Abstract
Antibiotics are life-saving drugs that fight bacterial infections by killing or inhibiting their reproduction. However, the overuse and misuse of this drug can contaminate water as it can reach the water surface very quickly through various pathways. The consumption of contaminated water may lead to the development of antibiotic resistance, which has been proliferating across the world recently. Azithromycin (AZM), an essential antibiotic drug, has been identified in wastewater and surface water, prompting apprehension regarding its potential environmental and public health consequences. The present investigation assessed the efficacy of photocatalytic degradation of AZM in water samples under sunlight. Exploiting the surface chemistry and high surface area of cellulose nanocrystals (CNC), nanocomposites with high loading (80 wt%) of titanium dioxide (TiO2) nanoparticles on a minimal amount of scaffold (20 wt% CNC) were synthesized and used as catalysts. Maximum removal efficiency of 98.8% was achieved in 5 h at a catalyst dose of 175 mg/L for an AZM solution with 10 mg/L concentration. Synthesized CNC–TiO2 nanocomposites demonstrated superior performance both in terms of high degradation efficiency and lowest catalyst loading per the g of AZM compared the material reported in the literature for the degradation of AZM. In conclusion, CNC–TiO2 nanocomposites are highly effective catalysts for the photocatalytic degradation of AZM. The developed method further ensures the hygiene of water sources and prevents the spread of antibiotic resistance.
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References
Abdullahi SS, Güner S, Koseoglu Y, Musa IM, Adamu BI, Abdulhamid M (2016) Sımple method for the determınatıon of band gap of a nanopowdered sample usıng kubelka munk theory. J Niger Assoc Math Phys 35:241–246
Acha J, Jayaram P (2022) Enhanced sunlight assisted photocatalyst degradation of cefixime using TiO 2 / RuO 2 / CuO ternary nanosystem. Mater Lett 321:132419. https://doi.org/10.1016/j.matlet.2022.132419
Birošová L, Mackuľak T, Bodík I, Ryba J, Škubák J, Grabic R (2014) Pilot study of seasonal occurrence and distribution of antibiotics and drug resistant bacteria in wastewater treatment plants in Slovakia. Sci Total Environ 490:440–444. https://doi.org/10.1016/j.scitotenv.2014.05.030
Chen X, Mao SS (2007) Titanium dioxide nanomaterials: synthesis, properties, modifications and applications. Chem Rev 107(7):2891–2959. https://doi.org/10.1021/cr0500535
Chen X, Yao L, He J, Li J, Xu S, Li N, Zhu Y, Chen X, Zhu R (2023) Enhanced degradation of tetracycline under natural sunlight through the synergistic effect of Ag 3 PO 4 / MIL-101 ( Fe ) photocatalysis and Fenton catalysis : mechanism, pathway, and toxicity assessment. J Hazard Mater 449:131024. https://doi.org/10.1016/j.jhazmat.2023.131024
Čizmić M, Ljubas D, Rožman M, Ašperger D, Ćurković L, Babíc S (2019) Photocatalytic degradation of azithromycin by nanostructured TiO 2 film: kinetics, degradation products, and toxicity. Materials 16(6):873. https://doi.org/10.3390/ma12060873
Ćurković L, Ljubas D, Šegota S, Bačić I (2014) Photocatalytic degradation of Lissamine Green B dye by using nanostructured sol-gel TiO2 films. J Alloy Compd 604:309–316. https://doi.org/10.1016/j.jallcom.2014.03.148
Davoodi S, Dahrazma B, Goudarzi N, Gorji HG (2019) Adsorptive removal of azithromycin from aqueous solutions using raw and saponin-modified nano diatomite. Water Sci Technol 80(5):939–949. https://doi.org/10.2166/wst.2019.337
