Abstract
The effects of coagulant dosage, alkalinity, turbidity, ionic strength, and dissolved organic matter (DOM) on the removal of sulfadimethoxazole (SMZ) and oxytetracycline (OTC) by coagulation were studied and the reaction mechanisms of the coagulation process were revealed in this research. From our results, alkalinity, turbidity, ionic strength, and DOM had different effects on the removal of antibiotics. The SMZ and OTC removals were improved with increase in poly-aluminum chloride (PACl) dosage, whereas the turbidity had less influence on the removal of SMZ and OTC because the adsorption of SMZ and OTC to kaolin was low, confirmed by a control when no PACl added. The hydrolysate of PACl played a more important role than turbidity in SMZ and OTC removals. The SMZ and OTC removals were significantly increased with the increase in alkalinity, which provided a suitable condition in situ for coagulant to form more optimal species of hydrolysate. The ionic strength, which was adjusted by NaNO3, also had a positive effect on the removal of SMZ but no obvious effect on the OTC removal. Furthermore, DOM had a higher effect on the removal of SMZ than that of OTC. In another word, if a water plant wants to improve the removal of SMZ and OTC by coagulation unit, PACl hydrolysate, alkalinity, and DOM are the three key factors to be considered primarily. Moreover, an experiment for the recovery of antibiotics from the flocs was done and the results showed that OTC and SMZ were removed by different mechanisms. The OTC was removed via complexation formed through the reaction between OTC and coagulant while the SMZ was removed through the pathway of adsorption and inter-particle bridging to the surface of coagulant hydrolysate.
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References
Adams C, ASCE M, Wang Y, Loftin K, Meyer M (2002) Removal of antibiotics from surface and distilled water in conventional water treatment processes. J Environ Eng 128(3):253–260. https://doi.org/10.1061/(ASCE)0733-9372(2002)128:3(253)
Akkanen J, Vogt RD, Kukkonen JVK (2004) Essential characteristics of natural dissolved organic matter affecting the sorption of hydrophobic organic contaminants. Aquat Sci 66(2):171–177. https://doi.org/10.1007/s00027-004-0705-x
Al-Degs YS, El-Barghouthi MI, El-Sheikh AH, Walker GM (2008) Effect of solution pH, ionic strength, and temperature on adsorption behavior of reactive dyes on activated carbon. Dyes Pigments 77(1):16–23. https://doi.org/10.1016/j.dyepig.2007.03.001
Bi Z, Feng CH, Wang DS, Ge XP, Tang HX (2013) Transformation of planar Mögel Al13 coagulant during the dilution and aging process. Colloids Surf A Physicochem Eng Asp 416(1):73–79. https://doi.org/10.1016/j.colsurfa.2012.06.029
Chefetz B, Deshmukh AP, Hatcher PG, Guthrie EA (2000) Pyrene sorption by natural organic matter. Environ Sci Technol 34(14):2925–2930. https://doi.org/10.1021/es9912877
Chen W, Westerhoff P, Leenheer JA, Booksh K (2003) Fluorescence excitation-emission matrix regional integration to quantify spectra for dissolved organic matter. Environ Sci Technol 37(24):5701–5710. https://doi.org/10.1021/es034354c
Choi KJ, Kim SG, Kim SH (2008) Removal of antibiotics by coagulation and granular activated carbon filtration. J Hazard Mater 151(1):38–43. https://doi.org/10.1016/j.jhazmat.2007.05.059
Deng SB, Zhou Q, Yu G, Huang J, Fan Q (2011) Removal of perfluorooctanoate from surface water by polyaluminium chloride coagulation. Water Res 45(4):1774–1780. https://doi.org/10.1016/j.watres.2010.11.029
