Skip to main content
SpringerLink
Log in

Magnetic Graphene Solid-Phase Extraction for the Determination of 47 Kinds of Non-steroidal Anti-inflammatory Drug Residues in Animal Food with Liquid Chromatography Tandem Mass Spectrometry

  • Published:
Food Analytical Methods Aims and scope Submit manuscript

Abstract

Based on magnetic graphene (Fe3O4-G), a liquid chromatography with tandem mass spectrometric detection (LC-MS/MS) method coupled with magnetic solid-phase extraction was developed for the simultaneous detection of 47 kinds of nonsteroidal anti-inflammatory drug (NSAID) residues in meat of swine, chicken, and bovine. The samples were extracted with acetonitrile-phosphate, then the extracts were purified by dispersed solid-phase extraction based on magnetic graphene (Fe3O4-G). The linearity range is 0.1–50 μg L−1. Limits of detection were between 0.1 μg kg−1 and 0.5 μg kg−1, and limits of quantification were between 0.5 μg kg−1 and 1.0 μg kg−1. The average recoveries were 72.4–97.1% at spiking levels. The inter-day RSDs varied from 5.3 to 12.6%. Due to the advantages of easy collection of magnetic solid-phase extraction materials, the method was more rapid and efficient for the enrichment and separation without filling columns. The sensitivity, precision, and accuracy method was suitable for simultaneous detection of multi-component residues of nonsteroidal anti-inflammatory drugs.

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

Access this article

Log in via an institution

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

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3

Similar content being viewed by others

References

  • Abbas P, Saeid A, Sanaz A, Vinod Kumar G (2016) Highly sensitive and efficient voltammetric determination of ascorbic acid in food and pharmaceutical samples from aqueous solutions based on nanostructure carbon paste electro de as a sensor. J Mol Liq 216:387–391

    Article  CAS  Google Scholar 

  • Afkhami A, Moosavi R (2010) Adsorptive removal of Congo red, a carcinogenic textile dye, from aqueous solutions by maghemite nanoparticles. J Hazard Mater 174:398–403

    Article  CAS  PubMed  Google Scholar 

  • Chang KC, Lin JS, Cheng C (2015) Online eluent-switching technique coupled anion-exchange liquid chromatography-ion trap tandem mass spectrometry f or analysis of non-steroidal anti-inflammatory drugs in pig serum. Journal of Chromatography A 1422:222–229

    Article  CAS  PubMed  Google Scholar 

  • Commission Regulation (2010) (EU) No. 37/2010 of 22 December 2009 on pharmacologically active substances and their classification regarding maximum residue limits in foodstuffs of animal origin. Off J Eur Union L 15:1

    Google Scholar 

  • Dowling G, Malone E (2011) Analytical strategy for the confirmatory analysis of the non-steroidal anti-inflammatory drugs firocoxib, propyphenazone, ramifenazone and piroxicam in bovine plasma by liquid chromatography tandem mass spectrometry. J Pharm Biomed Anal 56(2):359–365

    Article  CAS  PubMed  Google Scholar 

  • Dowling G, Gallo P, Malone E, Reqan L (2009) Rapid confirmatory analysis of non-steroidal anti-inflammatory drugs in bovine milk by rapid resolution liquid chromatography tandem mass spectrometry. J Chromatogr A 1216(46):8117–8131

    Article  CAS  PubMed  Google Scholar 

  • Fouladgar M, Ahmadzadeh S (2016) Application of a nanostructured sensor based on NiO nanoparticles modified carbon paste electrode for determination of methyldopa in the presence of folic acid. Appl Surf Sci 379:150–155

    Article  CAS  Google Scholar 

  • Gouda AA, El-Sayed MIK, Amin AS, El Sheikh R (2013) Spectrophotometric and spectrofluorometric methods for the determination of non-steroidal anti-inflammatory drugs: a review. Arab J Chem 6(2):145–163

    Article  CAS  Google Scholar 

  • Heshmatollah A, Amiri A, Tarahomi M, Maleki B (2018) Magnetic solid-phase extraction of non-steroidal anti-inflammatory drugs from environmental water samples using polyamidoamine dendrimer functionalized with magnetite nanoparticles as a sorbent. Talanta 183:149–157

    Article  CAS  Google Scholar 

  • Hoshina K, Horiyama S, Matsunaga H, Haqinaka J (2011) Simultaneous determination of non-steroidal anti-inflammatory drugs in river water samples by liquid chromatography-tandem mass spectrometry using molecularly imprinted polymers as a pretreatment column. J Pharm Biomed Anal 55(5):916–922