El-Yazbi AF, Khamis EF, Youssef RM, El-Sayed MA, Aboukhalil FM (2020) Green analytical methods for simultaneous determination of compounds having relatively disparate absorbance; application to antibiotic formulation of azithromycin and levofloxacin. Heliyon 6(9):e04819. https://doi.org/10.1016/j.heliyon.2020.e04819
Fair RJ, Tor Y (2014) Antibiotics and bacterial resistance in the 21st century. Perspect Med Chem 6:25–64. https://doi.org/10.4137/PMC.S14459
Feizi ZH, Fatehi P (2021) Changes in the molecular structure of cellulose nanocrystals upon treatment with solvents. Cellulose 28(11):7007–7020. https://doi.org/10.1007/s10570-021-03972-x
Goudarzi M, Hamzah Abdulhusain Z, Salavati-Niasari M (2023) Low-cost and eco-friendly synthesis of Mn-doped Tl2WO4 nanostructures for efficient visible light photocatalytic degradation of antibiotics in water. Sol Energy 262:111912. https://doi.org/10.1016/j.solener.2023.111912
Hamad H, Hamad H, Bailón-García E, Morales-Torres S, Pérez-Cadenas AF, Carrasco-Marín F & Maldonado-Hódar FJ (2020) Cellulose–TiO2 composites for the removal of water pollutants. Bio-Based materials and biotechnologies for eco-efficient construction, 329–358. https://doi.org/10.1016/B978-0-12-819481-2.00016-7
Imanipoor J, Mohammadi M, Dinari M (2021) Evaluating the performance of L-methionine modified montmorillonite K10 and 3-aminopropyltriethoxysilane functionalized magnesium phyllosilicate organoclays for adsorptive removal of azithromycin from water. Sep Purif Technol 275:119256. https://doi.org/10.1016/j.seppur.2021.119256
Kaushik M, Moores A (2016) Review: nanocelluloses as versatile supports for metal nanoparticles and their applications in catalysis. Green Chem 18(3):622–637. https://doi.org/10.1039/c5gc02500a
Kiely-Collins HJ, Sechi I, Brennan PE, McLaughlin MG (2018) Mild, calcium catalysed Beckmann rearrangements. Chem Commun 54(6):654–657. https://doi.org/10.1039/c7cc09491d
Kumar A, Rana A, Guo C, Sharma G, Mohammedsaleh K, Katubi M, Mohammed F, Naushad M, Sillanp M (2021) Acceleration of photo-reduction and oxidation capabilities of Bi4O5I2/SPION @ calcium alginate by metallic Ag: wide spectral removal of nitrate and azithromycin. Chem Eng J 423:130173–130181. https://doi.org/10.1016/j.cej.2021.130173
Li C, Jin H, Hou Z, Guo Y (2020a) Study on degradation of azithromycin antibiotics by molybdenum sulfide graphene oxide composites under visible light. IOP Conf Ser: Mater Sci Eng 774(1):012019. https://doi.org/10.1088/1757-899X/774/1/012019
Li Y, Zhang J, Zhan C, Kong F, Li W, Yang C, Hsiao BS (2020b) Facile synthesis of TiO2/CNC nanocomposites for enhanced Cr(VI) photoreduction: synergistic roles of cellulose nanocrystals. Carbohydr Polym 233:115838. https://doi.org/10.1016/j.carbpol.2020.115838
Liu YY, Wang Y, Walsh TR, Yi LX, Zhang R, Spencer J, Doi Y, Tian G, Dong B, Huang X, Yu LF, Gu D, Ren H, Chen X, Lv L, He D, Zhou H, Liang Z, Liu JH, Shen J (2016) Emergence of plasmid-mediated colistin resistance mechanism MCR-1 in animals and human beings in China: a microbiological and molecular biological study. Lancet Infect Dis 16(2):161–168. https://doi.org/10.1016/S1473-3099(15)00424-7
Mann A, Nehra K, Rana JS, Dahiya T (2021) Antibiotic resistance in agriculture: perspectives on upcoming strategies to overcome upsurge in resistance. Curr Res Microb Sci 2:100030. https://doi.org/10.1016/j.crmicr.2021.100030