Edzwald JK, Tobiason JE (1999) Enhanced coagulation: US requirements and a broader view. Water Sci Technol 40(9):63–70. https://doi.org/10.1016/S0273-1223(99)00641-1
Fukushima M, Tanabe Y, Yabuta H, Tanaka F, Ichikawa H, Tatsumi K, Watanabe A (2006) Water solubility enhancement effects of some polychlorinated organic pollutants by dissolved organic carbon from a soil with a higher organic carbon content. J Environ Sci Health, Part A 41(8):1483–1494. https://doi.org/10.1080/10934520600754748
Gao GY (2017) Performance and mechanism of catalytic ozonation of sulfamethoxazole in water by composite iron–manganese silicate. Harbin Instit Technol 3. (in Chinese)
Gao LH, Shi YL, Li WH, Liu JM, Cai YQ (2012) Occurrence, distribution and bioaccumulation of antibiotics in the Haihe River in China. J Environ Monit 14(4):1248–1254. https://doi.org/10.1039/C2EM10916F
Grover DP, Zhou JL, Frickers PE, Readman JW (2011) Improved removal of estrogenic and pharmaceutical compounds in sewage effluent by full scale granular activated carbon: impact on receiving river water. J Hazard Mater 185(2-3):1005–1011. https://doi.org/10.1016/j.jhazmat.2010.10.005
Gu C, Karthikeyan KG (2005) Interaction of tetracycline with aluminum and iron hydrous oxides. Environ Sci Technol 39(8):2660–2667. https://doi.org/10.1021/es048603o
Hermosilla D, Ordóñez R, Blanco L, de la Fuente E, Blanco A (2012) pH and particle structure effects on silica removal by coagulation. Chem Eng Technol 35:1632–1640. https://doi.org/10.1002/ceat.201100527
Huber MM, GÖbel A, Joss A, Hermann N, LÖffler D, McArdell CS, Ried A, Siegrist H, Ternes TA, Gunten U (2005) Oxidation of pharmaceuticals during ozonation of municipal wastewater effluents: a pilot study. Environ Sci Technol 39(11):4290–4299. https://doi.org/10.1021/es048396s
Jiang L, Hu XL, Yin DQ, Zhang HC, Yu ZY (2011) Occurrence, distribution and seasonal variation of antibiotics in the Huangpu River, Shanghai, China. Chemosphere 82(6):822–828. https://doi.org/10.1016/j.chemosphere.2010.11.028
Kim SC, Carlson K (2007) Temporal and spatial trends in the occurrence of human and veterinary antibiotics in aqueous and river sediment matrices. Environ Sci Technol 41(1):50–57. https://doi.org/10.1021/es060737+
Košutić K, Dolar D, Ašperger D, Kunst B (2007) Removal of antibiotics from a model wastewater by RO/NF membranes. Sep Purif Technol 53(3):244–249. https://doi.org/10.1016/j.seppur.2006.07.015
Kulshrestha P, Giese RF, Aga DS (2004) Investigating the molecular interactions of oxytetracycline in clay and organic matter: insights on factors affecting its mobility in soil. Environ Sci Technol 38(15):4097–4105. https://doi.org/10.1021/es034856q
Latour I, Miranda R, Blanco A (2013) Silica removal from newsprint mill effluents with aluminum salts. Chem Eng J 230:522–531. https://doi.org/10.1016/j.cej.2013.06.039
Li XQ, Zhang JW, Wang QJ, Qiu N (2004) Function of turbidity on water purification in polluted river. Sci Geogr Sin 24(2):245–249. (in Chinese). https://doi.org/10.13249/j.cnki.sgs.2004.02.020
Lin JL, Chin CJM, Huang C, Pan JR, Wang D (2008) Coagulation behavior of Al13 aggregates. Water Res 42(16):4281–4290. https://doi.org/10.1016/j.watres.2008.07.028
Managaki S, Murata A, Takada H, Tuyen BC, Chiem NH (2007) Distribution of macrolides, sulfonamides, and trimethoprim in tropical waters: ubiquitous occurrence of veterinary antibiotics in the Mekong Delta. Environ Sci Technol 41(23):8004–8010. https://doi.org/10.1021/es0709021
