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Kinetics of tetracycline, oxytetracycline, and chlortetracycline adsorption and desorption on two acid soils

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Abstract

The purpose of this work was to quantify retention/release of tetracycline, oxytetracycline, and chlortetracycline on two soils, paying attention to sorption kinetics and to implications of the adsorption/desorption processes on transfer of these pollutants to the various environmental compartments. We used the stirred flow chamber (SFC) procedure to achieve this goal. All three antibiotics showed high affinity for both soils, with greater adsorption intensity for soil 1, the one with the highest organic matter and Al and Fe oxides contents. Desorption was always <15 %, exhibiting strong hysteresis in the adsorption/desorption processes. Adsorption was adequately modeled using a pseudo first-order equation with just one type of adsorption sites, whereas desorption was better adjusted considering both fast and slow sorption sites. The adsorption maximum (q max ) followed the sequence tetracycline > oxytetracycline > chlortetracycline in soil 1, with similar values for the three antibiotics and the sequence tetracycline > chlortetracycline > oxytetracycline in soil 2. The desorption sequences were oxytetracycline > tetracycline > chlortetracycline in soil 1 and oxytetracycline > chlortetracycline > tetracycline in soil 2. In conclusion, the SFC technique has yielded new kinetic data regarding tetracycline, oxytetracycline, and chlortetracycline adsorption/desorption on soils, indicating that it can be used to shed further light on the retention and transport processes affecting antibiotics on soils and other media, thus increasing knowledge on the behavior and evolution of these pharmaceutical residues in the environment.

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References

  • Aharoni C, Sparks DL (1991) Kinetics of soil chemical reactions—a theoretical treatment. In: Sparks DL, Suarez DL (eds) Rates of soil chemical processes. Soil Science Society of America, Madison, pp 1–18

    Google Scholar 

  • Avisar D, Primor O, Gozlan I (2010) Sorption of sulfonamides and tetracyclines to montmorillonite clay. Water Air Soil Pollut 209:439–450

    Article  CAS  Google Scholar 

  • Bermúdez-Couso A, Fernández-Calviño D, Pateiro-Moure M, Garrido-Rodríguez B, Nóvoa-Muñoz JC, Arias-Estévez M (2011) Adsorption and desorption behavior of metalaxyl in intensively cultivated acid soils. J Agric Food Chem 59:7286–7293

    Article  Google Scholar 

  • Bermúdez-Couso A, Fernández-Calviño D, Rodríguez-Salgado I, Nóvoa-Muñoz JC, Arias-Estévez M (2012) Comparison of batch, stirred flow chamber, and column experiments to study adsorption, desorption and transport of carbofuran within two acidic soils. Chemosphere 88:106–112

    Article  Google Scholar 

  • Carrasquillo AJ, Bruland GL, MacKay AA, Vasudevan D (2008) Sorption of ciprofloxacin and oxytetracycline zwitterions to soils and soil minerals: Influence of compound structure. Environ Sci Technol 42(20):7634–7642

    Article  CAS  Google Scholar 

  • Chee-Sanford JC, Mackie RI, Koike S, Krapac IG, Lin YF, Yannarell AC, Maxwell S, Aminov RI (2009) Fate and transport of antibiotic residues and antibiotic resistance genes following land application of manure waste. J Environ Qual 38(3):1086–1108

    Article  CAS  Google Scholar 

  • Chen WR, Huang CH (2010) Adsorption and transformation of tetracycline antibiotics with aluminum oxide. Chemosphere 79:779–785

    Article  CAS  Google Scholar 

  • Clarke BO, Smith SR (2011) Review of ‘emerging’ organic contaminants in biosolids and assessment of international research priorities for the agricultural use of biosolids. Environ Int 37(1):226–247

    Article  CAS  Google Scholar 

  • Díaz-Cruz MS, López de Alda MJ, Barceló D (2003) Environmental behavior and analysis of veterinary and human drugs in soils sediments and sludge. Trends Anal Chem 22(6):340–351

    Article  Google Scholar 

  • Figueroa-Diva RA, Vasudevan D, MacKay AA (2010) Trends in soil sorption coefficients within common antimicrobial families. Chemosphere 79:786–793

    Article  CAS  Google Scholar 

  • Fisher PMJ, Scott R (2008) Evaluating and controlling pharmaceutical emissions from dairy farms: a critical first step in developing a preventative management approach. J Clean Prod 16:1437–1446

    Article  Google Scholar 

  • Giger W, Alder AC, Golet EM, Kohler HE, McArdell CS, Molnar E, Siegrist H, Suter MJ (2003) Occurrence and fate of antibiotics as trace contaminants in wastewaters sewage sludges and surface waters. Chimia 57:485–491

