M., El-Gendy, R. A., Saleh, M. R., & Thabet, S. M. (2022). High adsorption capacity of phenol and methylene blue using activated carbon derived from lignocellulosic agriculture wastes. Scientific reports, 12(1), 5499. [Google Scholar] [Crossref]
13. Fang, Y., Yang, L., Rao, F., Zhang, K., Qin, Z., Song, Z., & Na, Z. (2024). Behaviors and mechanisms of adsorption of MB and Cr (VI) by geopolymer microspheres under single and binary systems. Molecules, 29(7), 1560. [Google Scholar] [Crossref]
14. Gurav, P. P., Ray, S., Datta, S., Choudhari, P., & Hartmann, C. (2024). Role of clay cation exchange capacity, location of charge, and clay mineralogy on potassium availability in Indian Vertisols. Clays and Clay Minerals, 72, e3. [Google Scholar] [Crossref]
15. Hiba, Z., Mondamert, L., Remaury, Q. B., Cleon, A., Leitner, N. K. V., & Labanowski, J. (2021). Occurrence of carbamazepine, diclofenac, and their related metabolites and transformation products in a French aquatic environment and preliminary risk assessment. Water Research, 196, 117052. [Google Scholar] [Crossref]
16. Hijazi, N., Bavykina, A., Yarulina, I., Shoinkhorova, T., Ramos-Fernandez, E. V., & Gascon, J. (2025). Chemical engineering of zeolites: alleviating transport limitations through hierarchical design and shaping. Chemical Society Reviews. [Google Scholar] [Crossref]
17. Ilau-Uli, A., Oguyo, H., Ngozi, N. A., & Olajided, I. O. Development of Sustainable Water Management Technologies for Communities Using Low-Cost Filter Materials. [Google Scholar] [Crossref]
18. Jin, H., Hong, K., Liu, J., Qiu, C., Zhu, M., Li, C., & Wang, Q. (2025). Structural and functional design of CTAB-geopolymer adsorbents for rapid removal of tetracycline: A comparative study. Separation and purification technology, 356, 129872. [Google Scholar] [Crossref]
19. Jin, H., Zhang, Y., Wang, Q., Chang, Q., & Li, C. (2021). Rapid removal of methylene blue and nickel ions and adsorption/desorption mechanism based on geopolymer adsorbent. Colloid and Interface Science Communications, 45, 100551. [Google Scholar] [Crossref]
20. Khan, R., Iqbal, S., Soliyeva, M., Ali, A., & Elboughdiri, N. (2025). Advanced clay-based geopolymer: influence of structural and material parameters on its performance and applications. RSC advances, 15(16), 12443-12471. [Google Scholar] [Crossref]
21. Kryuchkova, M., Batasheva, S., Akhatova, F., Babaev, V., Buzyurova, D., Vikulina, A., . . . Rozhina, E. (2021). Pharmaceuticals removal by adsorption with montmorillonite nanoclay. International Journal of Molecular Sciences, 22(18), 9670. [Google Scholar] [Crossref]
22. Kumar, S. G. K. M., Kinuthia, J. M., Oti, J., & Adeleke, B. O. (2025). Geopolymer Chemistry and Composition: A Comprehensive Review of Synthesis, Reaction Mechanisms, and Material Properties—Oriented with Sustainable Construction. Materials, 18(16), 3823. [Google Scholar] [Crossref]
23. Kumari, N., & Mohan, C. (2021). Basics of clay minerals and their characteristic properties. Clay Clay Miner, 24(1), 1-29. [Google Scholar] [Crossref]
24. Li, Q., Yi, M., Shao, L., Kou, Y., Wei, Y., & Wang, K. (2024). CTAB modified metakaolin-based geopolymer microspheres for the selective adsorption and recovery of TcO4−/ReO4−. Separation and purification technology, 350, 127853. [Google Scholar] [Crossref]
