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Development and application of magnetic solid phase extraction in tandem with liquid–liquid extraction method for determination of four tetracyclines by HPLC with UV detection

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Abstract

A novel HPLC-UV method was developed for the determination of four tetracyclines based on magnetic solid phase extraction in tandem with liquid–liquid extraction. The water-soluble amino functionalized magnetite nanoparticle (MNP-NH2) was used as an adsorbent for extraction/preconcentration of tetracycline, oxytetracycline, chlortetracycline, and doxycycline from bovine milk samples. Fourier transform infrared spectrometer, transmission electron microscope, X-ray diffraction, and elemental analyze techniques were used to characterize the material. Some key parameters which influence liquid–liquid extraction and magnetic dispersive solid-phase extraction procedure, including volume of extraction solvent, the amount of adsorbent, the pH, extraction and desorption time, the composition of the eluent, and elution frequency were investigated. The proposed method exhibited a linear range of 50.0–2500.0 μg L−1 (r2 = 0.9941) with and good reproducibility (RSD < 2.2%, n = 3). The limit of detection and quantification were 40.0 and 50.0 μg L−1. This method was verified using milk sample spiked with four tetracyclines (100.0–200.0 μg L−1), and accuracies of 87.8−107.5%, which confirmed its applicability in real-sample analysis. The proposed method also shows potential application prospects for other water-soluble adsorbents.

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References

  • Ahamad T, Naushad M, Eldesoky GE, Al-Saeedi SI, Nafady A, Al-Kadhi NS, Al-Muhtaseb AH, Khan AA, Khan A (2019) Effective and fast adsorptive removal of toxic cationic dye (MB) from aqueous medium using amino-functionalized magnetic multiwall carbon nanotubes. J Mol Liq 282:154–161

    Article  CAS  Google Scholar 

  • Al-Afy N, Sereshti H, Hijazi A, Rashidi Nodeh H (2018) Determination of three tetracyclines in bovine milk using magnetic solid phase extraction in tandem with dispersive liquid-liquid microextraction coupled with HPLC. J Chromatogr B 1092:480–488

    Article  CAS  Google Scholar 

  • Anastassiades M, Lehotay SJ, Štajnbaher D, Schenck FJ (2003) Fast and easy multiresidue method employing acetonitrile extraction/partitioning and “dispersive solid-phase extraction” for the determination of pesticide residues in produce. J AOAC Int 86(2):412–431

    Article  CAS  Google Scholar 

  • Baile P, Vidal L, Canals A (2019) A modified zeolite/iron oxide composite as a sorbent for magnetic dispersive solid-phase extraction for the preconcentration of nonsteroidal anti-inflammatory drugs in water and urine samples. J Chromatogr A 1603:33–43

    Article  CAS  Google Scholar 

  • Brion M, Lambs L, Berthon G (1986) Metal ion-tetracycline interactions in biological fluids. Part 6. Formation of copper(ii) complexes with tetracycline and some of its derivatives and appraisal of their biological significance. Inorg Chim Acta 123(2):61–68

    Article  CAS  Google Scholar 

  • Buldini PL, Ricci L, Sharma JL (2002) Recent applications of sample preparation techniques in food analysis. J Chromatogr A 975(1):47–70

    Article  CAS  Google Scholar 

  • Chang PH, Li Z, Jean JS, Jiang WT, Wu Q, Kuo CY, Kraus J (2013) Desorption of tetracycline from montmorillonite by aluminum, calcium, and sodium: an indication of intercalation stability. Int J Environ Sci Technol 11(3):633–644

    Article  Google Scholar 

  • Chen L, Liu J, Zeng Q, Wang H, Yu A, Zhang H, Ding L (2009) Preparation of magnetic molecularly imprinted polymer for the separation of tetracycline antibiotics from egg and tissue samples. J Chromatogr A 1216(18):3710–3719

