The presence of residual antibiotics in the environment is one of the major global concerns, and it is imperative to control their discharge in water bodies. The present study used a combination of Fe3O4 nanoparticles/persulfate in conjunction with ultrasound to address this problem; the influence of effective parameters in the remediation process, persulfate concentration, nanoparticle concentrations, initial antibiotic concentration, contact time and pH was investigated. The highest removal rate of tetracycline antibiotic was observed at pH 10, the amount of magnetic nanoparticles being (0.3 g/L), with persulfate concentration at 4 mM for the removal of antibiotic concentration at 10 mg/L; TC and COD removal efficiency is 92.99 and 79.85%, respectively. The deployment of sonocatalytic process, along with the use of magnetite nanoparticles and persulfates as oxidizing agents, appears to be an effective means for decreasing the high-level tetracycline concentration in water.
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Bacanli M, Başaran N (2019) Importance of antibiotic residues in animal food. Food Chem Toxicol 125: 462–466
Bahadir T, Celebi H, Simsek I, Tulun S (2019) Antibiotic applications in fish farms and environmental problems. Turk J Eng 3:60–67
Chatel G, Colmenares JC (2017) Sonochemistry: from basic principles to innovative applications. Top Curr Chem 375:8. https://doi.org/10.1007/s41061-016-0096-1
Colmenares JC et al (2016) Mild ultrasound-assisted synthesis of TiO2 supported on magnetic nanocomposites for selective photo-oxidation of benzyl alcohol. Appl Catal B 183:107–112. https://doi.org/10.1016/j.apcatb.2015.10.034
Fang G, Gao J, Dionysiou DD, Liu C, Zhou D (2013) Activation of persulfate by quinones: free radical reactions and implication for the degradation of PCBs. Environ Sci Technol 47:4605–4611
Feiz-Arefi M, Ghorbani-Shahna F, Bahrami A, Ebrahimi H, Mahjub A (2019) Photocatalytic removal of methylbenzene vapors by MnO2/Al2O3/Fe2O3 nano composite. Iran J Health Saf Environ 6:1158–1166
Fernandez Rivas D, Kuhn S (2016) Synergy of microfluidics and ultrasound. Top Curr Chem 374:70. https://doi.org/10.1007/s41061-016-0070-y
Ghasemi A, Kheirmand M, Heli H (2019) Synthesis of novel NiFe2O4 nanospheres for high performance pseudocapacitor applications. Russ J Electrochem 55:206–214. https://doi.org/10.1134/s1023193519020022
Ghauch A, Ayoub G, Naim S (2013) Degradation of sulfamethoxazole by persulfate assisted micrometric Fe0 in aqueous solution. Chem Eng J 228:1168–1181. https://doi.org/10.1016/j.cej.2013.05.045
Gustafson R, Bowen R (1997) Antibiotic use in animal agriculture. J Appl Microbiol 83:531–541
Heidari MR, Malakootian M (2018) Removal of cyanide from synthetic wastewater by combined coagulation and advanced oxidation process. Desalination Water Treat 133:204–211
Jeong J, Song W, Cooper WJ, Jung J, Greaves J (2010) Degradation of tetracycline antibiotics: mechanisms and kinetic studies for advanced oxidation/reduction processes. Chemosphere 78:533–540
Khachatourians GG (1998) Agricultural use of antibiotics and the evolution and transfer of antibiotic-resistant bacteria. CMAJ 159:1129–1136
Khan FU et al (2017a) Visible light inactivation of E. coli, cytotoxicity and ROS determination of biochemically capped gold nanoparticles. Microb Pathog 107:419–424. https://doi.org/10.1016/j.micpath.2017.04.024
Khan ZUH et al (2017b) Biomedical applications of green synthesized Nobel metal nanoparticles. J Photochem Photobiol B 173:150–164. https://doi.org/10.1016/j.jphotobiol.2017.05.034
