Skip to main content
Log in

The optimization of the antibiotics extraction from wastewaters and manure using Box–Behnken experimental design

  • Original Paper
  • Published:
International Journal of Environmental Science and Technology Aims and scope Submit manuscript

Abstract

The aim of this study was to optimize the solid-phase extraction method of several antibiotics in order to determine their concentration in wastewater (influent and effluent) and manure samples. The selected antibiotics for the present study were ampicillin, ceftazidime, cefepime, imipenem, piperacillin/tazobactam, tetracycline, erythromycin, ciprofloxacin, norfloxacin, vancomycin, gentamicin, sulfamethoxazole/trimethoprim. The optimum extraction conditions were established using a three- and four-factor Box–Behnken design under response surface methodology. The extraction of the antibiotics from liquid matrices was performed on several types of cartridges (Oasis HLB, Strata-X and HyperSep Retain PEP). With Oasis HLB cartridges were obtained the best recovery degrees (74.81 and 105.39% with the exception of tazobactam 58.70% and gentamicin 51.57%). This type of cartridges was further used for all of the samples collected for this study. In the case of the manure samples were tested two different extraction techniques: ultrasounds- and microwave-assisted solvent extraction, the first one being the most efficient. All the extractions obtained during the present study were evaluated by high-performance liquid chromatography with two detectors, diode array and mass spectrometer in positive ionization mode.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5

Similar content being viewed by others

References

  • Ašperger D, Mutavdžić D, Babić S, Horvat AJM, Kaštelan-Macan M (2006) Solid-phase extraction and TLC quantification of enrofloxacin, oxytetracycline, and trimethoprim in wastewater. JPC-J Planar Chromatogr 19:129–134

    Article  Google Scholar 

  • Chang X, Meyer MT, Liu X, Zhao Q, Chen H, Chen J, Qui Z, Yang L, Cao J, Shu W (2010) Determination of antibiotics in sewage from hospitals, nursery and slaughter house, wastewater treatment plant and source water in Chongqing region of Three Gorge Reservoir in China. Environ Pollut 158:1444–1450

    Article  CAS  Google Scholar 

  • Chen H, Liu S, Xu XR, Zhou GJ, Liu SS, Yue WZ, Sun KF, Ying GG (2015) Antibiotics in the coastal environment of the Hailing Bay region, South China Sea: spatial distribution, source analysis and ecological risks. Mar Pollut Bull 95:365–373

    Article  CAS  Google Scholar 

  • Dahl EL, Shock JL, Shenai BR, Gut J, DeRisi JL, Rosenthal PJ (2006) Tetracyclines specifically target the apicoplast of the malaria parasite Plasmodium falciparum. Antimicrob Agents Chemother 50:3124–3131

    Article  CAS  Google Scholar 

  • Ding Y, Zheng J, Xia X, Ren T, Kan J (2016) Box-Behnken design for the optimization of nanoscale retrograded starch formation by high-power ultrasonication. LWT—Food Sci Technol 67:206–213

    CAS  Google Scholar 

  • Feitosa-Felizzola J, Temime B, Chiron S (2007) Evaluating on-line solid-phase extraction coupled to liquid chromatography-ion trap mass spectrometry for reliable quantification and confirmation of several classes of antibiotics in urban wastewaters. J Chromatogr A 1164:95–104

    Article  CAS  Google Scholar 

  • Ferreira SLC, Bruns RE, Ferreira HS, Matos GD, David JM, Brandão GC, da Silva EGP, Portugal LA, dos Reis PS, Souza AS, dos Santos WNL (2007) Box-Behnken design: an alternative for the optimization of analytical methods. Anal Chim Acta 597:179–186

    Article  CAS  Google Scholar 

  • Fouladian HR, Behbahani M (2015) Solid phase extraction of Pb(II) and Cd(II) in food, soil, and water samples based on 1-(2-pyridylazo)-2-naphthol-functionalized organic–inorganic mesoporous material with the aid of experimental design methodology. Food Anal Methods 8:982–993

    Article  Google Scholar 

  • García-Campaña AM, Gámiz-Gracia L, Lara FJ, del Olmo Iruela M, Cruces-Blanco C (2009) Applications of capillary electrophoresis to the determination of antibiotics in food and environmental samples. Anal Bioanal Chem 395:967–986

    Article  Google Scholar 

  • García-Galán MJ, Díaz-Cruz MS, Barceló D (2010) Determination of 19 sulfonamides in environmental water samples by automated on-line solid-phase extraction-liquid chromatography-tandem mass spectrometry (SPE-LC-MS/MS). Talanta 81:355–366

    Article  Google Scholar 

  • Ho YB, Zakaria MP, Latif PA, Saari N (2012) Simultaneous determination of veterinary antibiotics and hormone in broiler manure, soil and manure compost by liquid chromatography–tandem mass spectrometry. J Chromatogr A 1262:160–168

    Article  CAS  Google Scholar 

  • Hu X, Luo Y, Zhou Q (2010) Simultaneous analysis of selected typical antibiotics in manure by microwave-assisted extraction and LC–MS. Chromatographia 71(3/4):217–223

    Article  CAS  Google Scholar 

  • Joshi S, Sharma A, Rawat MSM, Dhiman C (2009) Development of conditions for rapid thin-layer chromatography of β-lactam antibiotics. JPC-J Planar Chromatogr 22:435–437

    Article  CAS  Google Scholar 

  • Kemper N (2008) Veterinary antibiotics in the aquatic and terrestrial environment. Ecol Indic 8:1–13

    Article  CAS  Google Scholar 

  • Kümmerer K (2009) Antibiotics in the aquatic environment—a review—Part I. Chemosphere 75:417–434