25. Luhar, I., Luhar, S., Abdullah, M. M. A. B., Razak, R. A., Vizureanu, P., Sandu, A. V., & Matasaru, P.-D. (2021). A state-of-the-art review on innovative geopolymer composites designed for water and wastewater treatment. Materials, 14(23), 7456. [Google Scholar] [Crossref]
26. Maged, A., El-Fattah, H. A., Kamel, R. M., Kharbish, S., & Elgarahy, A. M. (2023). A comprehensive review on sustainable clay-based geopolymers for wastewater treatment: circular economy and future outlook. Environmental monitoring and assessment, 195(6), 693. [Google Scholar] [Crossref]
27. Mennas, N., Lahreche, S., Chouli, F., Sabantina, L., & Benyoucef, A. (2023). Adsorption of methylene blue dye by cetyltrimethylammonium bromide intercalated polyaniline-functionalized montmorillonite clay nanocomposite: Kinetics, isotherms, and mechanism study. Polymers, 15(17), 3518. [Google Scholar] [Crossref]
28. Moya-Llamas, M.-J., Trapote, A., & Prats, D. (2021). Carbamazepine removal from low-strength municipal wastewater using a combined UASB-MBR treatment system. Water Science and Technology, 83(8), 1920-1931. [Google Scholar] [Crossref]
29. Naghdi, M., Taheran, M., Pulicharla, R., Rouissi, T., Brar, S. K., Verma, M., & Surampalli, R. Y. (2019). Pine-wood derived nanobiochar for removal of carbamazepine from aqueous media: Adsorption behavior and influential parameters. Arabian Journal of Chemistry, 12(8), 5292-5301. [Google Scholar] [Crossref]
30. Ncibi, M. C., & Sillanpää, M. (2017). Optimizing the removal of pharmaceutical drugs Carbamazepine and Dorzolamide from aqueous solutions using mesoporous activated carbons and multi-walled carbon nanotubes. Journal of Molecular Liquids, 238, 379-388. [Google Scholar] [Crossref]
31. Pahari, S., Dorneles de Mello, M., Shah, M. S., Josephson, T. R., Ren, L., Nguyen, H. G. T., . . . Siepmann, J. I. (2021). Ethanol and Water Adsorption in Conventional and Hierarchical All-Silica MFI Zeolites. ACS Physical Chemistry Au, 2(2), 79-88. [Google Scholar] [Crossref]
32. Paparo, R., Di Serio, M., Roviello, G., Ferone, C., Trifuoggi, M., Russo, V., & Tarallo, O. (2024). Geopolymer-based materials for the removal of ibuprofen: a preliminary study. Molecules, 29(10), 2210. [Google Scholar] [Crossref]
33. Scolaro, L., Schackow, A., Folgueras, M., & Ueno, O. (2025). Using response surface analysis for the optimization of mechanical strength and microstructure of geopolymers with different SiO2/Al2O3 and SiO2/Na2O ratios. Cerâmica, 71, eSMWS5780. [Google Scholar] [Crossref]
34. Shan, D., Deng, S., Zhao, T., Wang, B., Wang, Y., Huang, J., . . . Wiesner, M. R. (2016). Preparation of ultrafine magnetic biochar and activated carbon for pharmaceutical adsorption and subsequent degradation by ball milling. Journal of hazardous materials, 305, 156-163. [Google Scholar] [Crossref]
35. Shirzad-Siboni, M., Khataee, A., Hassani, A., & Karaca, S. (2015). Preparation, characterization and application of a CTAB-modified nanoclay for the adsorption of an herbicide from aqueous solutions: Kinetic and equilibrium studies. Comptes Rendus Chimie, 18(2), 204-214. [Google Scholar] [Crossref]
36. Singhal, A., Gangwar, B. P., & Gayathry, J. (2017). CTAB modified large surface area nanoporous geopolymer with high adsorption capacity for copper ion removal. Applied Clay Science, 150, 106-114. [Google Scholar] [Crossref]
