Page Header

Home > ONLINE FIRST > Thao

Exploring the Mechanism for the Photocatalytic Degradation of Oxytetracycline in Water using TiO2 and Supplementary Oxidants

Tran Quoc Thao, Ngo Thi Thu Hien, Phan Thanh Lam, Nguyen Nhat Huy, Pham Tan Thi, Nguyen Trung Thanh, Phan Phuoc Toan, Le Tri Thich, Nguyen Thi Thuy

Abstract


The persistent presence of antibiotics in wastewater, exemplified by oxytetracycline (OTC), poses environmental risks, necessitating robust removal strategies. This study investigates the effectiveness of photocatalysis utilizing TiO2 (P25) treated at various temperatures, combined with different oxidants such as hydrogen peroxide (H2O2), potassium peroxydisulfate (PDS), potassium peroxomonosulfate (PMS) under diverse experimental conditions. The research systematically explores the impact of temperature, pH, and oxidant concentration on the efficiency of OTC degradation. Our findings reveal that the combination of P25/500, PDS, UV irradiation, and stirring demonstrates superior OTC degradation, surpassing 99% efficiency after 180 min. Optimal pH conditions are identified, emphasizing the importance of balancing acidity for enhanced performance. The study also provides insights into the optimal PDS concentration, indicating a threshold beyond which further increases yield diminishing returns. Mechanistic understanding is enhanced through scavenger experiments, elucidating the pivotal role of reactive oxygen species, particularly O2•−, in the photocatalytic process. This research offers a practical framework for TiO2-based photocatalysis in wastewater treatment, emphasizing tailored conditions for efficient antibiotic removal. The outcomes contribute valuable insights to the development of sustainable wastewater treatment protocols targeting antibiotic pollutants.

Keywords



[1]    P. Huo, X. Gao, Z. Lu, X. Liu, Y. Luo, W. Xing, J. Li, and Y. Yan, “Photocatalytic degradation of antibiotics in water using metal ion@ TiO2/HNTs under visible light,” Desalination and Water Treatment, vol. 52, pp. 6985–6995, 2014.

[2]    P. T. P. Hoa, S. Managaki, N. Nakada, H. Takada, A. Shimizu, D. H. Anh, P. H. Viet, and S. Suzuki, “Antibiotic contamination and occurrence of antibiotic-resistant bacteria in aquatic environments of northern Vietnam,” Science of the Total Environment, vol. 409, pp. 2894–2901, 2011.

[3]    M. Teuber, “Veterinary use and antibiotic resistance,” Current opinion in microbiology, vol. 4, pp. 493–499, 2001.

[4]    D. A. Goff, R. Kullar, E. J. Goldstein, M. Gilchrist, D. Nathwani, A. C. Cheng, K. A. Cairns, K. Escandón-Vargas, M. V. Villegas, and A. Brink, “A global call from five countries to collaborate in antibiotic stewardship: united we succeed, divided we might fail,” The Lancet Infectious Diseases, vol. 17, pp. e56–e63, 2017.

[5]    E. Y. Klein, M. Milkowska-Shibata, K. K. Tseng, M. Sharland, S. Gandra, C. Pulcini, and R. Laxminarayan, “Assessment of WHO antibiotic consumption and access targets in 76 countries, 2000–15: An analysis of pharmaceutical sales data,” The Lancet Infectious Diseases, vol. 21, pp. 107–115, 2021.

[6]    A. J. Browne, M. G. Chipeta, G. Haines-Woodhouse, E. P. Kumaran, B. H. K. Hamadani, S. Zaraa, N. J. Henry, A. Deshpande, R. C. Reiner, and N. P. Day, “Global antibiotic consumption and usage in humans, 2000–18: A spatial modelling study,” The Lancet Planetary Health, vol. 5, pp. e893–e904, 2021.