Khatami M, Alijani HQ, Fakheri B, Mobasseri MM, Heydarpour M, Farahani ZK, Khan AU (2019) Super-paramagnetic iron oxide nanoparticles (SPIONs): greener synthesis using Stevia plant and evaluation of its antioxidant properties. J Clean Prod 208:1171–1177. https://doi.org/10.1016/j.jclepro.2018.10.182
Lacasse E, Brouillette E, Larose A, Parr TR, Rubio A, Malouin F (2019) In vitro activity of tebipenem (SPR859) against penicillin-binding proteins of gram-negative and gram-positive bacteria. Antimicrob Agents Chemother 63:e02181-18
Lan L, Kong X, Sun H, Li C, Liu D (2019) High removal efficiency of antibiotic resistance genes in swine wastewater via nanofiltration and reverse osmosis processes. J Environ Manage 231:439–445
Li X et al (2019) Enhanced methane production from waste activated sludge by combining calcium peroxide with ultrasonic: performance, mechanism, and implication. Biores Technol 279:108–116
Malakootian M, Gharaghani MA, Dehdarirad A, Khatami M, Ahmadian M, Heidari MR, Mahdizadeh H (2019) ZnO nanoparticles immobilized on the surface of stones to study the removal efficiency of 4-nitroaniline by the hybrid advanced oxidation process (UV/ZnO/O3). J Mol Struct 1176:766–776. https://doi.org/10.1016/j.molstruc.2018.09.033
Martina K, Tagliapietra S, Barge A, Cravotto G (2016) Combined microwaves/ultrasound, a hybrid technology. Top Curr Chem 374:79. https://doi.org/10.1007/s41061-016-0082-7
Murugesan R, Sivakumar S, Karthik K, Anandan P, Haris M (2019) Structural, optical and magnetic behaviors of Fe/Mn-doped and co-doped CdS thin films prepared by spray pyrolysis method. Appl Phys A 125:281. https://doi.org/10.1007/s00339-019-2577-x
Nadour M, Boukraa F, Benaboura A (2019) Removal of diclofenac, paracetamol and metronidazole using a carbon-polymeric membrane. J Environ Chem Eng 7:103080. https://doi.org/10.1016/j.jece.2019.103080
Nagaraju G, Karthik K, Shashank M (2019) Ultrasound-assisted Ta2O5 nanoparticles and their photocatalytic and biological applications. Microchem J 147:749–754. https://doi.org/10.1016/j.microc.2019.03.094
Nasrollahzadeh M, Sajjadi M, Varma RS (2019) A catalyst-free and expeditious general synthesis of N-benzyl-N-arylcyanamides under ultrasound irradiation at room temperature. Ultrason Sonochem 56:481–486. https://doi.org/10.1016/j.ultsonch.2019.04.038
Östman M, Björlenius B, Fick J, Tysklind M (2019) Effect of full-scale ozonation and pilot-scale granular activated carbon on the removal of biocides, antimycotics and antibiotics in a sewage treatment plant. Sci Total Environ 649:1117–1123
Oturan N, Wu J, Zhang H, Sharma VK, Oturan MA (2013) Electrocatalytic destruction of the antibiotic tetracycline in aqueous medium by electrochemical advanced oxidation processes: effect of electrode materials. Appl Catal B 140:92–97
Rahdar S, Ahmadi S (2019) The removal of amoxicillin with Zno nanoparticles in combination with US-H2O2 advanced oxidation processes from aqueous solutions. Iran J Health Sci 7:36–45
Ravikumar K et al (2019) Enhanced tetracycline removal by in situ NiFe nanoparticles coated sand in column reactor. J Environ Manage 236:93–99
Safaei M, Foroughi MM, Ebrahimpoor N, Jahani S, Omidi A, Khatami M (2019) A review on metal-organic frameworks: synthesis and applications. TrAC Trends Anal Chem 118:401–425. https://doi.org/10.1016/j.trac.2019.06.007
Safari GH, Nasseri S, Mahvi AH, Yaghmaeian K, Nabizadeh R, Alimohammadi M (2015) Optimization of sonochemical degradation of tetracycline in aqueous solution using sono-activated persulfate process. J Environ Health Sci Eng 13:76
Saien J, Ojaghloo Z, Soleymani A, Rasoulifard M (2011) Homogeneous and heterogeneous AOPs for rapid degradation of Triton X-100 in aqueous media via UV light, nano titania hydrogen peroxide and potassium persulfate. Chem Eng J 167:172–182