37. Siyal, A. A., Shamsuddin, M. R., & Low, A. (2021). Fly ash based geopolymer for the adsorption of cationic and nonionic surfactants from aqueous solution–A feasibility study. Materials Letters, 283, 128758. [Google Scholar] [Crossref]
38. Soni, I., Kumar, P., Shandilya, P., Kumar, M., & Chauhan, V. (2025). Surfactant-Assisted Modification of Adsorbents for Optimized Dye Removal. ACS omega. [Google Scholar] [Crossref]
39. Šuránek, M., Melichová, Z., Mirković, M. M., Ivanović, M., Pavlović, V. B., Kljajević, L., & Nenadović, S. (2023). The study of Cu (II) adsorption onto synthetically modified geopolymers. Sustainability, 15(4), 2869. [Google Scholar] [Crossref]
40. Temkin, M. (1940). Kinetics of ammonia synthesis on promoted iron catalysts. Acta physiochim. URSS, 12, 327-356. [Google Scholar] [Crossref]
41. To, M.-H., Hadi, P., Hui, C.-W., Lin, C. S. K., & McKay, G. (2017). Mechanistic study of atenolol, acebutolol and carbamazepine adsorption on waste biomass derived activated carbon. Journal of Molecular Liquids, 241, 386-398. [Google Scholar] [Crossref]
42. Viegas, R. M., Melo, M. L., Brandão Lima, L. C., Garcia, R. R., Filho, E. C. S., Osajima, J. A., & Chiavone-Filho, O. (2024). Carbamazepine adsorption with a series of organoclays: removal and toxicity analyses. Applied Water Science, 14(6), 133. [Google Scholar] [Crossref]
43. Vigdorowitsch, M., Pchelintsev, A., Tsygankova, L., & Tanygina, E. (2021). Freundlich isotherm: An adsorption model complete framework. Applied Sciences, 11(17), 8078. [Google Scholar] [Crossref]
44. Wang, Z., & Lu, D. (2020). Study on the effect of emulsifiers on the pore structures of geopolymer prepared by emulsion templating. Materials Research Express, 7(5), 055508. [Google Scholar] [Crossref]
45. Werling, N., Kaltenbach, J., Weidler, P. G., Schuhmann, R., Dehn, F., & Emmerich, K. (2022). Solubility of calcined kaolinite, montmorillonite, and illite in high molar NaOH and suitability as precursors for geopolymers. Clays and Clay Minerals, 70(2), 270-289. [Google Scholar] [Crossref]
46. Yasmin, P. (2021). 3D-printed geopolymers for adsorption of carbamazepine removal. [Google Scholar] [Crossref]
47. You, S., Ho, S. W., Li, T., Maneerung, T., & Wang, C.-H. (2019). Techno-economic analysis of geopolymer production from the coal fly ash with high iron oxide and calcium oxide contents. Journal of hazardous materials, 361, 237-244. [Google Scholar] [Crossref]
48. Yu, Y., Chen, D., Xie, S., Sun, Q., Zhang, Z.-X., & Zeng, G. (2022). Adsorption behavior of carbamazepine on Zn-MOFs derived nanoporous carbons: Defect enhancement, role of N doping and adsorption mechanism. Journal of environmental chemical engineering, 10(3), 107660. [Google Scholar] [Crossref]
49. Zayyat, R. M., Yahfoufi, R., Al-Hindi, M., Kordahi, M. A., Ayoub, G. M., & Ahmad, M. N. (2024). Elucidating the dynamics of carbamazepine uptake using date pit-derived activated carbon: a comprehensive kinetic and thermodynamic analysis. Heliyon, 10(20). [Google Scholar] [Crossref]
Metrics
Views & Downloads
Similar Articles
- Ayurveda and Skin Health: A Comprehensive Framework for the Management of Dermatological Disorders
- Gender and Political Exclusion: An Analysis of Women's Marginalization in India's Democracy
- Safety Standards Compliance among Universities Employees in Nairobi County, Kenya During the Covid-19 Pandemic
- Cedi Appreciation Relative to Fuel Prices - A Machine Learning and Ancient Geomantic Approach