    Article  CAS  Google Scholar 

  • Deng Y-H, Wang C-C, Hu J-H, Yang W-L, Fu S-K (2005) Investigation of formation of silica-coated magnetite nanoparticles via sol–gel approach. Colloid Surface A 262(1–3):87–93

    Article  CAS  Google Scholar 

  • Dominguez-Salas P, Galiè A, Omore A, Omosa E, Ouma E (2019) Contribution of milk production to food and nutrition security. In: Pasquale F, Elliot MB, Jock RA (eds) Encyclopedia of food security and sustainability (volume 3), 1st edn. Elservier, Amsterdam, pp 278–291

    Chapter  Google Scholar 

  • Gul H, Demirkaya E, Eser B, Kapucu H, Tuncbilek V, Simsek D (2015) Colchicine measurement using LC-MS/MS with ESI in serum with liquid liquid extraction. Pediatric Rheumatol 13(Suppl 1):P118

    Article  Google Scholar 

  • Karaoglu O, Alpdogan G, Zor SD, Bildirir H, Ertas E (2019) Efficient solid phase extraction of α-tocopherol and β-sitosterol from sunflower oil waste by improving the mesoporosity of the zeolitic adsorbent. Food Chem 311:125890

    Article  Google Scholar 

  • 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

    Article  CAS  Google Scholar 

  • Lambs L, Reverend DL, Kozlowski H, Berthon G (1988) Metal ion-tetracycline interactions in biological fluids. 9. Circular dichroism spectra of calcium and magnesium complexes with tetracycline, oxytetracycline, doxycycline, and chlortetracycline and discussion of their binding modes. Inorg Chem 27(17):3001–3012

    Article  CAS  Google Scholar 

  • Liu F, Xiong W, Liu J, Cheng Q, Cheng G, Shi L, Zhang Y (2018) Novel amino-functionalized carbon material derived from metal organic framework: a characteristic adsorbent for U(VI) removal from aqueous environment. Colloid Surf A 556:72–80

    Article  CAS  Google Scholar 

  • Loftin KA, Adams CD, Meyer MT, Surampalli R (2008) Effects of ionic strength, temperature, and ph on degradation of selected antibiotics. J Environ Qual 37(2):378–386

    Article  CAS  Google Scholar 

  • Lv YK, Zhao CX, Li P, He YD, Yang ZR, Sun HW (2013) Preparation of doxycycline-imprinted magnetic microspheres by inverse-emulsion suspension polymerization for magnetic dispersion extraction of tetracyclines from milk samples. J Sep Sci 36(16):2656–2663

    Article  CAS  Google Scholar 

  • Meng C, Zhikun W, Qiang L, Chunling L, Shuangqing S, Songqing H (2018) Preparation of amino-functionalized Fe3O4@mSiO2 core-shell magnetic nanoparticles and their application for aqueous Fe3+ removal. J Hazard Mater 341:198–206

    Article  Google Scholar 

  • National Food Safety Standard of P.R.C. (2007) GB/T21317-2007 Determination of tetracyclines residues in food of animal origin—LC-MS/MS method and HPLC method

  • Paleologos EK, Kontominas MG (2004) On-line solid-phase extraction with surfactant accelerated on-column derivatization and micellar liquid chromatographic separation as a tool for the determination of biogenic amines in various food substrates. Anal Chem 76(5):1289–1294

    Article  CAS  Google Scholar 

  • Pinheiro PC, Fateixa S, Nogueira HIS, Trindade T (2018) Magnetite-supported gold nanostars for the uptake and sers detection of tetracycline. Nanomaterials (Basel) 9(1):31

    Article  Google Scholar 

  • Reymond C, Dubuis A, Le Masle A, Colas C, Chahen L, Destandau E et al (2019) Characterization of liquid-liquid extraction fractions from lignocellulosic biomass by high performance liquid chromatography hyphenated to tandem high-resolution mass spectrometry. J Chromatogr A 1610:460569

