An rGO-decorated TiO2-Fe2O3 Ternary Composite for Photocatalysis of Tetracycline Under Visible Light Irradiation

Anthoni Batahan Aritonang, Hafsoh Tri Mustika Rahimi, Muhamad Agus Wibowo, Warsidah Warsidah

Abstract

Tetracycline (TC) antibiotic residues entering water bodies pose a global health threat, necessitating technology to reduce their concentration. Photocatalysis of rGO-modified TiO₂/Fe₂O₃ composites can degrade TC into simple molecules that are harmless to the environment. In this study, an rGO-decorated TiO₂/Fe₂O₃ composite was successfully synthesized using a combined green synthesis and hydrothermal method. The green-synthesized TiO₂ exhibited a band gap of 3.26 eV. Incorporating Fe₂O₃ into the TiO₂ matrix reduced the band gap to 2.97 eV and demonstrated good photocatalytic activity for the degradation of 30 ppm tetracycline (TC) under visible light irradiation for 120 minutes, achieving a degradation efficiency of 54%. The addition of rGO at weight ratios of 1%, 2%, and 3% to the TiO₂/Fe₂O₃ matrix formed TiO₂/Fe₂O₃/rGO composites designated as TF1, TF2, and TF3 with band gaps of 2.92, 2.82, and 2.94 eV, respectively. The optimal rGO-to-TiO₂/Fe₂O₃ weight ratio was 2% (TF2), yielding the highest TC degradation efficiency of 72%. This enhanced photocatalytic activity for TC degradation stems from the synergistic contribution between the TiO₂/Fe₂O₃ heterojunction composite and rGO, facilitated by charge-pair separation through charge transfer from the TiO₂/Fe₂O₃ to the rGO surface.

Keywords

degradation; photocatalytic; tetracycline; TiO2/Fe2O3/rGO; visible light.

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References

Aritonang, A.B., Putri, R.A., Sisca, V., Madiabu, M.J., and Khoiriah, K., 2025. Photocatalytic Degradation of Acid Yellow 25 Using Nanoparticle TiO2 Mediated Petai Pod Extract. Baghdad Science Journal, 22, 1851–1862. https://doi.org/10.21123/2411-7986.4960.

Aritonang, A.B., Krisnandi, Y.K., and Gunlazuardi, J., 2018. Modification of TiO2 Nanotube Arrays with N Doping and Ag Decorating for Enhanced Visible Light Photoelectrocatalytic Degradation of Methylene Blue. International Journal on Advanced Science Engineering Information Technology, 8, 234–24. https://doi.org/10.18517/ijaseit.8.1.2342.

Aritonang, A.B., Parwanty, P., Wibowo, M.S., Ardiningsih, P., and Adhitiyawarman, A., 2022. Sintesis TiO2-rGO dengan Pereduksi Alumunium untuk Fotokatalisis Degradasi Metilen Biru dibawah Irradiasi Sinar Tampak, Equilibrium Journal of Chemical Engineering, 6, 150–156. https://doi.org/10.20961/equilibrium.v6i2.65518.

Aritonang, A.B., Pratiwi E., Warsidah., Nurdiansyah S.I, and Risko., 2021. Fe-doped TiO2/Kaolinite as an Antibacterial Photocatalyst under Visible Light Irradiation. Bulletin of Chemical Reaction Engineering & Catalysis, 16, 293–301. https://doi.org/10.9767/bcrec.16.2.10325.293-301.

Botsa, M.B., 2025. Reduced Graphene Oxide Assisted TiO2 Fe2O3 Ternary Nanocomposite for Efficient Visible Light Driven Photocatalysis of Nitrobenzene and Dye Pollutants. Advanced Composites and Hybrid Materials, 8, 384–399. https://doi.org/10.1007/s42114-025-01431-w.

Cao, Y., Yang, W., Zhang, W., Liu, G., and Yue, P., 2004. Improved Photocatalytic Activity of Sn4+ Doped TiO2 Nanoparticulate Films Prepared by Plasma-Enhanced Chemical Vapor Deposition. New Journal of Chemistry, 28, 218–222. https://doi.org/10.1039/b306845e.