    Article  Google Scholar 

  • Li B, Zhang T, Xu Z, Fang HHP (2009) Rapid analysis of 21 antibiotics of multiple classes in municipal wastewater using ultra performance liquid chromatography-tandem mass spectrometry. Anal Chim Acta 645:64–72

    Article  CAS  Google Scholar 

  • Li L, Sun M, Zhou H, Zhou Y, Chen P, Min H, Shen G (2015) Response surface optimization of a rapid ultrasound-assisted extraction method for simultaneous determination of tetracycline antibiotics in manure. J Anal Methods Chem 2015, Article ID290903, 10 pages

  • Loganathan B, Phillips M, Mowery H, Jones-Lepp TL (2009) Contamination profiles and mass loadings of macrolide antibiotics and illicit drugs from a small urban wastewater treatment plant. Chemosphere 75:70–77

    Article  CAS  Google Scholar 

  • Matinca D (2002) Antibiotice. Ed. Medicală Universitară „Iuliu Haţieganu”, Cluj-Napoca

  • McClure EL, Wong CS (2007) Solid phase microextraction of macrolide, trimethoprim, and sulfonamide antibiotics in wastewaters. J Chromatogr A 1169:53–62

    Article  CAS  Google Scholar 

  • Modi CM, Mody SK, Patel HB, Dudhatra GB, Kumar A, Sheikh TJ (2011) Growth promoting use of antimicrobial agents in animals. J of Appl Pharm Sci 01(08):33–36

    Google Scholar 

  • Opriş O, Coman V, Copaciu F, Vlassa M (2012) Solid phase extraction and high performance thin layer chromatography quantification of some antibiotics from surface waters. JPC-J Planar Chromatogr 25(6):516–522

    Article  Google Scholar 

  • Opriş O, Copaciu F, Soran LM, Ristoiu D, Niinemets Ü, Copolovici L (2013) Influence of nine antibiotics on key secondary metabolites and physiological characteristics in Triticum aestivum: leaf volatiles as a promising tool to assess toxicity. Ecotoxical Environ Saf 87:70–79

    Article  Google Scholar 

  • Rao NR, Venkateswarlu N, Narsimha R (2008) Determination of antibiotics in aquatic environment by solid-phase extraction followed by liquid chromatography-electrospray ionization mass spectrometry. J Chromatogr A 1187:151–164

    Article  Google Scholar 

  • Reda RM, Ibrahim RE, El-Nobi GA, El-Bouhy ZM (2013) Effect of oxytetracycline and florfenicol as growth promoters on the health status of cultured Oreochromis niloticus. Egypt J Aquat Res 39(4):241–248

    Article  Google Scholar 

  • Rossmann J, Schubert S, Gurke R, Oertel R, Kirch W (2014) Simultaneous determination of most prescribed antibiotics in multiple urban wastewater by SPE-LC-MS/MS. J Chromatogr B Analyt Technol Biomed Life Sci 969:162–170

    Article  CAS  Google Scholar 

  • Sapkota A, Sapkota AR, Kucharski M, Burke J, McKenzie S, Walker P, Lawrence R (2008) Aquaculture practices and potential human health risks: current knowledge and future priorities. Environ Int 34:1215–1226

    Article  Google Scholar 

  • Solliec M, Roy-Lachapelle A, Gasser MO, Coté C, Généreux M, Sauvé S (2016) Fractionation and analysis of veterinary antibiotics and their related degradation products in agricultural soils and drainage waters following swine manure amendment. Sci Total Environ 543:524–535

    Article  CAS  Google Scholar 

  • Sui Q, Cao X, Lu S, Zhao W, Qiu Z, Yu G (2015) Occurrence, sources and fate of pharmaceuticals and personal care products in the groundwater: a review. Emerg Contam 1(1):14–24

    Article  Google Scholar 

  • Surducan E, Surducan V (2008) Process and installation for dynamic processing of the substance in a microwave power field. Patent no. 122063

  • Tong L, Li P, Wang Y, Zhu K (2009) Analysis of veterinary antibiotic residues in swine wastewater and environmental water samples using optimized SPE-LC/MS/MS. Chemosphere 74:1090–1097

    Article  CAS  Google Scholar 

  • Van den Meersche T, Pamel EV, Poucke CV, Herman L, Heyndrickx M, Rasschaert G, Daeseleire E (2016) Development, validation and application of an ultra high performance liquid chromatographic-tandem mass spectrometric method for the simultaneous detection and quantification of five different classes of veterinary antibiotics in swine manure. J Chromatogr A 1429:248–257

    Article  Google Scholar 

  • Zuloaga O, Navarro P, Bizkarguenaga E, Iparraguirre A, Vallejo A, Olivares M, Prieto A (2012) Overview of extraction, clean-up and detection techniques for the determination of organic pollutants in sewage sludge: a review. Anal Chim Acta 736:7–29

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work was funded through the EEA 2009–2014 Financial Mechanism under the RO04—Reduction of hazardous substances scheme, Grant Number 3499/20.05.2015. The authors thank Dr. E. Surducan team (INCDTIM Cluj-Napoca) for all their experimental support with the device for dynamic processing of the substance in power microwave field.

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to M. L. Soran.

Additional information

Editorial responsibility: M. Abbaspour.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Opriş, O., Soran, M.L., Lung, I. et al. The optimization of the antibiotics extraction from wastewaters and manure using Box–Behnken experimental design. Int. J. Environ. Sci. Technol. 14, 473–480 (2017). https://doi.org/10.1007/s13762-016-1165-2

Download citation

  • Received:

  • Revised:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s13762-016-1165-2

Keywords

Navigation