McArdell CS, Molnar E, Sute MJ-F, Giger W (2003) Occurrence and fate of macrolide antibiotics in wastewater treatment plants and in the Glatt Valley watershed, Switzerland. Environ Sci Technol 37(24):5479–5486. https://doi.org/10.1021/es034368i
Meiera M, Namjesnik-Dejanovicb K, Mauriceb PA, China Y-P, Aikenc GR (1999) Fractionation of aquatic natural organic matter upon sorption to goethite and kaolinite. Chem Geol 157(3-4):275–284. https://doi.org/10.1016/S0009-2541(99)00006-6
Pan B, Ghosh S, Xing BS (2008) Dissolved organic matter conformation and its interaction with pyrene as affected by water chemistry and concentration. Environ Sci Technol 42(5):1594–1599. https://doi.org/10.1021/es702431m
Qiang ZM, Adams C (2004) Potentiometric determination of acid dissociation constants (pKa) for human and veterinary antibiotics. Water Res 38(12):2874–2890. https://doi.org/10.1016/j.watres.2004.03.017
Raber B, Kögel-Knabner I, Stein C, Klem D (1998) Partitioning of polycyclic aromatic hydrocarbons to dissolved organic matter from different soils. Chemosphere 36(1):79–97. https://doi.org/10.1016/S0045-6535(97)00352-4
Shamsnejati S, Chaibakhsh N, Pendashteh AR, Hayeripour S (2015) Mucilaginous seed of ocimum basilicum as a natural coagulant for textile wastewater treatment. Ind Crop Prod 69:40–47. https://doi.org/10.1016/j.indcrop.2015.01.045
Steelink C (2002) Investigating humic acids in soils. Anal Chem 74:327A–333A. https://doi.org/10.1021/ac022040m
Suarez S, Lema JM, Omil F (2009) Pre-treatment of hospital wastewater by coagulation-flocculation and flotation. Bioresour Technol 100(7):2138–2146. https://doi.org/10.1016/j.biortech.2008.11.015
Tarr MA, Wang WW, Bianchi TS, Engelhaupt E (2001) Mechanisms of ammonia and amino acid photoproduction from aquatic humic and colloidal matter. Water Res 35(15):3688–3696. https://doi.org/10.1016/S0043-1354(01)00101-4
Ternes TA, Meisenheimer M, McDowell D, Sacher F, Brauch H-J, Haist-Gulde B, Preuss G, Wilme U, Zulei-Seibert N (2002) Removal of pharmaceuticals during drinking water treatment. Environ Sci Technol 36(17):3855–3863. https://doi.org/10.1021/es015757k
Torres MF, González JM, Rojas MR, Mülle AJ, Sáez AE, Löf D, Schillén K (2007) Effect of ionic strength on the rheological behavior of aqueous cetyltrimethylammonium p-toluene sulfonate solutions. J Colloid Interface Sci 307(1):221–228. https://doi.org/10.1016/j.jcis.2006.11.002
Vermöhlen K, Lewandowski H, Narres H-D, Schwuger MJ (2000) Adsorption of polyelectrolytes onto oxides — the influence of ionic strength, molar mass, and Ca2+ ions. Colloids Surf A Physicochem Eng Asp 163(1):45–53. https://doi.org/10.1016/S0927-7757(99)00429-X
Vieno N, Tuhkanen T, Kronberg L (2006) Removal of pharmaceuticals in drinking water treatment: effect of chemical coagulation. Environ Technol 27(2):183–192. https://doi.org/10.1080/09593332708618632
Wang Y, Zhang H, Zhang JH, Lu C, Huang QQ, Wu J, Liu F (2011) Degradation of tetracycline in aqueous media by ozonation in an internal loop-lift reactor. J Hazard Mater 192(1):35–43. https://doi.org/10.1016/j.jhazmat.2011.04.086
Wang DS, Zhang T, Chao Y (2014) Influence of different strength and species of cation on adsorption of oxytetracycline in meadow soils. Ecol Environ Sci 23(5):870–875. (in Chinese). https://doi.org/10.16258/j.cnki.1674-5906.2014.05.018
