Optimization of the photocatalytic degradation process of amoxicillin antibiotic using SiO2@TiO2 nanocomposite

Document Type : Research Paper


1 Department of Environmental Sciences & Engineering, Faculty of Agriculture & Natural Resources, Ardakan University, Ardakan, Iran.

2 Department of Environmental Sciences, Faculty of Natural Resources and Environment, University of Birjand, Birjand, Iran.



Today, one of the most important challenges in wastewater treatment is the destruction of organic pollutants, especially antibiotics. This research investigated the efficiency of the photocatalytic process in removing the antibiotic amoxicillin from the water environment using SiO2@TiO2 nanocomposite. The desired nanocomposite has been synthesized using sol-gel method and characterized by XRD, FTIR and TEM techniques. To improve the performance of the fabricated nanocomposite, parameters such as pH, contact time, nanocomposite concentration, and drug concentration were studied and optimized using the response surface method and the Central Composite Design model. Characterization of nanocomposite with XRD showed the formation of crystalline phases and anatase structure. The formation of SiO2@TiO2 nanocomposite with Ti-O-Si bond was confirmed in FT-IR spectrum. Also, the TEM image showed that the particles have a spherical and uniform structure. The results of photocatalytic optimization experiments showed that the highest degradation efficiency (98.7%) of amoxicillin under pH:3, amoxicillin initial concentration: 10 mg/L, nanocomposite concentration: 2 g/L, contact time: 10 minutes, which is very close to the efficiency of predicted removal under optimal conditions in the BBD model (100%). Due to the high degradation efficiency and high production of free radicals, the synthetic photocatalyst has a high ability to degrade pharmaceutical pollutants, especially antibiotics, which develops its future applications for the degradation of organic pollutants with a similar chemical structure.