Martakov IS, Torlopov MA, Mikhaylov VI, Krivoshapkina EF, Silant’ev VE, Krivoshapkin PV (2018) Interaction of cellulose nanocrystals with titanium dioxide and peculiarities of hybrid structures formation. J Sol-Gel Sci Technol 88(1):13–21. https://doi.org/10.1007/s10971-017-4447-3
Mirzaei R, Mesdaghinia A, Hoseini SS, Yunesian M (2019) Antibiotics in urban wastewater and rivers of Tehran, Iran: consumption, mass load, occurrence, and ecological risk. Chemosphere 221:55–66. https://doi.org/10.1016/j.chemosphere.2018.12.187
Moghni N, Boutoumi H, Khalaf H, Makaoui N (2022) Enhanced photocatalytic activity of TiO 2 / WO 3 nanocomposite from sonochemical-microwave assisted synthesis for the photodegradation of ciprofloxacin and oxytetracycline antibiotics under UV and s. J Photochem Photobiol A : Chem 428:113848. https://doi.org/10.1016/j.jphotochem.2022.113848
Mohamed MA, Salleh WNW, Jaafar J, Ismail AF, Abd Mutalib M, Jamil SM (2015) Incorporation of N-doped TiO2 nanorods in regenerated cellulose thin films fabricated from recycled newspaper as a green portable photocatalyst. Carbohyd Polym 133:429–437. https://doi.org/10.1016/j.carbpol.2015.07.057
Mohammed HT, Alasedi KK, Ruyid R, Hussein SA, Jarallah AL, Dahesh SMA, Sultan MQ, Salman ZN, Bashar BS, Aldulaimi AKO, Obaid MA (2022) ZnO/Co3O4 nanocomposites: novel preparation, characterization, and their performance toward removal of antibiotics from wastewater. J Nanostruct 12(3):503–509. https://doi.org/10.22052/JNS.2022.03.003
Mohapatra S, Huang CH, Mukherji S, Padhye LP (2016) Occurrence and fate of pharmaceuticals in WWTPs in India and comparison with a similar study in the United States. Chemosphere 159:526–535. https://doi.org/10.1016/j.chemosphere.2016.06.047
Nandiyanto ABD, Zaen R, Oktiani R (2020) Correlation between crystallite size and photocatalytic performance of micrometer-sized monoclinic WO3 particles. Arab J Chem 13(1):1283–1296. https://doi.org/10.1016/j.arabjc.2017.10.010
Naraginti S, Yu YY, Fang Z, Yong YC (2019) Visible light degradation of macrolide antibiotic azithromycin by novel ZrO2/Ag@TiO2 nanorod composite: transformation pathways and toxicity evaluation. Process Saf Environ Prot 125:39–49. https://doi.org/10.1016/j.psep.2019.02.031
Odling G, Robertson N (2015) Why is anatase a better photocatalyst than rutile? the importance of free hydroxyl radicals. Chemsuschem 8(11):1838–1840. https://doi.org/10.1002/cssc.201500298
Pelaez M, Nolan NT, Pillai SC, Seery MK, Falaras P, Kontos AG, Dunlop PSM, Hamilton JWJ, Byrne JA, O’Shea K, Entezari MH, Dionysiou DD (2012) A review on the visible light active titanium dioxide photocatalysts for environmental applications. Appl Catal B 125:331–349. https://doi.org/10.1016/j.apcatb.2012.05.036
Rodriguez-Mozaz S, Vaz-Moreira I, Varela Della Giustina S, Llorca M, Barceló D, Schubert S, Berendonk TU, Michael-Kordatou I, Fatta-Kassinos D, Martinez JL, Elpers C, Henriques I, Jaeger T, Schwartz T, Paulshus E, Osullivan K, Pärnänen KMM, Virta M, Do TT, Manaia CM (2020) Antibiotic residues in final effluents of European wastewater treatment plants and their impact on the aquatic environment. Environ Intern 140:105733. https://doi.org/10.1016/j.envint.2020.105733
Rossmann J, Schubert S, Gurke R, Oertel R, Kirch W (2014) Simultaneous determination of most prescribed antibiotics in multiple urban wastewater by SPE-LC-MS/MS. J Chromatogr, B: Anal Technol Biomed Life Sci 969:162–170. https://doi.org/10.1016/j.jchromb.2014.08.008
Sadeghi M, Sadeghi R, Mardani BGG, Ahmadi A (2018) Removal of azithromycin from aqueous solution using UV-light alone and UV plus persulfate (UV/Na2S2O8) processes. Iran J Pharm Res 17(Special Issue 2):54–64
