* Corresponding Author
Advanced Oxidation Processes of Amoxicillin Based on Visible Light Active Nitrogen-Doped TiO2 Photocatalyst
https://doi.org/10.22146/ijc.81387 Kusuma Putri Suwondo(1), Nurul Hidayat Aprilita(2), Endang Tri Wahyuni(3*)
(1) Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Gadjah Mada, Sekip Utara, Yogyakarta 55281, Indonesia
(2) Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Gadjah Mada, Sekip Utara, Yogyakarta 55281, Indonesia
(3) Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Gadjah Mada, Sekip Utara, Yogyakarta 55281, Indonesia
(*) Corresponding Author
Abstract
Environmental consequences during the COVID-19 pandemic have attracted attention due to the excessive use of antibiotics which lead to the release of the drug's residue, such as amoxicillin (AMX), into the environment. In this work, an advanced oxidation process based on a visible, active N-doped TiO2 photocatalyst was carried out to eliminate AMX. Nitrogen with different initial doping concentrations (15, 30, 45% w/w) was doped into TiO2 by the sol-gel method. The characterization technique such as XRD, FTIR, UV-SRS, and SEM-EDX revealed that nitrogen with 30% doping concentration improved the TiO2 response in the visible region, attributed to the lower band gap energy (2.97 eV). In the photodegradation processes, the TiO2-N (30%) photocatalyst possessed higher AMX degradation than undoped TiO2 for both UV and visible light irradiation. In an aqueous solution, the degradation percentage of AMX by TiO2-N (30%) was 68.5 and 84.12%, while the degradation percentage of AMX by TiO2 was 38.7 and 78.01% under visible and UV light, respectively.
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[1] Center for Systems Science and Engineering (CSSE) at Johns Hopkins University, 2023, COVID-19 Dashboard [Updated 2023 January], https://coronavirus.jhu.edu/, accessed on January 10, 2023.
[2] Langford, B.J., So, M., Raybardhan, S., Leung, V., Soucy, J.P.R., Westwood, D., Daneman, N., and MacFadden, D.R., 2021, Antibiotic prescribing in patients with COVID-19: Rapid review and meta-analysis, Clin. Microbiol. Infect., 27 (4), 520–531.
[3] Salimi, M., Behbahani, M., Sobhi, H.R., Gholami, M., Jonidi Jafari, A., Rezaei Kalantary, R., Farzadkia, M., and Esrafili, A., 2019, A new nano-photocatalyst based on Pt and Bi co-doped TiO2 for efficient visible-light photo degradation of amoxicillin, New J. Chem., 43 (3), 1562–1568.
[4] Munguia, J., and Nizet, V., 2018, Pharmacological targeting of the host-pathogen interaction: Alternatives to classical antibiotics to combat drug-resistant superbugs, Trends Pharmacol. Sci., 38 (5), 473–488.
[5] Comber, S.D.W., Upton, M., Lewin, S., Powell, N., and Hutchinson, T.H., 2020, COVID-19, antibiotics and one health: A UK environmental risk assessment, J. Antimicrob. Chemother., 75 (11), 3411–3412.
[6] Alygizakis, N.A., Gago-Ferrero, P., Borova, V.L., Pavlidou, A., Hatzianestis, I., and Thomaidis, N.S., 2016, Occurrence and spatial distribution of 158 pharmaceuticals, drugs of abuse and related metabolites in offshore seawater, Sci. Total Environ., 541, 1097–1105.
[7] Khan, A.H., Khan, N.A., Ahmed, S., Dhingra, A., Singh, C.P., Khan, S.U., Mohammadi, A.A., Changani, F., Yousefi, M., Alam, S., Vambol, S., Vambol, V., Khursheed, A., and Ali, I., 2020, Application of advanced oxidation processes followed by different treatment technologies for hospital wastewater treatment, J. Cleaner Prod., 269, 122411.
[8] Cuerda-Correa, E.M., Alexandre-Franco, M.F., and Fernández-González, C., 2020, Advanced oxidation processes for the removal of antibiotics from water. An overview, Water, 12 (1), 102.
[9] Wang, J., and Zhuan, R., 2020, Degradation of antibiotics by advanced oxidation processes: An overview, Sci. Total Environ., 701, 135023.
[10] Byrne, C., Subramanian, G., and Pillai, S.C., 2018, Recent advances in photocatalysis for environmental applications, J. Environ. Chem. Eng., 6 (3), 3531–3555.
[11] Balarak, D., and Mostafapour, F.K., 2019, Photocatalytic degradation of amoxicillin using UV/Synthesized NiO from pharmaceutical wastewater, Indones. J. Chem., 19 (1), 211–218.