Wei QS, Zhu GF, Wu P, Cui L, Zhang KS, Zhou JJ, Zhang WR (2010) Distributions of typical contaminant species in urban short-term storm runoff and their fates during rain events: a case of Xiamen City. J Environ Sci 22(4):533–539. https://doi.org/10.1016/S1001-0742(09)60138-8
Wiegel S, Aulinger A, Brockmeyer R, Harms H, Löffler J, Reincke H, Schmidt R, Stachel B, Wv T, Wanke A (2004) Pharmaceuticals in the River Elbe and its tributaries. Chemosphere 57(2):107–126. https://doi.org/10.1016/j.chemosphere.2004.05.017
Wu FC, Wang LY, Li W, Zhang RY, Fu PQ, Liao HQ, Bai YC, Guo JY, Wang J (2008) Natural organic matter and its significance in terrestrial surface environment. J Lake Sci 20:1–12. (in Chinese). https://doi.org/10.18307/2008.0101
Xu WH, Zhang G, Zou SC, Ling ZH, Wang GL, Yan W (2009) A preliminary investigation on the occurrence and distribution of antibiotics in the Yellow River and its tributaries, China. Water Environ Res 81(3):248–254. https://doi.org/10.2175/106143008X325719
Yan CX, Yang Y, Zhou JL, Liu M, Nie MH, Shi H, Gu LJ (2013) Antibiotics in the surface water of the Yangtze Estuary: occurrence, distribution and risk assessment. Environ Pollut 175:22–27. https://doi.org/10.1016/j.envpol.2012.12.008
Ye CQ (2006) Al13 formation through meta-equilibrium and its electrostatic patch coagulation effect. Chin Acad Sci 39–40. (in Chinese)
Zhan XH, Zhou LX, Yang H, Jiang TH (2007) Infrared spectroscopy of DOM-PAHs complexes. Acta Pedol Sin 44(1):47–53. (in Chinese). https://doi.org/10.11766/trxb200510310108
Zhang WC, Wei QS, Luo ZX, You J, Xiao JH, Liu JS, Yan CZ (2015) Effects of alkalinity and turbidity on SMZ and OTC removal by coagulation. Res Environ Sci 28(5):802–807. (in Chinese). https://doi.org/10.13198/j.issn.1001-6929.2015.05.19
Zhou LJ, Ying GG, Zhao JL, Yang JF, Wang L, Yang B, Liu S (2011) Trends in the occurrence of human and veterinary antibiotics in the sediments of the Yellow River, Hai River and Liao River in northern China. Environ Pollut 159(7):1877–1885. https://doi.org/10.1016/j.envpol.2011.03.034
Zhu Y (2013) Research for environmental risk evaluation system of the use and disposal process of oxytetracycline resideue. Harbin Instit Technol 37–38. (in Chinese)
Zuccato E, Castiglioni S, Bagnati R, Melis M, Fanelli R (2010) Source, occurrence and fate of antibiotics in the Italian aquatic environment. J Hazard Mater 179(1-3):1042–1048. https://doi.org/10.1016/j.jhazmat.2010.03.110
Funding
This work was supported by the National Key Research and Development Program of China (Grant Nos. 2016YFC0400501, 2016YFC0400509) and the National Natural Science Foundation of China (Grant No. 21876025, No. 21277138) and the National water pollution control key project (Grant No. 2017ZX07202005-005).
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Weichao Zhang, Qunshan Wei, and Jiuhua Xiao carried out all the experiments and wrote the manuscript. Qunshan Wei, Jianshe Liu, and Changzhou Yan designed and supervised all the experiments. Qunshan Wei, Yanbiao Liu, Wolfgang Sand, and Christopher Chow revised the manuscript draft and the final version of the submitted manuscript.
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Zhang, W., Wei, Q., Xiao, J. et al. The key factors and removal mechanisms of sulfadimethoxazole and oxytetracycline by coagulation. Environ Sci Pollut Res 27, 16167–16176 (2020). https://doi.org/10.1007/s11356-019-06884-3
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DOI: https://doi.org/10.1007/s11356-019-06884-3