Chang, C., Rad, S., Gan, L., Li, Z., Dai, J., and Shahab, A., 2023. Review of The Sol-Gel Method in Preparing Nano TiO2 for Advanced Oxidation Process. Nanotechnology Reviews, 12, 1–23. https://doi.org/10.1515/ntrev-2023-0150.

Elmund, G.K., Mormson, S.M., Grant, D.W., and Nevlns, S.M.P., 1971. Role of Excreted ChlorTetracycline in Modifying the Decomposition Process in Feedlot Waste. Bulletin of Environmental Contamination & Toxicology, 6, 129–132.

Fakhouri, A.S., 2026. Biotechnological Potential of Sargassum Ilicifolium Seaweed: A Proximate Composition of Antibacterial, Antioxidant, and Hypoglycemic Bioactive Compounds. BioResources, 21, 3872–3893. https://doi.org/10.15376/biores.21.2.3872-3893

Farkaš, B., Terranova, U., and de Leeuw, N.H., 2019. Binding Modes of Carboxylic Acids on Cobalt Nanoparticles. Royal Society of Chemistry, 22, 985–996. https://doi.org/10.1039/c9cp04485j

Hidayati, U.F., Aritonang, A.B., and Destiarti, L., 2021. TiO2-rGO Composite for Photocatalytic Decolorization of Methylene Blue Under the Visible Light Illumination. Berkala Sainstek, 9, 167–173. https://doi.org/10.19184/bst.v9i4.27602.

Hong, T., Yin, J.Y., Nie, S.P., and Xie, M.Y., 2021. Applications of Infrared Spectroscopy in Polysaccharide Structural Analysis: Progress, Challenge and Perspective. Food Chemistry, 12, 100168. https://doi.org/10.1016/j.fochx.2021.100168.

Hossain, M.S., and Ahmed, S., 2023. Easy and Green Synthesis of TiO2 (Anatase and Rutile): Estimation of Crystallite Size Using Scherrer Equation, Williamson-Hall Plot, Monshi-Scherrer Model, Size-Strain Plot, Halder- Wagner Model. Results in Materials, 20, 100492. https://doi.org/10.1016/j.rinma.2023.100492.

Jo, W., and Selvam, N.C.S., 2015. Synthesis of GO Supported Fe2O3–TiO2 Nanocomposites for Enhanced Visible-Light Photocatalytic Applications. Dalton Transactions, 44, 16024–16035 https://doi.org/10.1039/c5dt02983j.

Juma, A.O., Acik, I.O., Mikli, V., Mere, A., and Krunks, M., 2015. Effect of Solution Composition on Anatase to Rutile Transformation of Sprayed TiO2 Thin Films. Thin Solid Films, 594, 1–6. https://doi.org/10.1016/j.tsf.2015.03.036.

Kaftelen-Odabaşi, H., 2024. Evaluation of Morphological, Structural, Thermal, Electrical, and Chemical Composition Properties of Graphene Oxide, and Reduced Graphene Oxide Obtained by Sequential Reduction Methods. Carbon Trends, 17, 1–10. https://doi.org/10.1016/j.cartre.2024.100429.

Khalafu, S.H.S., Wan Aida, W.M., Lim, S.J., and Maskat, M.Y., 2017. Effects of Deodorisation Methods on Volatile Compounds, Chemical Properties and Antioxidant Activities of Fucoidan Isolated from Brown Seaweed (Sargassum sp.). Algal Research, 25, 507–515. https://doi.org/10.1016/j.algal.2017.06.018.

Khasawneh, O.F.S., and Palaniandy, P., 2020. Removal of Organic Pollutants from Water by Fe2O3/TiO2 Based Photocatalytic Degradation : A Review. Environmental Technology & Innovation, 30, 1–20. https://doi.org/10.1016/j.eti.2020.101230.

Khavar, C.A.H., Moussavi, G., and Mahjoub, A.R. 2018. The preparation of TiO2 @rGO Nanocomposite efficiently Activated with UVA/LED and H2O2 for High Rate Oxidation Of Acetaminophen: Catalyst Characterization and Acetaminophen Degradation and Mineralization. Applied Surface Science, 440, 963–973. https://doi.org/10.1016/j.apsusc.2018.01.238.