[7]    P. K. Thai, L. X. Ky, V. N. Binh, P. H. Nhung, P. T. Nhan, N. Q. Hieu, N. T. T. Dang, N. K. B. Tam, and N. T. K. Anh, “Occurrence of antibiotic residues and antibiotic-resistant bacteria in effluents of pharmaceutical manufacturers and other sources around Hanoi, Vietnam,” Science of The Total Environment, vol. 645, pp. 393–400, 2018.

[8]    Y. Ben, C. Fu, M. Hu, L. Liu, M. H. Wong, and C. Zheng, “Human health risk assessment of antibiotic resistance associated with antibiotic residues in the environment: A review,” Environmental Research, vol. 169, pp. 483–493, 2019.

[9]    J. L. Martinez, “Environmental pollution by antibiotics and by antibiotic resistance determinants,” Environmental Pollution, vol. 157, pp. 2893–2902, 2009.

[10]  Z.-j. LI, W.-n. QI, F. Yao, Y.-w. LIU, S. Ebrahim, and L. Jian, “Degradation mechanisms of oxytetracycline in the environment,” Journal of Integrative Agriculture, vol. 18, pp. 1953–1960, 2019.

[11]  M. L. Tran, S.-W. Deng, C.-C. Fu, and R.-S. Juang, “Efficient removal of antibiotic oxytetracycline from water using optimized montmorillonite-supported zero-valent iron nanocomposites,” Environmental Science and Pollution Research, vol. 27, pp. 30853–30867, 2020.

[12]  L. Q. Huong, T. T. T. Hang, P. T. Ngoc, C. V. Tuat, V. I. Erickson, and P. Padungtod, “Pilot monitoring of antimicrobial residues in chicken and pork in Vietnam,” Journal of Food Protection, vol. 83, pp. 1701–1706, 2020.

[13]  D. S. Shen, X. Q. Tao, J. L. Shentu, and M. Z. Wang, “Residues of veterinary antibiotics in pig feeds and manures in Zhejiang Province,” Advanced Materials Research, vol. 1010, pp. 301–304, 2014.

[14]  M. D. Hernando, M. Mezcua, A. R. Fernández-Alba, and D. Barceló, “Environmental risk assessment of pharmaceutical residues in wastewater effluents, surface waters and sediments,” Talanta, vol. 69, pp. 334–342, 2006.

[15]  N. Olama, M. Dehghani, and M. Malakootian, “The removal of amoxicillin from aquatic solutions using the TiO 2/UV-C nanophotocatalytic method doped with trivalent iron,” Applied Water Science, vol. 8, pp. 1–12, 2018.

[16]  W. Wang, X. Liu, J. Fang, and C. Lu, “TiO2@ g-C3N4 heterojunction with directional charge migration behavior for photodegradation of tetracycline antibiotics,” Materials Letters, vol. 236, pp. 622–624, 2019.

[17]  A. Fujishima and X. Zhang, “Titanium dioxide photocatalysis: Present situation and future approaches,” Comptes Rendus Chimie, vol. 9, pp. 750–760, 2006.

[18]  M. Farzadkia, E. Bazrafshan, A. Esrafili, J.-K. Yang, and M. Shirzad-Siboni, “Photocatalytic degradation of Metronidazole with illuminated TiO2 nanoparticles,” Journal of Environmental Health Science and Engineering, vol. 13, pp. 1–8, 2015.

[19]  N. T. C. Tien, T. T. B. Huyen, N. T. Thuy, D. Van Thanh, N. T. Thanh, and N. N. Huy, “Degradation of enrofloxacin by photocatalysis using titanium dioxide nanomaterials,” in IOP Conference Series: Earth and Environmental Science, 2021, Art. no. 012033.

[20]  B. Kakavandi, N. Bahari, R. R. Kalantary, and E. D. Fard, “Enhanced sono-photocatalysis of tetracycline antibiotic using TiO2 decorated on magnetic activated carbon (MAC@ T) coupled with US and UV: A new hybrid system,” Ultrasonics Sonochemistry, vol. 55, pp. 75–85, 2019.