Sarmah AK, Meyer MT, Boxall AB (2006) A global perspective on the use, sales, exposure pathways, occurrence, fate and effects of veterinary antibiotics (VAs) in the environment. Chemosphere 65:725–759
Shaojun J, Zheng S, Daqiang Y, Lianhong W, Liangyan C (2008) Aqueous oxytetracycline degradation and the toxicity change of degradation compounds in photoirradiation process. J Environ Sci 20:806–813
Slots J, Ting M (2002) Systemic antibiotics in the treatment of periodontal disease. Periodontol 2000 28:106–176
Toolabi A et al (2018) Optimizing the photocatalytic process of removing diazinon pesticide from aqueous solutions and effluent toxicity assessment via a response surface methodology approach. Rend Lincei Sci Fis Nat 1:1. https://doi.org/10.1007/s12210-018-0751-2
Torkzadeh-Mahani R, Foroughi MM, Jahani S, Kazemipour M, Hassani Nadiki H (2019) The effect of ultrasonic irradiation on the morphology of NiO/Co3O4 nanocomposite and its application to the simultaneous electrochemical determination of droxidopa and carbidopa. Ultrason Sonochem 56:183–192. https://doi.org/10.1016/j.ultsonch.2019.04.002
Virkutyte J, Varma RS (2014) Eco-friendly magnetic iron oxide pillared montmorillonite for advanced catalytic degradation of dichlorophenol. ACS Sustain Chem Eng 2:1545–1550. https://doi.org/10.1021/sc5002512
Wacławek S, Grübel K, Silvestri D, Padil VVT, Wacławek M, Černík M, Varma RS (2018) Disintegration of wastewater activated sludge (WAS) for improved biogas production. Energies 12:21
Wang X, Wang Y, Li D (2013) Degradation of tetracycline in water by ultrasonic irradiation. Water Sci Technol 67:715–721
Wu Y et al (2019) Three-dimensional α-Fe2O3/amino-functionalization carbon nanotube sponge for adsorption and oxidative removal of tetrabromobisphenol. Sep Purif Technol 211:359–367
Xu L, Chu W, Graham N (2014) Degradation of di-n-butyl phthalate by a homogeneous sono–photo–Fenton process with in situ generated hydrogen peroxide. Chem Eng J 240:541–547
Xu J et al (2019) Insights into removal of tetracycline by persulfate activation with peanut shell biochar coupled with amorphous Cu-doped FeOOH composite in aqueous solution. Environ Sci Pollut Res 26:2820–2834
Yang X, Cheng X, Elzatahry AA, Chen J, Alghamdi A, Deng Y (2019) Recyclable Fenton-like catalyst based on zeolite Y supported ultrafine, highly-dispersed Fe2O3 nanoparticles for removal of organics under mild conditions. Chin Chem Lett 30:324–330
Zhang C, Xue J, Cheng D, Feng Y, Liu Y, Aly HM, Li Z (2019) Uptake, translocation and distribution of three veterinary antibiotics in Zea mays L. Environ Pollut 250:47–57
Zhu J, Snow DD, Cassada D, Monson S, Spalding R (2001) Analysis of oxytetracycline, tetracycline, and chlortetracycline in water using solid-phase extraction and liquid chromatography–tandem mass spectrometry. J Chromatogr A 928:177–186
Zhu Y, Liu J, Liao Y, Lv W, Ma L, Wang C (2018) Degradation of vanillin during lignin valorization under alkaline oxidation. Top Curr Chem 376:29. https://doi.org/10.1007/s41061-018-0208-1
Zou X, Zhou T, Mao J, Wu X (2014) Synergistic degradation of antibiotic sulfadiazine in a heterogeneous ultrasound-enhanced Fe0/persulfate Fenton-like system. Chem Eng J 257:36–44
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Malakotian, M., Asadzadeh, S.N., Khatami, M. et al. Protocol encompassing ultrasound/Fe3O4 nanoparticles/persulfate for the removal of tetracycline antibiotics from aqueous environments. Clean Techn Environ Policy 21, 1665–1674 (2019). https://doi.org/10.1007/s10098-019-01733-w
- Fe3O4 nanoparticles
- Ultrasonic wave