[12] Elmolla, E.S., and Chaudhuri, M., 2010, Photocatalytic degradation of amoxicillin, ampicillin and cloxacillin antibiotics in aqueous solution using UV/TiO2 and UV/H2O2/TiO2 photocatalysis, Desalination, 252 (1-3), 46–52.
[13] Moradi, M., Hasanvandian, F., Isari, A.A., Hayati, F., Kakavandi, B., and Setayesh, S.R., 2021, CuO and ZnO co-anchored on g-C3N4 nanosheets as an affordable double Z-scheme nanocomposite for photocatalytic decontamination of amoxicillin, Appl. Catal., B, 285, 119838.
[14] Chinnaiyan, P., Thampi, S.G., Kumar, M., and Balachandran, M., 2019, Photocatalytic degradation of metformin and amoxicillin in synthetic hospital wastewater: Effect of classical parameters, Int. J. Environ. Sci. Technol., 16 (10), 5463–5474.
[15] Dimitrakopoulou, D., Rethemiotaki, I., Frontistis, Z., Xekoukoulotakis, N.P., Venieri, D., and Mantzavinos, D., 2012, Degradation, mineralization and antibiotic inactivation of amoxicillin by UV-A/TiO2 photocatalysis, J. Environ. Manage., 98, 168–174.
[16] Xing, X., Du, Z., Zhuang, J., and Wang, D., 2018, Removal of ciprofloxacin from water by nitrogen doped TiO2 immobilized on glass spheres: Rapid screening of degradation products, J. Photochem. Photobiol., A, 359, 23–32.
[17] Wetchakun, K., Wetchakun, N., and Sakulsermsuk, S., 2019, An overview of solar/visible light-driven heterogeneous photocatalysis for water purification: TiO2- and ZnO-based photocatalysts used in suspension photoreactors, J. Ind. Eng. Chem., 71, 19–49.
[18] Bergamonti, L., Graiff, C., Bergonzi, C., Potenza, M., Reverberi, C., Ossiprandi, M.C., Lottici, P.P., Bettini, R., and Elviri, L., 2022, Photodegradation of pharmaceutical pollutants: New photocatalytic systems based on 3D printed scaffold-supported Ag/TiO2 nanocomposite, Catalysts, 12 (6), 580.
[19] Lalliansanga, L., Tiwari, D., Lee, S.M., and Kim, D.J., 2022, Photocatalytic degradation of amoxicillin and tetracycline by template synthesized nano-structured Ce3+@TiO2 thin film catalyst, Environ. Res., 210, 112914.
[20] Çağlar Yılmaz, H., Akgeyik, E., Bougarrani, S., El Azzouzi, M., and Erdemoğlu, S., 2020, Photocatalytic degradation of amoxicillin using Co-doped TiO2 synthesized by reflux method and monitoring of degradation products by LC–MS/MS, J. Dispersion Sci. Technol., 41 (3), 414–425.
[21] Mhemid, R.K.S., Salman, M.S., and Mohammed, N.A., 2022, Comparing the efficiency of N-doped TiO2 and commercial TiO2 as photo catalysts for amoxicillin and ciprofloxacin photodegradation under solar irradiation, J. Environ. Sci. Health, Part A: Toxic/Hazard. Subst. Environ. Eng., 57 (9), 813–829.
[22] Gomes, J., Lincho, J., Domingues, E., Quinta-Ferreira, R.M., and Martins, R.C., 2019, N-TiO2 photocatalysts: A review of their characteristics and capacity for emerging contaminants removal, Water, 11 (2), 373.
[23] Zhao, W., Liu, S., Zhang, S., Wang, R., and Wang, K., 2019, Preparation and visible-light photocatalytic activity of N-doped TiO2 by plasma-assisted sol-gel method, Catal. Today, 337, 37–43.
[24] Asahi, R., Morikawa, T., Irie, H., and Ohwaki, T., 2014, Nitrogen-doped titanium dioxide as visible-light-sensitive photocatalyst: Designs, developments, and prospects, Chem. Rev., 114 (19), 9824–9852.
[25] Nolan, N.T., Synnott, D.W., Seery, M.K., Hinder, S.J., Van Wassenhoven, A., and Pillai, S.C., 2012, Effect of N-doping on the photocatalytic activity of sol-gel TiO2, J. Hazard. Mater., 211-212, 88–94.
[26] Verma, M., and Haritash, A.K., 2020, Photocatalytic degradation of Amoxicillin in pharmaceutical wastewater: A potential tool to manage residual antibiotics, Environ. Technol. Innovation, 20, 101072.
[27] Hanaor, D.A.H., and Sorrell, C.C., 2011, Review of the anatase to rutile phase transformation, J. Mater. Sci., 46 (4), 855–874.
