Malays. J. Anal. Sci. Volume 30 Number 2 (2026): 1649

 

Research Article

 

Optimized synthesis of Cu2+-modified Samanea saman-derived carbon adsorbent for metformin adsorption

 

Mohd Raziff Mat Hasan, Erniza Mohd Johan Jaya, and Mohd Azmier Ahmad*

 

School of Chemical Engineering, Engineering Campus, Universiti Sains Malaysia, 14300 Nibong Tebal, Penang, Malaysia

 

*Corresponding author: chazmier@usm.my

 

Received: 6 August 2025; Revised: 21 January 2026; Accepted: 1 March 2026; Published: 28 April 2026

Abstract

This study explores the efficacy of copper-modified carbon adsorbent derived from Samanea saman (Cu²⁺-SSCA) for the removal of metformin (MET), a commonly detected pharmaceutical pollutant, from aqueous environments. The pristine SSCA was synthesized through pyrolysis of the precursor under nitrogen (N₂), followed by CO₂ activation in a vertical furnace. Subsequent surface modification was achieved via impregnation with copper (II) nitrate [Cu(NO₃)₂], yielding the Cu²⁺-SSCA. The resulting material demonstrated a Brunauer–Emmett–Teller surface area (S.A.BET) of 748.66 m²/g, a mesoporous surface area (S.A.MESO) of 548.74 m²/g, total pore volume (T.P.V.) of 0.3051 cm³/g, followed by an average pore diameter (A.P.D.) of 2.41 nm, characteristics indicative of a well-developed mesoporous network. Process optimization using response surface methodology (RSM) identified optimum conditions at an activation temperature of 579 °C, followed by activation time of 1.20 h, and lastly, a Cu²⁺ ion impregnation ratio (IR) of 0.50 g/g. Under these conditions, the model-predicted MET adsorption capacity and Cu²⁺-SSCA yield were 67.63 mg/g and 32.81%, respectively, in close agreement with experimental results of 68.90 mg/g (error of 1.84%) and 34.00% (error of 3.50%). Isotherm modelling revealed that MET adsorption adhered to the Langmuir model, exhibiting a Langmuir capacity (Qₘ) of 109.27 mg/g. The Freundlich heterogeneity index (nF) of 1.71 further confirmed favourable adsorption behaviour. In terms of kinetic study, the adsorption system followed pseudo-first order (PFO) the best.

 

Keywords: adsorption, surface modification, activated carbon, optimization, isotherm

 


References

1.    Mat Zaini, Y. M., Dina Amalia Purba, L., Abdullah, N., Yuzir, A., Iwamoto, K., and Mohamad, S. E. (2022). Removals of atenolol, gliclazide and prazosin using sequencing batch reactor. Materials Today: Proceedings, 65: 3007-3014.

2.    Mohamad, F. M. Y., Abdullah, A. Z., and Ahmad, M. A. (2024). Amoxicillin adsorption from aqueous solution by Cu(II) modified lemon peel based activated carbon: Mass transfer simulation, surface area prediction and F-test on isotherm and kinetic models. Powder Technology, 438: 119589.

3.    Ferri, B. B., Wernke, G., Resende, J. F., Ribeiro, A. C., Cusioli, L. F., Bergamasco, R., and Vieira, M. F. (2024). Natural zeolite as adsorbent for metformin removal from aqueous solutions: Adsorption and regeneration properties. Desalination and Water Treatment, 320: 100602.

4.    Ambrosio-Albuquerque, E. P., Cusioli, L. F., Bergamasco, R., Sinópolis Gigliolli, A. A., Lupepsa, L., Paupitz, B. R., Barbieri, P. A., Borin-Carvalho, L. A., and de Brito Portela-Castro, A. L. (2021). Metformin environmental exposure: A systematic review. Environmental Toxicology and Pharmacology, 83: 103588.

5.    Kumar, R., Akbarinejad, A., Jasemizad, T., Fucina, R., Travas-Sejdic, J., and Padhye, L. P. (2021). The removal of metformin and other selected PPCPs from water by poly(3,4-ethylenedioxythiophene) photocatalyst. Science of The Total Environment, 751: 142302.