[21]  Q. Cai and J. Hu, “Effect of UVA/LED/TiO2 photocatalysis treated sulfamethoxazole and trimethoprim containing wastewater on antibiotic resistance development in sequencing batch reactors,” Water Research, vol. 140, pp. 251–260, 2018.

[22]  A. Mekkaoui, E. G. Temam, S. Rahmane, and B. Gasmi, “A new study on the effect of pure anatase TiO2 film thickness on gentian violet photodegradation under sunlight: Considering the effect of hole scavengers,” Trends in Sciences, vol. 20, p. 3766, 2023.

[23]  M. Althamthami, E. Guettaf Temam, H. B. Temam, R. Saad, and G. G. Hasan, “Improved photocatalytic activity under the sunlight of high transparent hydrophilic Bi-doped TiO2 thin-films,” Journal of Photochemistry and Photobiology A: Chemistry, vol. 443, 2023, Art. no. 114818.

[24]  E. Guettaf Temam, F. Djani, S. Rahmane, H. Ben Temam, and B. Gasmi, “Photocatalytic activity of Al/Ni doped TiO2 films synthesized by sol-gel method: Dependence on thickness and crystal growth of photocatalysts,” Surfaces and Interfaces, vol. 31, 2022, Art. no. 102077.

[25]  C. Sriwong, K. Choojun, and S. Sriwong, “High photocatalytic performance of 3D porous-structured TiO2@ natural rubber hybrid sheet on the removal of indigo carmine dye in water,” SN Applied Sciences, vol. 1, p. 864, 2019.

[26]  H. Znad and Y. Kawase, “Synthesis and characterization of S-doped Degussa P25 with application in decolorization of Orange II dye as a model substrate,” Journal of Molecular Catalysis A: Chemical, vol. 314, pp. 55–62, 2009.

[27]  J. C. Yu, J. Yu, W. Ho, Jiang, and Zhang, “Effects of F-doping on the photocatalytic activity and microstructures of nanocrystalline TiO2 powders,” Chemistry of Materials, vol. 14, pp. 3808–3816, 2002.

[28]  F. Scarpelli, T. F. Mastropietro, T. Poerio, and N. Godbert, “Mesoporous TiO2 thin films: State of the art,” Titanium Dioxide-Material for a Sustainable Environment, vol. 508, pp. 135–142, 2018.

[29]  M. Takeuchi, G. Martra, S. Coluccia, and M. Anpo, “Investigations of the structure of H2O clusters adsorbed on TiO2 surfaces by near-infrared absorption spectroscopy,” The Journal of Physical Chemistry B, vol. 109, pp. 7387–7391, 2005.

[30]  E. Felis, M. Buta-Hubeny, W. Zieliński, J. Hubeny, M. Harnisz, S. Bajkacz, and E. Korzeniewska, “Solar-light driven photodegradation of antimicrobials, their transformation by-products and antibiotic resistance determinants in treated wastewater,” Science of The Total Environment, vol. 836, 2022, Art. no. 155447.

[31]  X. Jin, H. Xu, S. Qiu, M. Jia, F. Wang, A. Zhang, and X. Jiang, “Direct photolysis of oxytetracycline: Influence of initial concentration, pH and temperature,” Journal of Photochemistry and Photobiology A: Chemistry, vol. 332, pp. 224–231, 2017.

[32]  G. Dong, B. Chen, B. Liu, L. J. Hounjet, Y. Cao, S. R. Stoyanov, M. Yang, and B. Zhang, “Advanced oxidation processes in microreactors for water and wastewater treatment: Development, challenges, and opportunities,” Water Research, vol. 211, 2022, Art. no. 118047.

[33]  M. Sharma, A. Yadav, M. Mandal, and K. Dubey, “TiO2 based photocatalysis: A valuable approach for the removal of pharmaceuticals from aquatic environment,” International Journal of Environmental Science and Technology, vol. 20, pp. 4569–4584, 2023.