Abd Elkodous, M., Hassaan, A., Ghoneim, A.I., Abdeen, Z., 2018. C-dots dispersed macro-mesoporous TiO2 phtocatalyst for effective waste water treatment. Characterization and Application of Nanomaterials 1(2).
Adnan, M.A.M., Afzal, S., Johan, M.R., Julkapli, N.M., 2022. A comparative study on the photodegradation efficiency of TiO2-CS hybrid beads under wet and dry conditions. International Journal of Materials and Product Technology 65(1), 67-79.
Ahmadpour, N., Sayadi, M.H., Homaeigohar, S., 2020. A hierarchical Ca/TiO 2/NH 2-MIL-125 nanocomposite photocatalyst for solar visible light induced photodegradation of organic dye pollutants in water. RSC Advances 10(50), 29808-29820.
Al-Musawi, T.J., Kamani, H., Bazrafshan, E., Panahi, A.H., Silva, M.F., Abi, G., 2019. Optimization the effects of physicochemical parameters on the degradation of cephalexin in sono-Fenton reactor by using box-Behnken response surface methodology. Catalysis Letters 149(5), 1186-1196.
Balarak, D., Mostafapour, F.K., Azarpira, H., 2016. Adsorption isotherm studies of tetracycline antibiotics from aqueous solutions by maize stalks as a cheap biosorbent. International Journal of Pharmacy and Technology 8(3), 16664-16675.
Behera, A.K., Shadangi, K.P., Sarangi, P.K., 2022. Synthesis of dye-sensitized TiO2/Ag doped nano-composites using UV photoreduction process for phenol degradation: A comparative study. Environmental Pollution312, p.120019.
Budiarti, H.A., Puspitasari, R.N., Hatta, A.M., Risanti, D.D., 2017. Synthesis and characterization of TiO2@ SiO2 and SiO2@ TiO2 core-shell structure using lapindo mud extract via sol-gel method. Procedia Engineering, 170, 65-71.
Chamanehpour, E., Sayadi, M.H., Hajiani, M., 2022. A hierarchical graphitic carbon nitride supported by metal–organic framework and copper nanocomposite as a novel bifunctional catalyst with long-term stability for enhanced carbon dioxide photoreduction under solar light irradiation. Advanced Composites and Hybrid Materials 5(3), 2461-2477.
Chamanehpour, E., Sayadi, M.H., Hajiani, M., 2023. Metal-organic framework coordinated with g-C3N4 and metal ions for boosting photocatalytic H2 production under sunlight. Journal of Photochemistry and Photobiology A: Chemistry 434, 114221.
Chireh, M., Naseri, M. and Kamalianfar, A., 2020. 57Fe Mossbauer spectroscopy investigation of NiFe2O4 and MnFe2O4 ferrite nanoparticles prepared by thermal treatment method. Applied Physics A 126(7), 543.
de Franco, M.A.E., de Carvalho, C.B., Bonetto, M.M., de Pelegrini Soares, R., Féris, L.A., 2017. Removal of amoxicillin from water by adsorption onto activated carbon in batch process and fixed bed column: kinetics, isotherms, experimental design and breakthrough curves modelling. Journal of Cleaner Production 161, 947-956.
Deng, Y., Tang, L., Feng, C., Zeng, G., Wang, J., Zhou, Y., Liu, Y., Peng, B., Feng, H., 2018. Construction of plasmonic Ag modified phosphorous-doped ultrathin g-C3N4 nanosheets/BiVO4 photocatalyst with enhanced visible-near-infrared response ability for ciprofloxacin degradation. Journal of Hazardous Materials 344, 758-769.
Dubey, R.S., Rajesh, Y.B.R.D., More, M.A., 2015. Synthesis and characterization of SiO2 nanoparticles via sol-gel method for industrial applications. Materials Today: Proceedings 2(4-5), 3575-3579.
Eddy, D.R., Ishmah, S.N., Permana, M.D., Firdaus, M.L., 2020. Synthesis of titanium dioxide/silicon dioxide from beach sand as photocatalyst for Cr and Pb remediation. Catalysts 10(11), 1248.
Fahoul, N., Sayadi, M.H., Rezaei, M.R., Homaeigohar, S., 2022. Nickel ferrite nanoparticles catalyzed dark fermentation of dairy wastewater for biohydrogen production. Bioresource Technology Reports 19, 101153.
Hosseini, R., Sayadi, M.H., Shekari, H., 2019. Adsorption of nickel and chromium from aqueous solutions using copper oxide nanoparticles: adsorption isotherms, kinetic modeling, and thermodynamic studies. Avicenna Journal of Environmental Health Engineering 6(2), 66-74.
Hu, Y.Y., Pan, C., Zheng, X., Hu, F., Xu, L., Xu, G., Jian, Y., Peng, X., 2021. Prediction and optimization of adsorption properties for Cs+ on NiSiO@ NiAlFe LDHs hollow spheres from aqueous solution: kinetics, isotherms, and BBD model. Journal of Hazardous Materials 401, 123374.
Hussien, M.S., Yahia, I.S., 2021. Hybrid multifunctional core/shell gC 3 N 4@ TiO 2 heterojunction nano-catalytic for photodegradation of organic dye and pharmaceutical compounds. Environmental Science and Pollution Research 28, 29665-29680.
Jiang, R., on Tung, S., Tang, Z., Li, L., Ding, L., Xi, X., Liu, Y., Zhang, L., Zhang, J., 2018. A review of core-shell nanostructured electrocatalysts for oxygen reduction reaction. Energy Storage Materials 12, 260-276.
Kanakaraju, D., Kockler, J., Motti, C.A., Glass, B.D., Oelgemöller, M., 2015. Titanium dioxide/zeolite integrated photocatalytic adsorbents for the degradation of amoxicillin. Applied Catalysis B: Environmental 166, 45-55.
Kargar, F., Bemani, A., Sayadi, M.H., Ahmadpour, N., 2021. Synthesis of modified beta bismuth oxide by titanium oxide and highly efficient solar photocatalytic properties on hydroxychloroquine degradation and pathways. Journal of Photochemistry and Photobiology A: Chemistry 419, 113453.
