Abstract
Antibiotics are becoming ubiquitous emerging contaminants in the aquatic environments due to their large amount of production and extensive application, which have received increasing public concern. In this paper, the degradation and mineralization of sulfamethoxazole (SMX) by ionizing radiation in the presence of Fe3O4 as Fenton-like catalyst were evaluated, the influencing factors, such as the initial SMX concentration, initial pH, water matrix, and radical scavenger, etc. were examined. The results demonstrated that SMX could be efficiently degraded. The addition of Fe3O4 could improve the degradation efficiency of SMX and increased the dose constant at various SMX initial concentrations. More than 98% of SMX was degraded in Fe3O4/gamma radiation system at a wide range of pH (about 3.0–11.0). The mineralization of SMX in the presence of Fe3O4 was increased by 200%. Adding free radical scavenger (tert-butyl alcohol) inhibited the degradation of SMX. The addition of Fe3O4 enhanced the dose constant of ·OH, indicating that Fe3O4 promoted the formation of hydroxyl radicals (·OH) and then improved SMX degradation and mineralization. The degradation efficiency of SMX in secondary effluent of WWTP decreased from 100 to 84% in secondary effluent compared with that in deionized water. The intermediate products during the degradation of SMX by ionizing radiation were identified by high-performance liquid chromatography, and a possible pathway of SMX degradation in such a system was tentatively proposed.
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Abellan MN, Gebhardt W, Schroder HF (2008) Detection and identification of degradation products of sulfamethoxazole by means of LC/MS and -MSn after ozone treatment. Water Sci Technol 58:1803–1812
Basfar AA, Khan HM, Al-Shahrani AA, Cooper WJ (2005) Radiation induced decomposition of methyl tert-butyl ether in water in presence of chloroform: kinetic modelling. Water Res 39:2085–2095
Boreen AL, Arnold WA, McNeill K (2005) Triplet-sensitized photodegradation of sulfa drugs containing six-membered heterocyclic groups: Identification of an SO2 extrusion photoproduct. Environ Sci Technol 39:3630–3638
Changotra R, Guin JP, Khader SA, Varshney L, Dhir A (2019) Electron beam induced degradation of ofloxacin in aqueous solution: kinetics, removal mechanism and cytotoxicity assessment. Chem Eng J 356:973–984
Chen H, Wang JL (2019) Catalytic ozonation of sulfamethoxazole over Fe3O4/Co3O4 composites. Chemosphere 234:14–24
Chen K, Zhou JL (2014) Occurrence and behavior of antibiotics in water and sediments from the Huangpu River, Shanghai, China. Chemosphere 95:604–612
Chu LB, Zhuang ST, Wang JL (2018) Degradation kinetics and mechanism of penicillin G in aqueous matrices by ionizing radiation. Radiat Phys Chem 145:34–38
Dantas RF, Contreras S, Sans C, Esplugas S (2008) Sulfamethoxazole abatement by means of ozonation. J Hazard Mater 150:790–794
Gao L, Zhuang J, Nie L, Zhang J, Zhang Y, Gu N, Wang T, Feng J, Yang D, Perrett S (2007) Intrinsic peroxidase-like activity of ferromagnetic nanoparticles. Nat Nanotechnol 2(9):577–583
Garcia-Galan MJ, Diaz-Cruz MS, Barcelo D (2012) Kinetic studies and characterization of photolytic products of sulfamethazine, sulfapyridine and their acetylated metabolites in water under simulated solar irradiation. Water Res 46:711–722
Gobel A, Thomsen A, McArdell CS, Joss A, Giger W (2005) Occurrence and sorption behavior of sulfonamides, macrolides, and trimethoprim in activated sludge treatment. Environ Sci Technol 39:3981–3989
Gomez-Ramos MD, Mezcua M, Aguera A, Fernandez-Alba AR, Gonzalo S, Rodriguez A, Rosal R (2011) Chemical and toxicological evolution of the antibiotic sulfamethoxazole under ozone treatment in water solution. J Hazard Mater 192:18–25