    Article  Google Scholar 

  • Rodriguez JA, Espinosa J, Aguilar-Arteaga K, Ibarra IS, Miranda JM (2010) Determination of tetracyclines in milk samples by magnetic solid phase extraction flow injection analysis. Microchim Acta 171(3–4):407–413

    Article  CAS  Google Scholar 

  • Šafaříková M, Šafařík I (1999) Magnetic solid-phase extraction. J Magn Magn Mater 194(1–3):108–112

    Article  Google Scholar 

  • Solliec M, Roy-Lachapelle A, Gasser MO, Cote C, Genereux M, Sauve 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(Pt A):524–535

    Article  CAS  Google Scholar 

  • Song J, Niu X, Li X-M, He T (2018) Selective separation of copper and nickel by membrane extraction using hydrophilic nanoporous ion-exchange barrier membranes. Process Saf Environ Prot 113:1–9

    Article  CAS  Google Scholar 

  • Song Y, Yang LY, Wang YG, Yu D, Shen J, Ouyang XK (2019) Highly efficient adsorption of Pb(II) from aqueous solution using amino-functionalized SBA-15/calcium alginate microspheres as adsorbent. Int J Biol Macromol 125:808–819

    Article  CAS  Google Scholar 

  • Tsai WH, Huang TC, Huang JJ, Hsue YH, Chuang HY (2009) Dispersive solid-phase microextraction method for sample extraction in the analysis of four tetracyclines in water and milk samples by high-performance liquid chromatography with diode-array detection. J Chromatogr A 1216(12):2263–2269

    Article  CAS  Google Scholar 

  • Wei YH, Li XY, Gao J, Liu JJ, Yuan D, Yin BC et al (2018) Size-dependent modulation of CoOOH nanoflakes light scattering for rapid and selective detection of tetracycline in milk. J Anal Test 2(4):332–341

    Article  Google Scholar 

  • Weng R, Sun L, Jiang L, Li N, Ruan G, Li J et al (2019) Electrospun graphene oxide-doped nanofiber-based solid phase extraction followed by high-performance liquid chromatography for the determination of tetracycline antibiotic residues in food samples. Food Anal Methods 12(7):1594–1603

    Article  Google Scholar 

  • Yavuz E, Tokalioglu S, Patat S (2018) Core-shell Fe3O4 polydopamine nanoparticles as sorbent for magnetic dispersive solid-phase extraction of copper from food samples. Food Chem 263:232–239

    Article  CAS  Google Scholar 

  • Yu Y, Chen L, Fang Y, Jia X, Chen J (2019) High temperatures can effectively degrade residual tetracyclines in chicken manure through composting. J Hazard Mater 380:120862

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work is a part of the National Key R&D Program of China (No: 2017YFC1601101). Tianjin Scientific and Technology Support Program Funding Agency (No.16YFZCNC00730).

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Authors and Affiliations

  1. Tianjin Key Laboratory of Risk Assessment and Control Technology for Environment and Food Safety, Tianjin Institute of Environmental and Operational Medicine, No. 1, DaLi Road, HePing District, Tianjin, 300050, China

    Hong-zhi Tang, Yong-hui Wang, Shuang Li, Jin Wu, Zhi-xian Gao & Huan-ying Zhou

  2. Laboratory of Deep Sea Microbial Cell Biology, Institute of Deep-Sea Science and Engineering, Chinese Academy of Sciences, Sanya, China

    Hong-zhi Tang

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  1. Hong-zhi Tang
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  2. Yong-hui Wang
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  3. Shuang Li
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  4. Jin Wu
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  5. Zhi-xian Gao
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  6. Huan-ying Zhou
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Correspondence to Zhi-xian Gao or Huan-ying Zhou.

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Tang, Hz., Wang, Yh., Li, S. et al. Development and application of magnetic solid phase extraction in tandem with liquid–liquid extraction method for determination of four tetracyclines by HPLC with UV detection. J Food Sci Technol 57, 2884–2893 (2020). https://doi.org/10.1007/s13197-020-04320-w

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  • DOI: https://doi.org/10.1007/s13197-020-04320-w

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