[34]  R. Sabouni and H. Gomaa, “Comparative analysis of aeration and oscillation in a suspended catalyst photocatalytic membrane reactor,” Chemical Engineering Research and Design, vol. 173, pp. 55–62, 2021.

[35]  E. Azadi, A. Akbar Zinatizadeh, D. Yazdani, M. Sillanpää, and M. Joshaghani, “The photodegradation of oxytetracycline by Degussa P25-TiO2/FeO/ZnO ternary chain heterojunction in the presence of persulfate under visible light irradiation: The optimization and kinetic study,” Inorganic Chemistry Communications, vol. 166, 2024, Art. no. 112600.

[36]  Y. Zhang, Q. Chen, H. Qin, J. Huang, and Y. Yu, “Identification of reactive oxygen species and mechanism on visible light-induced photosensitized degradation of oxytetracycline,” International Journal of Environmental Research and Public Health, vol. 19, no. 23, 2022, Art. no. 15550.

[37]  S. Giannakis, K.-Y. A. Lin, and F. Ghanbari, “A review of the recent advances on the treatment of industrial wastewaters by Sulfate Radical-based Advanced Oxidation Processes (SR-AOPs),” Chemical Engineering Journal, vol. 406, 2021, Art. no. 127083.

[38]  F. Zaaboul, C. Haoufazane, A. Kari, R. Salim, K. Azzaoui, R. Sabbahi, and A. El Hourch, “Study of Reactive blue 203 removal by TiO2-P25 adsorption combined with photocatalysis for its degradation,” Moroccan Journal of Chemistry, vol. 12, pp. 1664–1682, 2024.

[39]  Y. Xin, P. Zhang, J. Shen, and S. Ren, “Development of vitamin B6-mediated biochar with nano zero-valent iron coating for oxytetracycline removal through adsorption and degradation under harsh acidic conditions,” Water, vol. 14, no. 17, p. 2734, 2022.

[40]  Y. Chen, K. Zhu, W. Qin, Z. Jiang, Z. Hu, M. Sillanpää, and K. Yan, “Enhanced electron transfer using NiCo2O4@ C hollow nanocages with an electron-shuttle effect for efficient tetracycline degradation,” Chemical Engineering Journal, vol. 488, 2024, Art. no. 150786.

[41]  L. He, H. Li, J. Wang, Q. Gao, and X. Li, “Peroxymonosulfate activation by Co-doped magnetic Mn3O4 for degradation of oxytetracycline in water,” Environmental Science and Pollution Research, vol. 29, pp. 39249–39265, 2022.

[42]  J. Xu, H. Zhang, J. Ma, L. Zhou, Q. Zhao, and Z. Ye, “A polystyrene resin in situ supported PANI/Fe3O4 composite as a heterogeneous Fenton catalyst for the efficient degradation of tetracycline in water,” Journal of Materials Chemistry A, vol. 12, pp. 22180–22200, 2024.

[43]  P. T. Le, T. P. Nguyen, T. H. Do, H. N. Nguyen, T. M. T. Dinh, T. T. Phan, T. Tsubota, and T. D. Nguyen, “Synergistic effect of the heterojunction gC3N4/Bi2MoO6/clinoptilolite to enhance the photocatalytic degradation of antibiotics in water in the presence of persulfate,” Environmental Science: Water Research & Technology, vol. 10, pp. 2665–2687, 2024.

[44]  Z. S. Wei, X. L. Chen, Z. S. Huang, H. Y. Jiao, and X. L. Xiao, “Insights into the removal of gaseous oxytetracycline by combined ozone and membrane biofilm reactor,” Environmental Engineering Research, vol. 27, pp. 210469–210470, 2021.

[45]  A. V. Demyanenko, A. S. Bogomolov, N. V. Dozmorov, A. I. Svyatova, A. P. Pyryaeva, V. G. Goldort, S. A. Kochubei, and A. V. Baklanov, “Singlet oxygen 1O2 in photocatalysis on TiO2. Where does it come from?,” The Journal of Physical Chemistry C, vol. 123, pp. 2175–2181, 2019.