Gros M, Petrovic M, Ginebreda A, Barcelo D (2010) Removal of pharmaceuticals during wastewater treatment and environmental risk assessment using hazard indexes. Environ Int 36:15–26
Guo Z, Fei Z, Zhao Y, Zhang C, Liu F, Bao C, Lin M (2012) Gamma irradiation-induced sulfadiazine degradation and its removal mechanisms. Chem Eng J 191:256–262
Hou LW, Wang LG, Royer S, Zhang H (2016) Ultrasound-assisted heterogeneous Fenton-like degradation of tetracycline over a magnetite catalyst. J Hazard Mater 302:458–467
Hu J, Wang JL (2007) Degradation of chlorophenols in aqueous solution by gamma-radiation. Radiat Phys Chem 76:1489–1492
Huang RX, Fang ZQ, Yan XM, Cheng W (2012) Heterogeneous sono-Fenton catalytic degradation of bisphenol A by Fe3O4 magnetic nanoparticles under neutral condition. Chem Eng J 197:242–249
Huang RX, Fang ZQ, Fang XB, Tsang EP (2014) Ultrasonic Fenton-like catalytic degradation of bisphenol A by ferroferric oxide (Fe3O4) nanoparticles prepared from steel pickling waste liquor. J Colloid Interface Sci 436:258–266
Karthikeyan KG, Meyer MT (2006) Occurrence of antibiotics in wastewater treatment facilities in Wisconsin, USA. Sci Total Environ 361:196–207
Khan S, Han C, Sayed M, Sohail M, Jan S, Sultana S, Khan HM, Dionysiou DD (2019) Exhaustive photocatalytic Lindane degradation by combined simulated solar light-activated nanocrystalline TiO2 and inorganic oxidants. Catalysts 9:425
Kim HY, Kim TH, Cha SM, Yu S (2017) Degradation of sulfamethoxazole by ionizing radiation: Identification and characterization of radiolytic products. Chem Eng J 313:556–566
Liu YK, Wang JL (2013) Degradation of sulfamethazine by gamma irradiation in the presence of hydrogen peroxide. J Hazard Mater 250:99–105
Liu Y, Wang JL (2019) Reduction of nitrate by zero valent iron (ZVI)-based materials: a review. Sci Total Environ 671:388–403
Liu YK, Hu J, Wang JL (2014) Fe2+ enhancing sulfamethazine degradation in aqueous solution by gamma irradiation. Radiat Phys Chem 96:81–87
Liu Y, Fan Q, Wang JL (2018) Zn-Fe-CNTs catalytic in situ generation of H2O2 for Fenton-like degradation of sulfamethoxazole. J Hazard Mater 342:166–176
Mirzaei A, Chen Z, Haghighat F, Yerushalmi L (2017) Removal of pharmaceuticals from water by homo/heterogonous Fenton-type processes—a review. Chemosphere 174:665–688
Niu HY, Zhang D, Zhang SX, Zhang XL, Meng ZF, Cai YQ (2011) Humic acid coated Fe3O4 magnetic nanoparticles as highly efficient Fenton-like catalyst for complete mineralization of sulfathiazole. J Hazard Mater 190:559–565
Peñalver JJL, Pacheco CVG, Polo MS, Utrilla JR (2013) Degradation of tetracyclines in different water matrices by advanced oxidation/reduction processes based on gamma radiation. J Chem Technol Biotechnol 88:1096–1108
Phan TPH, Managaki S, Nakada N, Takada H, Shimizu A, Anh DH, Viet PH, Suzuki S (2011) Antibiotic contamination and occurrence of antibiotic-resistant bacteria in aquatic environments of northern Vietnam. Sci Total Environ 409:2894–2901
Rehman F, Sayed M, Khan JA, Shah NS, Khan HM, Dionysiou DD (2018) Oxidative removal of brilliant green by UV/S2O8 2–, UV/HSO5 –and UV/H2O2 processes in aqueous media: a comparative study. J Hazard Mater 357:506–514
Sayed M, Ismail M, Khan S, Tabassum S, Khan HM (2016) Degradation of ciprofloxacin in water by advanced oxidation process: kinetics study, influencing parameters and degradation pathways. Environ Technol 37(5):590–602
Sayed M, Arooj A, Shah NS, Khan JA, Shah LA, Rehman F, Arandiyan H, Khan AM, Khan AR (2018) Narrowing the band gap of TiO2 by co-doping with Mn2+ and Co2+ for efficient photocatalytic degradation of enoxacin and its additional peroxidase like activity: a mechanistic approach. J Mol Liq 272:403–412