[28] Odling, G., and Robertson, N., 2015, Why is anatase a better photocatalyst than rutile? The importance of free hydroxyl radicals, ChemSusChem, 8 (11), 1838–1840.
[29] Zhao, Z., Omer, A.A., Qin, Z., Osman, S., Xia, L., and Singh, R.P., 2019, Cu/N-codoped TiO2 prepared by the sol-gel method for phenanthrene removal under visible light irradiation, Environ. Sci. Pollut. Res., 27 (15), 17530–17540.
[30] Li, H., Hao, Y., Lu, H., Liang, L., Wang, Y., Qiu, J., Shi, X., Wang, Y., and Yao, J., 2015, A systematic study on visible-light N-doped TiO2 photocatalyst obtained from ethylenediamine by sol-gel method, Appl. Surf. Sci., 344, 112–118.
[31] Yang, G., Jiang, Z., Shi, H., Xiao, T., and Yan, Z., 2010, Preparation of highly visible-light active N-doped TiO2 photocatalyst, J. Mater. Chem., 20 (25), 5301–5309.
[32] Huo, Y., Jin, Y., Zhu, J., and Li, H., 2009, Highly active TiO2-x-yNxFy visible photocatalyst prepared under supercritical conditions in NH4F/EtOH fluid, Appl. Catal., B, 89 (3-4), 543–550.
[33] Cheng, X., Yu, X., and Xing, Z., 2012, Characterization and mechanism analysis of N doped TiO2 with visible light response and its enhanced visible activity, Appl. Surf. Sci., 258 (7), 3244–3248.
[34] Liu, C., Yu, T., Tan, X., and Huang, X., 2017, Comparison N-Cu–codoped nanotitania and N-doped nanotitania in photocatalytic reduction of CO2 under UV light, Inorg. Nano-Met. Chem., 47 (1), 9–14.
[35] Reda, S.M., Khairy, M., and Mousa, M.A., 2020, Photocatalytic activity of nitrogen and copper doped TiO2 nanoparticles prepared by microwave-assisted sol-gel process, Arabian J. Chem., 13 (1), 86–95.
[36] Wang, H., Yang, X., Xiong, W., and Zhang, Z., 2015, Photocatalytic reduction of nitroarenes to azo compounds over N-doped TiO2: Relationship between catalysts and chemical reactivity, Res. Chem. Intermed., 41 (6), 3981–3997.
[37] Etacheri, V., Seery, M.K., Hinder, S.J., and Pillai, S.C., 2010, Highly visible light active TiO2-xNx heterojunction photocatalysts, Chem. Mater., 22 (13), 3843–3853.
[38] Bergamonti, L., Bergonzi, C., Graiff, C., Lottici, P.P., Bettini, R., and Elviri, L., 2019, 3D printed chitosan scaffolds: A new TiO2 support for the photocatalytic degradation of amoxicillin in water, Water Res., 163, 114841.
[39] Kanakaraju, D., Kockler, J., Motti, C.A., Glass, B.D., and Oelgemöller, M., 2015, Titanium dioxide/zeolite integrated photocatalytic adsorbents for the degradation of amoxicillin, Appl. Catal., B, 166-167, 45–55.
[40] Moreira, N.F.F., Orge, C.A., Ribeiro, A.R., Faria, J.L., Nunes, O.C., Pereira, M.F.R., and Silva, A.M.T., 2015, Fast mineralization and detoxification of amoxicillin and diclofenac by photocatalytic ozonation and application to an urban wastewater, Water Res., 87, 87–96.
[41] Gar Alalm, M., Tawfik, A., and Ookawara, S., 2016, Enhancement of photocatalytic activity of TiO2 by immobilization on activated carbon for degradation of pharmaceuticals, J. Environ. Chem. Eng., 4 (2), 1929–1937.
[42] Klauson, D., Babkina, J., Stepanova, K., Krichevskaya, M., and Preis, S., 2010, Aqueous photocatalytic oxidation of amoxicillin, Catal. Today, 151 (1-2), 39–45.
[43] Wahyuni, E.T., Yulikayani, P.Y., and Aprilita, N.H., 2020, Enhancement of visible-light photocatalytic activity of Cu-doped TiO2 for photodegradation of amoxicillin in water, J. Mater. Environ. Sci., 11 (4), 670–683.
[44] Nguyen, T.L., Pham, T.H., Viet, N.M., Thang, P.Q., Rajagopal, R., Sathya, R., Jung, S.H., and Kim, T., 2022, Improved photodegradation of antibiotics pollutants in wastewaters by advanced oxidation process based on Ni-doped TiO2, Chemosphere, 302, 134837.
DOI: https://doi.org/10.22146/ijc.81387
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