Saud HR, Al-Taweel SS (2016) New route for synthesis of pure anatase TiO 2 nanoparticles via utrasound-assisted sol-gel method. J Chem Pharm Res 8(2):620–626
Sayadi MH, Sobhani S, Shekari H (2019) Photocatalytic degradation of azithromycin using GO@Fe3O4/ZnO/SnO2 nanocomposites. J Clean Prod 232:127–136. https://doi.org/10.1016/j.jclepro.2019.05.338
Sciancalepore C, Cassano T, Curri ML, Mecerreyes D, Valentini A, Agostiano A, Tommasi R, Striccoli M (2008) TiO2 nanorods/PMMA copolymer-based nanocomposites: highly homogeneous linear and nonlinear optical material. Nanotechnology 19(20):205705. https://doi.org/10.1088/0957-4484/19/20/205705
Shajahan S, Abu Haija M (2023) Effective removal of azithromycin by novel g-C3N4/CdS/CuFe2O4 nanocomposite under visible light irradiation. Chemosphere 337:139372. https://doi.org/10.1016/j.chemosphere.2023.139372
Sheng Y, Wei Z, Miao H, Yao W, Li H, Zhu Y (2019) Enhanced organic pollutant photodegradation via adsorption/photocatalysis synergy using a 3D g-C3N4/TiO2 free-separation photocatalyst. Chem Eng J 370:287–294. https://doi.org/10.1016/j.cej.2019.03.197
Shukla S, Pandey H, Singh P, Tiwari AK, Baranwal V, Singh J, Pandey AC (2022) Time and concentration dependent; UV light–mediated photocatalytic degradation of major antibiotic consortium using ZnO. Braz J Phys 52(5):1–9. https://doi.org/10.1007/s13538-022-01178-5
Steingrimsson O, Olafsson JH, Thorarinsson H, Ryan RW, Johnson RB, Tilton RC (1990) Azithromycin in the treatment of sexually transmitted disease. J Antimicrob Chemother 25:109–114. https://doi.org/10.1093/jac/25.suppl_A.109
Sunday Samuel O, Mathew Adefusika A (2019) Influence of size classifications on the structural and solid-state characterization of cellulose materials. Cellulose. https://doi.org/10.5772/intechopen.82849
Tan KB, Reza AK, Abdullah AZ, Amini Horri B, Salamatinia B (2018) Development of self-assembled nanocrystalline cellulose as a promising practical adsorbent for methylene blue removal. Carbohyd Polym 199:92–101. https://doi.org/10.1016/j.carbpol.2018.07.006
Trache D, Tarchoun AF, Derradji M, Hamidon TS, Masruchin N, Brosse N, Hussin MH (2020) Nanocellulose: from fundamentals to advanced applications. In Front Chem 8:392. https://doi.org/10.3389/fchem.2020.00392
Wei X, Zhu G, Fang J, Chen J (2013) Synthesis, characterization, and photocatalysis of well-dispersible phase-pure anatase TiO2 nanoparticles. Int J Photo 201:1–6. https://doi.org/10.1155/2013/726872
Xue J, Song F, Yin XW, Zhang ZL, Liu Y, Wang XL, Wang YZ (2017) Cellulose nanocrystal-templated synthesis of mesoporous TiO2 with dominantly exposed (001) facets for efficient catalysis. ACS Sustain Chem Eng 5(5):3721–3725. https://doi.org/10.1021/acssuschemeng.7b00341
Zhao S, Jin S, Liu H, Li S, Chen K (2021) Effects of crystallinity on the photocatalytic polymerization of 3,4-ethylenedioxythiophene over cspbbr3 inverse opals. Catalysts 11(11):1331. https://doi.org/10.3390/catal11111331
Zhou Y, Ding EY, Li WD (2007) Synthesis of TiO2 nanocubes induced by cellulose nanocrystal (CNC) at low temperature. Mater Lett 61(28):5050–5052. https://doi.org/10.1016/j.matlet.2007.04.001
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Saha, A., Varanasi, S. Sunlight-assisted photocatalytic degradation of azithromycin using cellulose nanocrystals–TiO2 composites. Appl Nanosci 14, 675–686 (2024). https://doi.org/10.1007/s13204-024-03039-w
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DOI: https://doi.org/10.1007/s13204-024-03039-w