Sayed M, Gul M, Shah NS, Khan JA, Khan ZUH, Rehman F, Khan AR, Rauf S, Arandiyan H, Yang CP (2019) In-situ dual applications of ionic liquid coated Co2+ and Fe3+ co-doped TiO2: superior photocatalytic degradation of ofloxacin at pilot scale level and enhanced peroxidase like activity for calorimetric biosensing. J Mol Liq 282:275–285
Shah NS, Khan JA, Nawaz S, Khan, HM (2014) Role of aqueous electron and hydroxyl radical in the removal of endosulfan from aqueous solution using gamma irradiation. J Hazard Mater 278:40-48
Shah NS, Khan JA, Al-Muhtaseb AH, Sayed M, Khan HM (2016) Gamma radiolytic decomposition of endosulfan in aerated solution: the role of carbonate radical. Environ Sci Pollut Res 23(12):12362–12371
Shah NS, Khan JA, Sayed M, Khan ZUH, Rizwan AD, Muhammad N, Boczkaj G, Murtaza B, Imran M, Khan HM, Zaman G (2018a) Solar light driven degradation of norfloxacin using as-synthesized Bi3+ and Fe2+ co-doped ZnO with the addition of HSO5 −: toxicities and degradation pathways investigation. Chem Eng J 351:841–855
Shah NS, Rizwan AD, Khan JA, Sayed M, Khan ZUH, Murtaza B, Lqbal J, Din SU, Imran M, Nadeem M, Al-Muhtaseb AH, Muhammad N, Khan HM, Ghauri M, Zaman G (2018b) Toxicities, kinetics and degradation pathways investigation of ciprofloxacin degradation using iron-mediated H2O2 based advanced oxidation processes. Process Saf Environ Prot 117:473–482
Shah NS, Khan JA, Sayed M, Khan ZUH, Ali HS, Murtaza B, Khan HM, Imran M, Muhammad N (2019) Hydroxyl and sulfate radical mediated degradation of ciprofloxacin using nano zerovalent manganese catalyzed S2O8 2−. Chem Eng J 356:199–209
Shen YP, Zhuan R, Chu LB, Xiang X, Sun H, Wang JL (2019) Inactivation of antibiotic resistance genes in antibiotic fermentation residues by ionizing radiation: exploring the development of recycling economy in antibiotic pharmaceutical factory. Waste Manag 84:141–146
Sichel C, Garcia C, Andre K (2011) Feasibility studies: UV/chlorine advanced oxidation treatment for the removal of emerging contaminants. Water Res 45(19):6371–6380
Song WJ, Cheng MM, Ma JH, Ma WH, Chen CC, Zhao JC (2006) Decomposition of hydrogen peroxide driven by photochemical cycling of iron species in clay. Environ Sci Technol 40(15):4782–4787
Tang JT, Wang JL (2018a) Fenton-like degradation of sulfamethoxazole using Fe-based magnetic nanoparticles embedded into mesoporous carbon hybrid as an efficient catalyst. Chem Eng J 351:1085–1094
Tang JT, Wang JL (2018b) Metal organic framework with coordinatively unsaturated sites as efficient Fenton-like catalyst for enhanced degradation of sulfamethazine. Environ Sci Technol 52:5367–5377
Tang JT, Wang JL (2019) MOF-derived three-dimensional flower-like FeCu@C composite as an efficient Fenton-like catalyst for sulfamethazine degradation. Chem Eng J 375:122007
Trojanowicz M, Bartosiewicz I, Bojanowska-Czajka A, Kulisa K, Szreder T, Bobrowski K, Nichipor H, Garcia-Reyes JF, Nalecz-Jawecki G, Meczynska-Wielgosz S, Kisala J (2019) Application of ionizing radiation in decomposition of perfluorooctanoate (PFOA) in waters. Chem Eng J 357:698–714
Wan Z, Wang JL (2017) Degradation of sulfamethazine using Fe3O4-Mn3O4 /reduced graphene oxide hybrid as Fenton-like catalyst. J Hazard Mater 324:653–664
Wan Z, Hu J, Wang JL (2016) Removal of sulfamethazine antibiotics using Ce-Fe-graphene nanocomposite as catalyst by Fenton-like process. J Environ Manag 182:284–291
Wang JL, Bai ZY (2017) Fe-Based Catalysts for heterogeneous catalytic ozonation of emerging contaminants in water and wastewater. Chem Eng J 312:79–98
Wang JL, Chu LB (2016) Irradiation treatment of pharmaceutical and personal care products (PPCPs) in water and wastewater: an overview. Radiat Phys Chem 125:56–64
Wang JL, Wang SZ (2016) Removal of pharmaceuticals and personal care products (PPCPs) from wastewater: a review. J Environ Manag 182:620–640
Wang SZ, Wang JL (2017) Comparative study on sulfamethoxazole degradation by Fenton and Fe (II)-activated persulfate process. RSC Adv 7(77):48670–48677