6.    Garazade, N., Can-Güven, E., Güven, F., Yazici Guvenc, S., and Varank, G. (2025). Application of machine learning algorithms for the prediction of metformin removal with hydroxyl radical-based photochemical oxidation and optimization of process parameters. Journal of Hazardous Materials, 489: 137552.

7.    Hosseini, M. M., Solouki, M., Ghobadi-Nejad, Z., and Yaghmaei, S. (2026). Integrated Electrochemical–Biological Treatment for Efficient Removal of Metformin and Its By-Products: Optimization, Mineralization, and Toxicity Assessment. Case Studies in Chemical and Environmental Engineering: 101322.

8.    Khir, N. H. M., Salleh, N. F. M., Ghafar, N. A., Shukri, N. M., and Jusoh, R. (2025). Preparation and characterization of modified rambutan peels for the removal of chromium(VI) and nickel(II) from aqueous solution: Environmental impact and optimization Malaysian Journal of Analytical Sciences, 29(1): 1292.

9.    Ramlee, D. A., Nordin, N. A., Rahman, N. A., and Bahruji, H. (2024). Removal of acetaminophen by using electrospun pan/sago lignin-based activated carbon nanofibers. Malaysian Journal of Analytical Sciences, 28(6): 1442 - 1457.

10.  Aziz, A., Nasehir Khan, M. N., Mohamad Yusop, M. F., Mohd Johan Jaya, E., Tamar Jaya, M. A., and Ahmad, M. A. (2021). Single-stage microwave-assisted coconut-shell-based activated carbon for removal of dichlorodiphenyltrichloroethane (DDT) from aqueous solution: Optimization and batch studies. International Journal of Chemical Engineering, 2021(1): 9331386.

11.  Gunasekaran, S., Liu, A. J. X., and Ng, S. L. (2024). Activated carbon/iron oxide composites with different weight ratios for acid orange 7 removal. Malaysian Journal of Analytical Sciences, 28(6): 1359 - 1373.

12.  Nur Syahirah Mohamed, H., Farihahusnah, H., Lai Ti, G., and Mohamed Kheireddine, A. (2024). Characterisation of egg white-impregnated activated carbon for CO2 adsorption application. Malaysian Journal of Science, 43(Sp1): 20-25.

13.  Yusop, M. F. M., Tamar Jaya, M. A., Idris, I., Abdullah, A. Z., and Ahmad, M. A. (2023). Optimization and mass transfer simulation of remazol brilliant blue R dye adsorption onto meranti wood based activated carbon. Arabian Journal of Chemistry, 16: 104683.

14.  Saputra, D. A., Pratoto, A., Rahman, M. F., and Kodama, A. (2024). The effect of chemical activation agents and activation temperature on the pore structure of rice husk-derived activated carbon. Malaysian Journal of Science, 43(Sp1): 1-7.

15.  Firdaus, M. Y. M., Rashid, M. M., Alam, M. M., and Ahmad, M. A. (2025). Copper-modified surface of orange peel-derived activated carbon for amoxicillin removal: Mass transfer simulation, attraction mechanism, and regeneration studies. Arabian Journal for Science and Engineering.

16.  Firdaus, M. Y. M., Rashid, M. M., Alam, M. M., and Ahmad, M. A. (2025). Enhanced Cd2+ removal via deprotonated-mango trunk functionalized carbon: Optimization and F-test for linear and non-linear isotherm and kinetic models. Chemical Engineering Research and Design, 220: 96-116.

17.  Ahmad, M. A., Yusop, M. F. M., Awang, S., Yahaya, N. K. E. M., Rasyid, M. A., and Hassan, H. (2021). Carbonization of sludge biomass of water treatment plant using continuous screw type conveyer pyrolyzer for methylene blue removal. IOP Conference Series: Earth and Environmental Science, 765: 012112.

18.  Zainuddin, N. J., Jamaluddin, M. A., Gusri, N. A., Rahizal, N. A., and Yusof, N. H. I. M. (2024). Optimization study of methylene blue decolorization using waterfilter prototype embedded with sugarcane bagasse biochar. Malaysian Journal of Chemistry, 26(3): 264-272.

