CuO/Al2O3-EPC particles (prepared by an electroless plating-calcination method) were used to catalyze ozonation (O3) for the degradation of sulfamethoxazole (SMX) in aqueous solution. First, effects of key parameters including catalyst dosage (0–1.5 g/L), oxygen flow rate (100–500 mL/min), temperature (5–45°C), initial solution pH (3.0–9.0), and initial SMX concentration (19.75–98.75 μM) were investigated. The CuO/Al2O3-EPC/O3 system was effectively applicable for a broad pH range (∼3.0 − 9.0). Furthermore, CuO/Al2O3-EPC particles showed good stability and catalytic activity in CuO/Al2O3-EPC/O3 system. Presence of tert-butanol in CuO/Al2O3-EPC/O3 system accelerated the degradation of SMX. Based on eight intermediates detected by ultra-high performance liquid chromatography-quadrupole time-of-flight mass spectrometry, SMX in CuO/Al2O3-EPC/O3 system was degraded by six pathways. Finally, biological toxicity of SMX solution degraded by CuO/Al2O3-EPC/O3 system was reduced. In brief, this study suggests that the CuO/Al2O3-EPC/O3 system is an effective system for removing SMX from water.
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References
1.
AoX., and LiuW. (2017). Degradation of sulfamethoxazole by medium pressure UV and oxidants: Peroxymonosulfate, persulfate, and hydrogen peroxide. Chem. Eng. J. 313, 629.
2.
Arslan-AlatonI., AytenN., and Olmez-HanciT. (2010). Photo-Fenton-like treatment of the commercially important H-acid: Process optimization by factorial design and effects of photocatalytic treatment on activated sludge inhibition. Appl. Catal. B Environ. 96, 208.
3.
BaderH., and HoigniJ. (1981). Determination of ozone in water by the indigo method. Water Res. 15, 449.
4.
BeltránF.J., PocostalesP., ÁlvarezP.M., and López-PiñeiroF. (2009). Catalysts to improve the abatement of sulfamethoxazole and the resulting organic carbon in water during ozonation. Appl. Catal. B Environ. 92, 262.
5.
BeltránF.J., RivasF.J., and Montero-de-EspinosaR. (2002). Catalytic ozonation of oxalic acid in an aqueous TiO2 slurry reactor. Appl. Catal. B Environ. 39, 221.
6.
BuQ., WangB., HuangJ., DengS., and YuG. (2013). Pharmaceuticals and personal care products in the aquatic environment in China: A review. J. Hazard. Mater. 262, 189.
7.
BuxtonG.V., GreenstockC.L., HelmanW.P., and RossA.B. (1988). Critical review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals (•OH/•O− in aqueous solution. J. Phys. Chem. Ref. Data, 17, 513.
8.
ChenH.W., KuoY.L., ChiouC.S., YouS.W., MaC.M., and ChangC.T. (2010). Mineralization of reactive Black 5 in aqueous solution by ozone/H2O2 in the presence of a magnetic catalyst. J. Hazard. Mater. 174, 795.
9.
DantasR.F., ContrerasS., SansC., and EsplugasS. (2008). Sulfamethoxazole abatement by means of ozonation. J. Hazard. Mater. 150, 790.
10.
DuJ., GuoW., WangH., YinR., ZhengH., FengX., CheD., and RenN. (2018). Hydroxyl radical dominated degradation of aquatic sulfamethoxazole by Fe(0)/bisulfite/O2: Kinetics, mechanisms, and pathways. Water Res. 138, 323.
11.
FlammD.L. (1977). Analysis of ozone at low concentrations with boric acid buffered potassium iodide. Environ. Sci. Technol. 11, 978.
12.
GaoS., ZhaoZ., XuY., TianJ., QiH., LinW., and CuiF. (2014). Oxidation of sulfamethoxazole (SMX) by chlorine, ozone and permanganate—A comparative study. J. Hazard. Mater. 274, 258.
13.
GoncalvesA.G., OrfaoJ.J., and PereiraM.F. (2012). Catalytic ozonation of sulphamethoxazole in the presence of carbon materials: Catalytic performance and reaction pathways. J. Hazard. Mater. 239, 167.
14.
HoignéJ., and BaderH. (1983). Rate constants of reactions of ozone with organic and inorganic compounds in water—I: Non-dissociating organic compounds. Water Res. 17, 173.
15.
HouL., ZhangH., WangL., ChenL., XiongY., and XueX. (2013). Removal of sulfamethoxazole from aqueous solution by sono-ozonation in the presence of a magnetic catalyst. Sep. Purif. Technol. 117, 46.
16.
HuangC., DongC., and TangZ. (1993). Advanced chemical oxidation: Its present role and potential future in hazardous waste treatment. Waste Manage. 13, 361.
17.
JungY., HongE., KwonM., and KangJ.-W. (2017). A kinetic study of ozone decay and bromine formation in saltwater ozonation: Effect of O3 dose, salinity, pH, and temperature. Chem. Eng. J. 312, 30.
18.
Kasprzyk-HordernB. (2003). Catalytic ozonation and methods of enhancing molecular ozone reactions in water treatment. Appl. Catal. B Environ. 46, 639.
19.