Kassahun, S.K., Kiflie, Z., Kim, H., Baye, A.F., 2021. Process optimization and kinetics analysis for photocatalytic degradation of emerging contaminant using N-doped TiO2-SiO2 nanoparticle: Artificial Neural Network and Surface Response Methodology approach. Environmental Technology & Innovation 23, 101761.
Lin, Y.P., Mehrvar, M., 2018. Photocatalytic treatment of an actual confectionery wastewater using Ag/TiO2/Fe2O3: optimization of photocatalytic reactions using surface response methodology. Catalysts 8(10), 409.
Lucien, M.A.B., Canarie, M.F., Kilgore, P.E., Jean-Denis, G., Fénélon, N., Pierre, M., Cerpa, M., Joseph, G.A., Maki, G., Zervos, M.J., Dely, P., 2021. Antibiotics and antimicrobial resistance in the COVID-19 era: Perspective from resource-limited settings. International journal of Infectious Diseases 104, 250-254.
Luthfiah, A., Permana, M.D., Deawati, Y., Firdaus, M.L., Rahayu, I., Eddy, D.R., 2021. Photocatalysis of nanocomposite titania–natural silica as antibacterial against Staphylococcus aureus and Pseudomonas aeruginosa. RSC advances 11(61), 38528-38536.
Nasseh, N., Panahi, A.H., Esmati, M., Daglioglu, N., Asadi, A., Rajati, H. and Khodadoost, F., 2020. Enhanced photocatalytic degradation of tetracycline from aqueous solution by a novel magnetically separable FeNi3/SiO2/ZnO nano-composite under simulated sunlight: Efficiency, stability, and kinetic studies. Journal of Molecular Liquids 301, 112434.
Polat, S., Sayan, P., 2019. Application of response surface methodology with a Box–Behnken design for struvite precipitation. Advanced Powder Technology 30(10), 2396-2407.
Poorsajadi, F., Sayadi, M.H., Hajiani, M., Rezaei, M.R., 2022. Synthesis of CuO/Bi2O3 nanocomposite for efficient and recycling photodegradation of methylene blue dye. International journal of environmental Analytical Chemistry, 102(18), 7165-7178.
Raguram, T., Rajni, K.S., 2019. Synthesis and analysing the structural, optical, morphological, photocatalytic and magnetic properties of TiO 2 and doped (Ni and Cu) TiO 2 nanoparticles by sol–gel technique. Applied Physics A 125, 1-11.
Rawson, T.M., Ming, D., Ahmad, R., Moore, L.S., Holmes, A.H., 2020. Antimicrobial use, drug-resistant infections and COVID-19. Nature Reviews Microbiology 18(8), 409-410.
Rezaei, A., Rezaei, M.R., Sayadi, M.H., 2021. 3D network structure graphene hydrogel-Fe3O4@ SnO2/Ag via an adsorption/photocatalysis synergy for removal of 2, 4 dichlorophenol. Journal of the Taiwan Institute of Chemical Engineers 121, 154-167.
Sayadi, M.H., Ahmadpour, N., Homaeigohar, S., 2021. Photocatalytic and antibacterial properties of Ag-CuFe2O4@ WO3 magnetic nanocomposite. Nanomaterials 11(2), 298.
Sayadi, M.H., Chamanehpour, E., Fahoul, N., 2022. The ultrasonic process with titanium magnetic oxide nanoparticles to enhance the amoxicillin removal efficiency. Journal of Water and Environmental Nanotechnology 7(3), 241-251.
Sayadi, M.H., Chamanehpour, E., Fahoul, N., 2023. Recent advances and future outlook for treatment of pharmaceutical from water: an overview. International Journal of Environmental Science and Technology 20(3), 3437-3454.
Setyawati, M.I., Tay, C.Y., Leong, D.T., 2015. Mechanistic investigation of the biological effects of SiO2, TiO2, and ZnO nanoparticles on intestinal cells. Small 11(28), 3458-3468.
Sharma, S., Devi, A., Bhattacharyya, K.G., 2022. Photocatalytic Degradation of Methylene Blue in Aqueous Solution with Silver-Kaolinite-Titania Nanocomposite under Visible Light Irradiation. Journal of Nanostructures 12(2), 426-445.
Wang, M., Zhang, L., Zhang, G., Pang, T., Zhang, X., Cai, D., Wu, Z., 2017. In situ degradation of antibiotic residues in medical intravenous infusion bottles using high energy electron beam irradiation. Scientific Reports 7(1), pp.1-8.
Wu, J., Sun, Q., Lu, J., 2020. Synthesis of magnetic core-shell Fe3O4@ SiO2@ Mg (OH) 2 composite using waste bischofite and its catalytic performance for ozonation of antibiotics. Journal of Environmental Chemical Engineering 8(5), 104318.
Wu, Q., Lu, D., Kondamareddy, K.K., Ho, W., Cao, D., Zeng, Y., Zhang, B., Zhang, Y., Xie, L., Zhao, B., Wang, Z., 2022. Highly efficient photocatalytic degradation for antibiotics and mechanism insight for Bi2S3/g-C3N4 with fast interfacial charges transfer and excellent stability. Arabian Journal of Chemistry 15(3), 103689.
Xu, F., Meng, K., Cheng, B., Wang, S., Xu, J. and Yu, J., 2020. Unique S-scheme heterojunctions in self-assembled TiO2/CsPbBr3 hybrids for CO2 photoreduction. Nature communications 11(1), 4613.
Yuan, D., Zhang, C., Tang, S., Sun, M., Zhang, Y., Rao, Y., Wang, Z., Ke, J., 2020. Fe3+-sulfite complexation enhanced persulfate Fenton-like process for antibiotic degradation based on response surface optimization. Science of the Total Environment 727, 138773.
Zamchiy, A.O., Baranov, E.A., Merkulova, I.E., Khmel, S.Y., Maximovskiy, E.A., 2019. Determination of the oxygen content in amorphous SiOx thin films. Journal of Non-Crystalline Solids 518, 43-50.
Zhang, Z., Hu, L., Zhang, H., Yu, L., Liang, Y., 2020. Large-sized nano-TiO 2/SiO 2 mesoporous nanofilmconstructed macroporous photocatalysts with excellent photocatalytic performance. Frontiers of Materials Science 14, 163-176.