19.  Ahammad, N. A., Yusop, M. F. M., Mohd Din, A. T., and Ahmad, M. A. (2021). Preparation of alpinia galanga stem based activated carbon via single-step microwave irradiation for cationic dye removal. Sains Malaysiana, 50(8): 2251-2269.

20.  Daouda, M. M. A., Akowanou, A. V. O. e., Mahunon, S. E. R., Adjinda, C. K., Aina, M. P. e., and Drogui, P. (2021). Optimal removal of diclofenac and amoxicillin by activated carbon prepared from coconut shell through response surface methodology. South African Journal of Chemical Engineering, 38(1): 78-89.

21.  Yusop, M. F. M., Baharudin, M. H., Rashid, M. M., Alam, M. M., and Ahmad, M. A. (2025). Amoxicillin adsorption onto oil palm trunk-derived activated carbon: synthesis optimization, modelling of mass transfer and ultrasonic regeneration. Journal of Chemical Technology & Biotechnology, 100(6): 1310-1327.

22.  Mohamad, F. M. Y., Rashid, M. M., Alam, M. M., and Ahmad, M. A. (2025). Copper metal-functionalized carbon from rattan waste via microwave pyrolysis for enhanced chloramphenicol removal: Optimization and F-test study. Particuology, 100: 196-213.

23.  Tahir, Z. M., Mohamad Mohidin, F. S., and N Rosely, N. F. (2020). Visual Tree Analysis of Rain Trees (Samanea saman) in Universiti Sains Malaysia, Main Campus. IOP Conference Series: Earth and Environmental Science, 549(1): 012032.

24.  Alli, H., and Hishammuddin, U. (2022). Investigation and Development of Raintree Furniture From The Waste of Urban Tree. International Journal of Social Science Research, 4(1): 34-45.

25.  Fröhlich, A., Przepióra, F., Drobniak, S., Mikusiński, G., and Ciach, M. (2024). Public safety considerations constraint the conservation of large old trees and their crucial ecological heritage in urban green spaces. Science of The Total Environment, 948: 174919.

26.  Langmuir, I. (1918). The adsorption of gases on plane surfaces of glass, mica and platinum. Journal of the American Chemical Society, 40(9): 1361-1403.

27.  Freundlich, H. (1906). Over the adsorption in solution. Journal of Physical Chemistry, 57(385471): 1100-1107.

28.  Tempkin, M., and Pyzhev, V. (1940). Kinetics of ammonia synthesis on promoted iron catalyst. Acta Physicochimica URSS, 12(1): 327.

29.  Mohamad, F. M. Y., Abdullah, A. Z., and Ahmad, M. A. (2023). Adsorption of remazol brilliant blue R dye onto jackfruit peel based activated carbon: Optimization and simulation for mass transfer and surface area prediction. Inorganic Chemistry Communications, 158: 111721.

30.  Lagergren, S. K. (1898). About the Theory of So-called Adsorption of Soluble Substances. Sven. Vetenskapsakad. Handingarl, 24: 1-39.

31.  Ho, Y. S., and McKay, G. (1998). Sorption of dye from aqueous solution by peat. Chemical Engineering Journal, 70(2): 115-124.

32.  Kılıç, M., Bekman, M. E., Bodur, F., Yıldız, A., and Varol, E. A. (2025). Modeling and optimization of flash heating process conditions for activated carbon production using Response Surface Methodology (RSM). Diamond and Related Materials, 154: 112239.

33.  Sulaiman, N. S., Hashim, R., Mohamad Amini, M. H., Danish, M., and Sulaiman, O. (2018). Optimization of activated carbon preparation from cassava stem using response surface methodology on surface area and yield. Journal of Cleaner Production, 198: 1422-1430.

34.  Sopandi, T. P., Sulianto, A. A., Anugroho, F., Yusoff, M. Z. M., Mohamed, M. S., Farid, M. A. A., and Setyawan, H. Y. (2025). RSM-optimized biochar production from young coconut waste (Cocos nucifera): Multivariate analysis of non-linear interactions between temperature, time, and activator concentration. Industrial Crops and Products, 223: 120157.

35.  Beyan, S. M., Prabhu, S. V., Sissay, T. T., and Getahun, A. A. (2021). Sugarcane bagasse based activated carbon preparation and its adsorption efficacy on removal of BOD and COD from textile effluents: RSM based modeling, optimization and kinetic aspects. Bioresource Technology Reports, 14: 100664.