[46]  N. T. Dung, P. T. H. Hanh, V. D. Thao, N. T. Thuy, D. T. M. Thanh, N. T. Phuong, K.-Y. A. Lin, and N. N. Huy, “Decomposition and mineralization of glyphosate herbicide in water by radical and non-radical pathways through peroxymonosulfate activation using Co3O4/gC3 N4: A comprehensive study,” Environmental Science: Water Research & Technology, vol. 9, pp. 221–234, 2023.

[47]  I. Arora, H. Chawla, A. Chandra, S. Sagadevan, and S. Garg, “Advances in the strategies for enhancing the photocatalytic activity of TiO2: Conversion from UV-light active to visible-light active photocatalyst,” Inorganic Chemistry Communications, vol. 143, 2022, Art. no. 109700.

[48]  S. P. Mulakov, P. M. Gotovtsev, A. A. Gainanova, G. V. Kravchenko, G. M. Kuz’micheva, and V. V. Podbel’skii, “Generation of the Reactive Oxygen Species on the surface of nanosized titanium (IV) oxides particles under UV-irradiation and their connection with photocatalytic properties,” Journal of Photochemistry and Photobiology A: Chemistry, vol. 393, 2020, Art. no. 112424.

[49]  M. G. Kim, J. M. Kang, J. E. Lee, K. S. Kim, K. H. Kim, M. Cho, and S. G. Lee, “Effects of calcination temperature on the phase composition, photocatalytic degradation, and virucidal activities of TiO2 nanoparticles,” ACS Omega, vol. 6, pp. 10668–10678, 2021.

[50]  N. Mediouni, F. Dappozze, L. Khrouz, S. Parola, A. B. H. Amara, H. B. Rhaiem, N. Jaffrezic-Renault, P. Namour, and C. Guillard, “Correlation between Photocatalytic Properties of ZnO and Generation of Hydrogen Peroxide—Impact of Composite ZnO/TiO2 Rutile and Anatase,” Catalysts, vol. 12, p. 1445, 2022.

[51]  M. Ge, Z. Hu, J. Wei, Q. He, and Z. He, “Recent advances in persulfate-assisted TiO2-based photocatalysis for wastewater treatment: Performances, mechanism and perspectives,” Journal of Alloys and Compounds, vol. 888, 2021, Art. no. 161625.

[52]  A. A. Babaei, M. Golshan, and B. Kakavandi, “A heterogeneous photocatalytic sulfate radical-based oxidation process for efficient degradation of 4-chlorophenol using TiO2 anchored on Fe oxides@ carbon,” Process Safety and Environmental Protection, vol. 149, pp. 35–47, 2021.

[53]  G. Zhang, L. Zhao, X. Hu, X. Zhu, and F. Yang, “Synergistic activation of sulfate by TiO2 nanotube arrays-based electrodes for berberine degradation: Insight into pH-dependant ORR-strengthened reactive radicals co-generation mechanism,” Applied Catalysis B: Environmental, vol. 313, 2022, Art. no. 121453.

[54]  W.-J. Xue, Y.-H. Cui, Z.-Q. Liu, S.-Q. Yang, J.-Y. Li, and X.-L. Guo, “Treatment of landfill leachate nanofiltration concentrate after ultrafiltration by electrochemically assisted heat activation of peroxydisulfate,” Separation and Purification Technology, vol. 231, 2020, Art. no. 115928.

[55]  J. Wang and S. Wang, “Reactive species in advanced oxidation processes: Formation, identification and reaction mechanism,” Chemical Engineering Journal, vol. 401, 2020, Art. no. 126158.

Full Text: PDF

DOI: 10.14416/j.asep.2024.11.007

Refbacks

  • There are currently no refbacks.


Copyright © 2024 by King Mongkut’s University of Technology North Bangkok. All rights reserved.