Lavelim, B., Destiarti, L., Adhitiyawarman, A., and Sasri, R., 2023. Synthesis of Reduced Graphene Oxide-Bentonite Composite and Its Application as a Lead (II) Ion Adsorbent. Indonesian Journal of Chemistry, 23, 1–11. https://doi.org/10.22146/ijc.67993.

Li, Y., Zheng, Y., Zhang, Y., Yang, Y., Wang, P., Imre, B., Wong, A.C.Y., Hsieh, Y.S.Y., and Wang, D., 2021. Brown Algae Carbohydrates: Structures, Pharmaceutical Properties, and Research Challenges. Marine Drugs, 19, 1–21. https://doi.org/10.3390/md19110620.

Magro, M.R., Vella, D.A., and Cassar, G., 2025. Synthesis of Graphene Oxide: A Refined Approach. Carbon Trends, 20, 100509. https://doi.org/10.1016/j.cartre.2025.100509.

Mei, Q., Zhang, F., Wang, N., Yang, Y., Wu, R., and Wang, W., 2019. TiO2/Fe2O3 Heterostructures with Enhanced Photocatalytic Reduction of Cr(VI) under Visible Light Irradiation. Royal Society of Chemistry, 9, 22764–22771. https://doi.org/10.1039/c9ra03531a.

Mohamed, H.H., Alomair, N.A., Akhtar, S., and Youssef, T.E., 2019. Eco-Friendly Synthesized α-Fe2O3/TiO2 Heterojunction with Enhanced Visible Light Photocatalytic Activity. Journal of Photochemistry and Photobiology A: Chemistry, 382, 1–12. https://doi.org/10.1016/j.jphotochem.2019.111951.

Mohammadi, M., Sabbaghi, S., Binazadeh, M., Ghaedi, S., and Rajabi, H., 2023. Type-1 α-Fe2O3/TiO2 Photocatalytic Degradation of Tetracycline from Wastewater Using CCD-Based RSM Optimization. Chemosphere, 336, 1–13. https://doi.org/10.1016/j.chemosphere.2023.139311.

Padmanabhan, N.T., Nishanth, T., Louis, J., Mathew, D.T., Ganguly, P., John, H., and Pillai, S.C., 2021. Graphene Coupled TiO2 Photocatalysts for Environmental Applications: A review. Chemosphere, 271, 129506–129539. https://doi.org/10.1016/j.chemosphere.2020.129506.

Palanisamy, B., Babu, C.M., Sundaravel, B., Anandan, S., and Murugesan, V., 2013. Sol–Gel Synthesis of Mesoporous Mixed Fe2O3/TiO2 Photocatalyst : Application for Degradation of 4-Chlorophenol. Journal of Hazardous Materials, 252–253, 233–242. https://doi.org/10.1016/j.jhazmat.2013.02.060.

Prasad, G., Tamang, S., Jha, S., Bhattacharyya, N.K., and Biswas, J., 2025. A Theoretical Insight into Graphene-Based Materials: A DFT Study. Results in Surfaces and Interfaces, 18, 100463. https://doi.org/10.1016/j.rsurfi.2025.100463.

Rashid, M.M., Simončič, B., Zorc, M., Fink, R., Čelan Korošin, N., Šuligoj, A., Kovač, J., Jerman, I., and Tomšič, B., 2025. Synthesis of a New Amino/Phosphate-Modified TiO2/rGO Hybrid Nanocomposite for Sustainable Textile Functionalization. Journal of Environmental Chemical Engineering, 13, 1–19. https://doi.org/10.1016/j.jece.2025.116555.

Rathi, V.H., Rejo, A., and Jayakumar, K., 2023. Applied Surface Science Advances Green Synthesis of Ag/CuO and Ag/TiO2 Nanoparticles for Enhanced Photocatalytic Dye Degradation, Antibacterial, and Antifungal Properties. Applied Surface Science Advances, 18, 1–13. https://doi.org/10.1016/j.apsadv.2023.100476.

Roopa, M.C., Kallimani, S., Thirumala, S., and Mylarappa, M., 2026. Synthesis and Development of rGO/ZnO Composite for Photocatalytic Studies, Next Materials, 12, 102217. https://doi.org/10.1016/j.nxmate.2026.102217.