36.  Yu, H., Mikšík, F., Thu, K., and Miyazaki, T. (2024). Characterization and optimization of pore structure and water adsorption capacity in pinecone-derived activated carbon by steam activation. Powder Technology, 431: 119084.

37.  Weldekidan, H., Patel, H., Mohanty, A., and Misra, M. (2024). Synthesis of porous and activated carbon from lemon peel waste for CO2 adsorption. Carbon Capture Science & Technology, 10: 100149.

38.  Firdaus, M. Y. M., Nasran, M. N. K., Ridzuan, Z., Zuhairi, A. A., and Azmier, M. A. (2023). Mass transfer simulation on remazol brilliant blue R dye adsorption by optimized teak wood Based activated carbon. Arabian Journal of Chemistry, 16(6): 104780.

39.  Yaacob, N. A., Khasri, A., Ridzuan, M. J. M., and Salleh, N. H. M. (2021). Statistical optimization of methylene blue dye removal efficiency by merbau based activated carbon via RSM-CCD. AIP Conference Proceedings, 2339(1): 020223.

40.  Nasran, N. K. M., Firdaus, M. Y. M., Faizal, P. M. L. M., and Azmier, A. M. (2023). Alteration of Tecoma chip wood waste into microwave-irradiated activated carbon for amoxicillin removal: Optimization and batch studies. Arabian Journal of Chemistry, 16(10): 105110.

41.  Yusop, M. F. M., Mohd Johan Jaya, E., Mohd Din, A. T., Bello, O. S., and Ahmad, M. A. (2022). Single-stage optimized microwave-induced activated carbon from coconut shell for cadmium adsorption. Chemical Engineering & Technology, 45(11): 1943-1951.

42.  Wei, X., Huang, S., Yang, J., Liu, P., Li, X., Wu, Y., and Wu, S. (2023). Adsorption of phenol from aqueous solution on activated carbons prepared from antibiotic mycelial residues and traditional biomass. Fuel Processing Technology, 242: 107663.

43.  Firdaus, M. Y. M., Rashid, M. M., Alam, M. M., and Ahmad, M. A. (2025). Synthesis of deprotonated grape stem functionalized carbon for boosted Cu2+ adsorption – Optimization, interaction mechanism, and F-test analysis. Microchemical Journal, 218: 115795.

44.  Aziz, A., Mohamad Yusop, M. F., and Ahmad, M. A. (2024). Harnessing microwave energy to transform Nephelium lappaceum L. peel into activated carbon for chloramphenicol eradication in aqueous solutions. Materials Chemistry and Physics, 318: 129311.

45.  Wu, W., Zhao, B., Qu, Z., Pan, J., and Guo, Q. (2025). Adsorption of metformin in aqueous system by biochars derived from different biomasses: Performance and mechanisms. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 727: 138438.

46.  Mohammad, A. H., Radovic, I., Ivanović, M., and Kijevčanin, M. (2022). Adsorption of metformin on activated carbon produced from the water hyacinth biowaste using H3PO4 as a chemical activator. Sustainability, 14(18): 11144.

47.  Jimoh, O. S., Omotayo, I. A., and and Bello, O. S. (2023). Metformin adsorption onto activated carbon prepared by acid activation and carbonization of orange peel. International Journal of Phytoremediation, 25(2): 125-136.

48.  Quesada, H. B., de Araújo, T. P., Cusioli, L. F., de Barros, M. A. S. D., Gomes, R. G., and Bergamasco, R. (2021). Evaluation of novel activated carbons from chichá-do-cerrado (Sterculia striata St. Hil. et Naud) fruit shells on metformin adsorption and treatment of a synthetic mixture. Journal of Environmental Chemical Engineering, 9(1): 104914.

49.  Pap, S., Shearer, L., and Gibb, S. W. (2023). Effective removal of metformin from water using an iron-biochar composite: Mechanistic studies and performance optimisation. Journal of Environmental Chemical Engineering, 11(5): 110360.

50.  Vareda, J. P. (2023). On validity, physical meaning, mechanism insights and regression of adsorption kinetic models. Journal of Molecular Liquids, 376: 121416.