LaiL., YanJ., LiJ., and LaiB. (2018). Co/Al2O3-EPM as peroxymonosulfate activator for sulfamethoxazole removal: Performance, biotoxicity, degradation pathways and mechanism. Chem. Eng. J. 343, 676.
20.
LiJ., LiuQ., Ji, Q.q., and LaiB. (2017). Degradation of p-nitrophenol (PNP) in aqueous solution by Fe0-PM-PS system through response surface methodology (RSM). Appl. Catal. B Environ. 200, 633.
21.
MaJ., SuiM., ZhangT., and GuanC. (2005). Effect of pH on MnOx/GAC catalyzed ozonation for degradation of nitrobenzene. Water Res. 39, 779.
22.
MullaS.I., HuA., SunQ., LiJ., SuanonF., AshfaqM., and YuC.P. (2018). Biodegradation of sulfamethoxazole in bacteria from three different origins. J. Environ. Manage. 206, 93.
23.
NawrockiJ., and Kasprzyk-HordernB. (2010). The efficiency and mechanisms of catalytic ozonation. Appl. Catal. B Environ. 99, 27.
24.
QuJ., LiH., LiuH., and HeH. (2004). Ozonation of alachlor catalyzed by Cu/Al2O3 in water. Catal. Today, 90, 291.
25.
RenY., LiJ., PengJ., JiF., and LaiB. (2018). Strengthening the catalytic activity for ozonation of Cu/Al2O3 by an electroless plating–calcination process. Indus. Eng. Chem. Res. 57, 1815.
26.
StaehelinJ., and HoigneJ. (1985). Decomposition of ozone in water in the presence of organic solutes acting as promoters and inhibitors of radical chain reactions. Environ. Sci. Technol. 19, 1206.
27.
TisaF., Abdul RamanA.A., and Wan DaudW.M.A. (2014). Applicability of fluidized bed reactor in recalcitrant compound degradation through advanced oxidation processes: A review. J. Environ. Manage. 146, 260.
28.
Vijaya ChamundeeswariS.P., James Jebaseelan SamuelE., and SundaraganesanN. (2014). Molecular structure, vibrational spectra, NMR and UV spectral analysis of sulfamethoxazole. Spectrochim. Acta A Mol. Biomol. Spectrosc. 118, 1.
29.
von GuntenU. (2003). Ozonation of drinking water: Part I. Oxidation kinetics and product formation. Water Res., 37, 1443.
30.
Von SonntagC., and Von GuntenU. (2012). Chemistry of Ozone in Water and Wastewater Treatment. London: IWA Publishing; DOI: 10.2166/97817804008.
31.
WesterhoffP., SongR., AmyG., and MinearR. (1997). Applications of ozone decomposition models. Ozone Sci. Eng. 19, 55.
32.
WillachS., LutzeH.V., EckeyK., LoppenbergK., LulingM., TerhalleJ., WolbertJ.B., JochmannM.A., KarstU., and SchmidtT.C. (2017). Degradation of sulfamethoxazole using ozone and chlorine dioxide—Compound-specific stable isotope analysis, transformation product analysis and mechanistic aspects. Water Res. 122, 280.
33.
WuJ., ChenS., and MuruganandhamM. (2008). Catalytic ozonation of oxalic acid using carbon-free rice husk ash catalysts. Indus. Eng. Chem. Res. 47, 2919.
34.
XiongZ., CaoJ., LaiB., and YangP. (2018a). Comparative study on degradation of p-nitrophenol in aqueous solution by mFe/Cu/O 3 and mFe0/O3 processes. J. Indus. Eng. Chem. 59, 196.
35.
XiongZ., LaiB., and YangP. (2018b). Insight into a highly efficient electrolysis-ozone process for N,N-dimethylacetamide degradation: Quantitative analysis of the role of catalytic ozonation, fenton-like and peroxone reactions. Water Res. 140, 12.
36.
YangY., LuX., JiangJ., MaJ., LiuG., CaoY., LiuW., LiJ., PangS., KongX., et al. (2017a). Degradation of sulfamethoxazole by UV, UV/H2O2 and UV/persulfate (PDS): Formation of oxidation products and effect of bicarbonate. Water Res. 118, 196.
37.
YangZ., DaiD., YaoY., ChenL., LiuQ., and LuoL. (2017b). Extremely enhanced generation of reactive oxygen species for oxidation of pollutants from peroxymonosulfate induced by a supported copper oxide catalyst. Chem. Eng. J. 322, 546.
38.
YinR., GuoW., WangH., DuJ., ZhouX., WuQ., ZhengH., ChangJ., and RenN. (2018). Selective degradation of sulfonamide antibiotics by peroxymonosulfate alone: Direct oxidation and nonradical mechanisms. Chem. Eng. J. 334, 2539.
39.
ZhangH., JiF., ZhangY., PanZ., and LaiB. (2018). Catalytic ozonation of N,N-dimethylacetamide (DMAC) in aqueous solution using nanoscaled magnetic CuFe2O4. Sep. Purif. Technol. 193, 368.
40.
ZouX., ZhouT., MaoJ., and WuX. (2014). Synergistic degradation of antibiotic sulfadiazine in a heterogeneous ultrasound-enhanced FeO/persulfate Fenton-like system. Chem. Eng. J. 257, 36.
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