    Article  CAS  PubMed  Google Scholar 

  • Hu T, Peng T, Li XJ, Chen DD, Dai HH, Deng XJ, Yue ZF, Wang GM, Shen JZ, Xia X, Ding SY, Zhou YN, Zhu AL, Jiang HY (2012) Simultaneous determination of thirty non-steroidal anti-inflammatory drug residues in swine muscle by ultra-high-performance liquid chromatography with tandem mass spectrometry. J Chromatogr A 1219(1):104–113

    Article  CAS  PubMed  Google Scholar 

  • Igualada C, Moragues F, Pitarch J (2007) Rapid method for the determination of non-steroidal anti-inflammatory drugs in animal tissue by liquid chromatography-mass spectrometry with ion-trap detector. Anal Chim Acta 586(1–2):432–439

    Article  CAS  PubMed  Google Scholar 

  • Jedziniak P, Szprengier-Juszkiewicz T, Olejnik M, Zmudzki J (2010) Determination of non-steroidal anti-inflammatory drugs residues in animal muscles by liquid chromatography–tandem mass spectrometry. Anal Chim Acta 672:85–92

    Article  CAS  PubMed  Google Scholar 

  • Jedziniak P, Olejnik M, Pietruk K, Protasiuk E, Szprengier-Juszkiewicz T, Żmudzki J (2016) Simultaneous determination of residues of non-steroidal anti-inflammatory drugs and glucocorticosteroids in animal muscle by liquid chromatography-tandem mass spectrometry. Food Anal Methods 9(6):1837–1848

    Article  Google Scholar 

  • Kassim AA, Rezayi MA, Ahmadzadeh SA, Rounaghi GB, Mohajeri MB, Yusof NAA, Tee TWA, Heng LYA, Abdullah AHA (2009) A novel ion - Selective polymeric membrane sensor for determining thallium(I) with high selectivity. Materials Science and Engineering Conference Series 17(1):012010

  • Liu XX, Xie SY, Ni TT, Chen DM, Wang X, Pan YH, Wang YL, Huang LL, Cheng GY, Qu W, Liu ZL, Tao YF, Yuan ZH (2017) Magnetic solid-phase extraction based on carbon nanotubes for the determination of polyether antibiotic and s-triazine drug residues in animal food with LC-MS/MS. J Sep Sci 00:1–15

    Google Scholar 

  • Majid R, Lee Yook H, Anuar K, Saeid A, Yadollah A, Hossein J (2012) Immobilization of ionophore and surface characterization studies of the titanium (III) ion in a PVC-membrane sensor. Sensors 12:8806–8814

    Article  CAS  Google Scholar 

  • Maryam A, Yamini Y, Safari M, Asiabi H (2016) Magnetite nanoparticles coated with covalently immobilized ionic liquids as a sorbent for extraction of non-steroidal anti-inflammatory drugs from biological fluids. Microchim Acta 183:2297–2305

    Article  CAS  Google Scholar 

  • Paíga P, Lolić A, Hellebuyck F, Santos LH, Correia M, Delerue-Matos C (2015) Development of a SPE-UHPLC-MS/MS methodology for the determination of non-steroidal anti-inflammatory and analgesic pharmaceuticals in seawater. J Pharm Biomed Anal 106:61–70

    Article  CAS  PubMed  Google Scholar 

  • Peng T, Zhu AL, Zhou YN, Hu T, Yue ZF, Chen DD, Wang GM, Kang G, Fan CL, Chen Y, Jiang HY (2013) Development of a simple method for simultaneous determination of nine subclasses of non-steroidal anti-inflammatory drugs in milk and dairy products by ultra-performance liquid chromatography with tandem mass spectrometry. J Chromatogr B Analyt Technol Biomed Life Sci 933(3):15–23

    Article  CAS  PubMed  Google Scholar 

  • Rago MD, Saar E, Rodda LN, Turfus S, Kotsos A, Gerostamoulos D, Drummer OH (2014) Fast targeted analysis of 132 acidic and neutral drugs and poisons in whole blood using LC–MS/MS. Forensic Sci Int 243:35–43

    Article  CAS  PubMed  Google Scholar 

  • Saeid A, Anuar K, Majid R, Yadollah A, Gholam HR (2011) A conductometric study of complexation reaction between meso-octamethylcalix[4]pyrrole with titanium cation in acetonitrile–ethanol binary mixtures. Int J Electrochem Sci 6:4749–4759

    Google Scholar 

  • Saeid A, Majid R, Anuar K, Majid A (2015a) Cesium selective polymeric membrane sensor based on p-isopropylcalix[6]arene and its application in environmental samples. RSC Adv 5:39209–39217