Wang JL, Wang SZ (2018a) Activation of persulfate (PS) and peroxymonosulfate (PMS) and application for the degradation of emerging contaminants. Chem Eng J 334:1502–1517
Wang JL, Wang SZ (2018b) Microbial degradation of sulfamethoxazole in the environment. Appl Microbiol Biotechnol 102:3573–3582
Wang SZ, Wang JL (2018c) Radiation-induced degradation of sulfamethoxazole in the presence of various inorganic anions. Chem Eng J 351:688–696
Wang JL, Wang SZ (2019) Activation of peroxymonosulfate by sludge-derived biochar for the degradation of triclosan in water and wastewater. Chem Eng J 356:350–358
Wang JL, Xu LJ (2012) Advanced oxidation processes for wastewater treatment: formation of hydroxyl radical and application. Crit Rev Environ Sci Technol 42:251–325
Wang JJ, Guo ZY, Shen XY, Guo QJ, Zhao YF, Zhu SN, Guo ZB (2017) Gamma irradiation-induced decomposition of sulfamethoxazole in aqueous solution: the influence of additives, biological inhibitory, and degradation mechanisms. Environ Sci Pollut Res 24:23658–23665
Wang JL, Zhuan R, Chu LB (2019) The occurrence, distribution and degradation of antibiotics by ionizing radiation: an overview. Sci Total Environ 646:1385–1397
Wardman P (1989) Reduction potentials of one-electron couples involving free-radicals in aqueous-solution. J Phys Chem Ref Data 18:1637–1755
Xu LJ, Wang JL (2011) A heterogeneous Fenton-like system with nanoparticulate zero-valent iron for removal of 4-chloro-3-methyl phenol. J Hazard Mater 186:256–264
Xu LJ, Wang JL (2012a) Magnetic nanoscaled Fe3O4/CeO2 composite as an efficient Fenton-like heterogeneous catalyst for degradation of 4-chlorophenol. Environ Sci Technol 46:10145–10153
Xu LJ, Wang JL (2012b) Fenton-like degradation of 2,4-dichlorophenol using Fe3O4 magnetic nanoparticles. Appl Catal B Environ 123:117–126
Yang B, Tian Z, Zhang L, Guo YP, Yan SQ (2015) Enhanced heterogeneous Fenton degradation of methylene blue by nanoscale zero valent iron (nZVI) assembled on magnetic Fe3O4/reduced graphene oxide. J Water Process Eng 5:101–111
Yu S, Lee B, Lee M, Cho IH, Chang SW (2008) Decomposition and mineralization of cefaclor by ionizing radiation: kinetics and effects of the radical scavengers. Chemosphere 71(11):2106–2112
Yu SQ, Hu J, Wang JL (2010a) Gamma radiation-induced degradation of p-nitrophenol (PNP) in the presence of hydrogen peroxide (H2O2) in aqueous solution. J Hazard Mater 177:1061–1067
Yu SQ, Hu J, Wang JL (2010b) Radiation-induced catalytic degradation of p-nitrophenol (PNP) in the presence of TiO2 nanoparticles. Radiat Phys Chem 79:1039–1046
Zhang SX, Zhao XL, Niu HY, Shi YL, Cai YQ, Jiang GB (2009) Superparamagnetic Fe3O4 nanoparticles as catalysts for the catalytic oxidation of phenolic and aniline compounds. J Hazard Mater 167(1-3):560–566
Zheng BG, Zheng Z, Zhang JB, Luo XZ, Wang JQ, Liu Q, Wang LH (2011) Degradation of the emerging contaminant ibuprofen in aqueous solution by gamma irradiation. Desalination 276(1-3):379–385
Zhuan R, Wang JL (2019) Degradation of sulfamethoxazole by ionizing radiation: Kinetics and implications of additives. Sci Total Environ 668:67–73
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We are thankful for the financial support from the National Natural Science Foundation of China (51338005) and the Program for Changjiang Scholars and Innovative Research Team in University (IRT-13026).
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Zhuan, R., Wang, J. Enhanced mineralization of sulfamethoxazole by gamma radiation in the presence of Fe3O4 as Fenton-like catalyst. Environ Sci Pollut Res 26, 27712–27725 (2019). https://doi.org/10.1007/s11356-019-05925-1
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DOI: https://doi.org/10.1007/s11356-019-05925-1