Sari, U.R.K., Wahyuningsih, S., and Ramelan, A., 2019. Preparation of Fe2O3-TiO2/GO Composites as a Visible Light Oxidation Photocatalyst Material. IOP Conference Series: Materials Science and Engineering, 578, 1–8. https://doi.org/10.1088/1757-899X/578/1/012042.

Septiyanti, M., Liana, L., Sutriningsih, S., Kumayanjati, B., and Meliana, Y., 2019. Formulation and Evaluation of Serum from Red, Brown and Green Algae Extract for Anti- Aging Base Material Formulation and Evaluation of Serum from Red, Brown and Green Algae Extract for Anti-Aging Base Material. AIP Conference Proceedings, 2175, 1–12.

Silerio-Vázquez, F. de J., González-Burciaga, L.A., Antileo, C., Núñez-Núñez, C.M., and Proal-Nájera, J.B., 2024. Photocatalytic Degradation of Antibiotics in Water via TiO2-x: Research Needs for Technological Advancements. Journal of Hazardous Materials Advances, 16, 1–20. https://doi.org/10.1016/j.hazadv.2024.100506.

Sobuj, M.K.A., Shemul, M.S., Islam, M.S., Islam, M.A., Mely, S.S., Ayon, M.H., Pranto, S.M., Alam, M.S., Bhuiyan, M.S., and Rafiquzzaman, S.M., 2024. Qualitative and Quantitative Phytochemical Analysis of Brown Seaweed Sargassum Polycystum Collected from Bangladesh with Its Antioxidant Activity Determination. Food Chemistry Advances, 4, 1–9. https://doi.org/10.1016/j.focha.2023.100565.

Utami, M., Yenn, T.W., Alam, M.W., Ravindran, B., Husniati, Purnama, I., Salmahaminati, Hidayat, H., Dhetaya, F.N., and Salsabilla, S.N., 2024. Efficient Photocatalytic Bactericidal Performance of Green-Synthesised TiO2/Reduced Graphene Oxide Using Banana Peel Extracts. Heliyon, 10, 1–20. https://doi.org/10.1016/j.heliyon.2024.e26636.

Xu, C., Yuan, R. S., and Wang, X., 2014. Selective Reduction of Graphene Oxide. New Carbon Materials, 29, 61–66. https://doi.org/10.1016/S1872-5805(14)60126-8.

Xu, L., Zhang, H., Xiong, P., Zhu, Q., Liao, C., and Jiang, G., 2021. Occurrence, Fate, and Risk Assessment of Typical Tetracycline Antibiotics in the Aquatic Environment: A Review. Science of the Total Environment, 753, 1–17. https://doi.org/10.1016/j.scitotenv.2020.141975.

Yang, H., 2021. Short Review A Short Review on Heterojunction Photocatalysts: Carrier Transfer Behavior and Photocatalytic Mechanisms. Materials Research Bulletin, 142, 1–9. https://doi.org/10.1016/j.materresbull.2021.111406.

Zajac, A.T., Synowiec, M., Zakrzewska, K., Zazakowny, K., Kowalski, K., Dziedzic, A., and Radecka, M., 2022. Scavenger-Supported Photocatalytic Evidence of an Extended Type I Electronic Structure of the Fe2O3@TiO2 Interface. Applied Materials & Interfaces, 14, 38255–38269. https://doi.org/10.1021/acsami.2c06404.

Zhang, J., Zhou, P., Liu, J., and Yu, J., 2014. New Understanding of the Difference of Photocatalytic Activity among Anatase, Rutile and Brookite TiO2. Physical Chemistry Chemical Physics, 16, 20382–20386. https://doi.org/10.1039/C4CP02201G.

Zheng, R., Yang, D., Chen, Y., Bian, Z., and Li, H., 2023. Fe2O3/TiO2/Reduced Graphene Oxide-Driven Recycled Visible-Photocatalytic Fenton Reactions to Mineralize Organic Pollutants in a Wide PH Range. Journal of Environmental Sciences, 134, 11–20. https://doi.org/10.1016/j.jes.2022.01.042.

DOI: https://doi.org/10.20961/alchemy.22.2.123560.452-462

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