    Article  CAS  Google Scholar 

  • Gu C, Karthikeyan KG (2005) Interaction of tetracycline with aluminum and iron hydrous oxides. Environ Sci Technol 39:2660–2667

    Article  CAS  Google Scholar 

  • Gu C, Karthikeyan KG, Sibley SD, Pedersen JA (2007) Complexation of the antibiotic tetracycline with humic acid. Chemosphere 66(8):1494–1501

    Article  CAS  Google Scholar 

  • Hamscher G, Sczesny S, Höper H, Nau H (2002) Determination of persistent tetracycline residues in soil fertilized with liquid manure by high-performance liquid chromatography with electrospray ionization tandem mass spectrometry. Anal Chem 74:1509–1518

    Article  CAS  Google Scholar 

  • Huang X, Liu C, Li K, Liu F, Liao D, Liu L, Zhu G, Liao J (2013) Occurrence and distribution of veterinary antibiotics and tetracycline resistance genes in farmland soils around swine feedlots in Fujian Province China. Environ Sci Pollut Res 20:9066–9074

    Article  CAS  Google Scholar 

  • Iglesias A, Nebot C, Miranda JM, Vázquez BI, Cepeda A (2012) Detection and quantitative analysis of 21 veterinary drugs in river water using high-pressure liquid chromatography coupled to tandem mass spectrometry. Environ Sci Pollut Res 19:3235–3249

    Article  CAS  Google Scholar 

  • Iglesias A, Nebot C, Vázquez BI, Miranda JM, Franco-Abuín CM, Cepeda A (2014) Detection of veterinary drug residues in surface waters collected nearby farming areas in Galicia North of Spain. Environ Sci Pollut Res 21(3):2367–2377

    Article  CAS  Google Scholar 

  • Ji L, Wan Y, Zheng S, Zhu D (2011) Adsorption of tetracycline and sulfamethoxazole on crop residue-derived ashes: implication for the relative importance of black carbon to soil sorption. Environ Sci Technol 45:5580–5586

    Article  CAS  Google Scholar 

  • Kang J, Liu H, Zheng YM, Qu J, Chen JP (2010) Systematic study of synergistic and antagonistic effects on adsorption of tetracycline and copper onto a chitosan. J Colloid Interface Sci 344(1):117–125

    Article  CAS  Google Scholar 

  • Kong W, Li C, Dolhi JM, Li S, He J, Qiao M (2012) Characteristics of oxytetracycline sorption and potential bioavailability in soils with various physical–chemical properties. Chemosphere 87:542–548

    Article  CAS  Google Scholar 

  • Kumar K, Gupta SC, Chander Y, Singh AK (2005) Antibiotic use in agriculture and its impact on the terrestrial environment. Adv Agron 87:1–54

    Article  CAS  Google Scholar 

  • Kümmerer K (2009) The presence of pharmaceuticals in the environment due to human use—Present knowledge and future challenges. J Environ Manag 90(8):2354–2366

    Article  Google Scholar 

  • Leung HW, Minh TB, Murphy MB, Lam JCW, So MK, Martin M, Lam PKS, Richardson BJ (2012) Distribution fate and risk assessment of antibiotics in sewage treatment plants in Hong Kong South China. Environ Int 42:1–9

    Article  CAS  Google Scholar 

  • Lin Y, Xu S, Li J (2013) Fast and highly efficient tetracyclines removal from environmental waters by graphene oxide functionalized magnetic particles. Chem Eng J 225:679–685

    Article  CAS  Google Scholar 

  • López-Peñalver JJ, Sánchez-Polo M, Gómez-Pacheco CV, Rivera-Utrilla J (2010) Photodegradation of tetracyclines in aqueous solution by using UV and UV/H2O2 oxidation processes. J Chem Technol Biotechnol 85:1325–1333

    Article  Google Scholar 

  • López-Periago JE, Arias-Estévez M, Nóvoa-Muñoz JC, Fernández-Calviño D, Soto B, Pérez-Novo C, Simal-Gándara J (2008) Copper retention kinetics in acid soils. Soil Sci Soc Am J 72:63–72

    Article  Google Scholar 

  • Oldenkamp R, Huijbregts MAJ, Hollander A, Versporten A, Goossens H, Ragas AMJ (2013) Spatially explicit prioritization of human antibiotics and antineoplastics in Europe. Environ Int 51:13–26

    Article  CAS  Google Scholar 

  • Pérez-Novo C, Fernández-Calviño D, Bermúdez-Couso A, López-Periago JE, Arias-Estévez M (2011) Influence of phosphorus on Cu sorption kinetics: Stirred flow chamber experiments. J Hazard Mater 185:220–226

    Article  Google Scholar 

  • Pils JV, Laird DA (2007) Sorption of tetracycline and chlortetracycline on K- and Ca-saturated soil clays humic substances and clay-humic complexes. Environ Sci Technol 41:1928–1933

    Article  CAS  Google Scholar 

  • Rivera-Utrilla J, Gómez-Pacheco CV, Sánchez-Polo M, López-Peñalver JJ, Ocampo-Pérez R (2013) Tetracycline removal from water by adsorption/bioadsorption on activated carbons and sludge-derived adsorbents. J Environ Manag 131:16–24

    Article  CAS  Google Scholar 

  • Sassman SA, Lee LS (2005) Sorption of three tetracyclines by several soils: Assessing the role of pH and cation exchange. Environ Sci Technol 39:7452–7459

    Article  CAS  Google Scholar 

  • Spanish Agency for Drugs and Sanitary Products (2011) Sales of veterinary antimicrobial agents in Spain in 2009 Madrid http://www.aemps.gob.es/en/informa/notasInformativas/medicamentosVeterinarios/2011/docs/ventas-antimicrobianos_Espana-2009.pdf

  • Suárez S, Reif R, Lema JM, Omil F (2012) Mass balance of pharmaceutical and personal care products in a pilot-scale single-sludge system: Influence of T SRT and recirculation ratio. Chemosphere 89:164–171

    Article  Google Scholar 

  • Teixidó M, Granados M, Prat MD, Beltrán JL (2012) Sorption of tetracyclines onto natural soils: Data analysis and prediction. Environ Sci Pollut Res 19:3087–3095

    Article  Google Scholar 

  • Torre A, Iglesias I, Carballo M, Ramírez P, Muñoz MJ (2012) An approach for mapping the vulnerability of European Union soils to antibiotic contamination. Sci Total Environ 414:672–679

    Article  Google Scholar 

  • Wu L, Pan X, Chen L, Huang Y, Teng Y, Luo Y, Christie P (2013) Occurrence and distribution of heavy metals and tetracyclines in agricultural soils after typical land use change in east China. Environ Sci Pollut Res 20:8342–8354

    Article  CAS  Google Scholar 

  • Yin Y, Allen HE, Huang CP, Sparks DL, Sanders PF (1997) Kinetics of mercury(II) adsorption and desorption on soil. Environ Sci Technol 31:496–503

    Article  CAS  Google Scholar 

  • Zhang Z, Sun K, Gao B, Zhang G, Liu X, Zhao Y (2011) Adsorption of tetracycline on soil and sediment: Effects of pH and the presence of Cu(II). J Hazard Mater 190:856–862

    Article  CAS  Google Scholar 

Download references

Acknowledgments

The authors acknowledge the financial support of CIA3, which was granted by FEDER founds through the program of Consolidation and Arrangement of Research Units from Consellería de Educación (Xunta de Galicia, Spain). We thank the editor and the anonymous reviewers involved in the revision process, who have greatly aided to improve the original manuscript.

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Authors and Affiliations

  1. Department of Plant and Environmental Sciences, University of Copenhagen, Frederiksberg, Denmark

    David Fernández-Calviño

  2. Soil Science and Agricultural Chemistry Area, Faculty of Sciences, University of Vigo, Campus Univ. Ourense, Ourense, Galicia, Spain

    Alipio Bermúdez-Couso, Manuel Arias-Estévez & Juan Carlos Nóvoa-Muñoz

  3. Department of Soil Science and Agricultural Chemistry, Engineering Polytechnic School, University of Santiago de Compostela, Campus Univ. Lugo, Lugo, Galicia, Spain

    Maria J. Fernández-Sanjurjo, Esperanza Álvarez-Rodríguez & Avelino Núñez-Delgado

Authors
  1. David Fernández-Calviño
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  2. Alipio Bermúdez-Couso
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  3. Manuel Arias-Estévez
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  4. Juan Carlos Nóvoa-Muñoz
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  5. Maria J. Fernández-Sanjurjo
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  7. Avelino Núñez-Delgado
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Correspondence to Avelino Núñez-Delgado.

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Responsible editor: Zhihong Xu

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Fernández-Calviño, D., Bermúdez-Couso, A., Arias-Estévez, M. et al. Kinetics of tetracycline, oxytetracycline, and chlortetracycline adsorption and desorption on two acid soils. Environ Sci Pollut Res 22, 425–433 (2015). https://doi.org/10.1007/s11356-014-3367-9

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  • DOI: https://doi.org/10.1007/s11356-014-3367-9

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