    Article  CAS  Google Scholar 

  • Saeid A, Majid R, Hassan KM, Yatimah A (2015b) Conductometric measurements of complexation study between 4-isopropylcalix[4]arene and Cr3+ cation in THF–DMSO binary solvents. Measurement 70:214–224

    Article  Google Scholar 

  • Sagristà E, Larsson E, Ezoddin M, Hidalgo M, Salvadó V, Jönsson JA (2010) Determination of non-steroidal anti-inflammatory drugs in sewage sludge by direct hollow fiber supported liquid membrane extraction and liquid chromatography-mass spectrometry. J Chromatogr A 1217(40):6153–6158

    Article  CAS  PubMed  Google Scholar 

  • Shirako J, Kawasaki M, Komine K, Kunisue Y, Terada M, Sasaki C, Irie W, Murakami C, Tonooka K, Tomobe K, Shinozuka T (2013) Simultaneous determination for oxicam non-steroidal anti-inflammatory drugs in human serum by liquid chromatography-tandem mass spectrometry. Forensic Sci Int 227(1–3):100–102

    Article  CAS  PubMed  Google Scholar 

  • Siti MAW, Ibrahim WAW, Sanagi MM, Kamboh MA, Abdul Keyon AS (2018) Magnetic sporopollenin-cyanopropyl triethoxysilane-dispersive micro-solid phase extraction coupled with high performance liquid chromatography for the determination of selected non-steroidal anti-inflammatory drugs in water samples. Chromatogr A 1532:50–57

    Article  CAS  Google Scholar 

  • SN/T (1992–2007) Determination of residues of paracetamol and acetylsalicylic acid in foodstuffs of animal origin for import and export LC–MS/MS method

  • Stoyke M, Bieber C, Monch S, Gowik P (2006) Confirmatory method for the determination of acid NSAIDs in muscle, liver and kidney with LC-MS/MS (Poster). In: Proceedings of 5th International Symposium on Hormone and Veterinary Drug Analysis, Antwerp, Belgium, 16.–19.05.2006

  • Yun L, Huang C, Yang J, Peng J, Jin J, Ma H, Chen J (2017) Multifunctionalized mesoporous silica as an efficient Reversed-phase/anion exchange mixed-mode sorbent for solid-phase extraction of four acidic nonsteroidal anti-inflammatory drugs in environmental water samples. J Chromatogr A 1527:10–17

    Article  CAS  Google Scholar 

  • Zhang H, Du Z, Ji Y, Mei M (2013) Simultaneous trace determination of acidic non-steroidal anti-inflammatory drugs in purified water, tap water, juice, soda and energy drink by hollow fiber-based liquid-phase microextraction and ultra-high pressure liquid chromatography coupled to tandem mass spectrometry. Talanta 109(9):177

    Article  CAS  PubMed  Google Scholar 

  • Zhang H, Peng Z, Yu J, Jie T, Zhenxia D (2015) Photocatalytic degradation of four non-steroidal anti-inflammatory drugs in water under visible light by P25-TiO2 /tetraethyl orthosilicate film and determination via ultra performance liquid chromatograph electrospray tandem mass spectrometry. Chem Eng J 262:1108–1115

    Article  CAS  Google Scholar 

Download references

Funding

This study was financially supported by the National Natural Science Foundation of China (grant number 31602115) and the Ministry of Agriculture the People’s Republic of China (2011BAK10B07-5), which enabled for this work to be carried out.

Author information

Authors and Affiliations

  1. National Reference Laboratory of Veterinary Drug Residues (HZAU) and MAO Key Laboratory for Detection of Veterinary Drug Residues, Wuhan, 430070, Hubei, China

    Yuke Wang, Yahong Ou, Shuyu Xie, Xu Wang, Yuanhu Pan, Lingli Huang, Guyue Cheng, Wei Qu, Yanfei Tao & Zonghui Yuan

  2. Hubei Collaborative Innovation Center for Animal Nutrition and Feed Safety, Huazhong Agricultural University, Wuhan, 430070, Hubei, China

    Shuyu Xie, Dongmei Chen & Zonghui Yuan

  3. MOA Laboratory for Risk Assessment of Quality and Safety of Livestock and Poultry Products, Wuhan, 430070, Hubei, China

    Dongmei Chen, Yulian Wang, Lingli Huang, Zhenli Liu & Yanfei Tao

Authors
  1. Yuke Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Yahong Ou
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Shuyu Xie
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Dongmei Chen
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Xu Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Yuanhu Pan
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Yulian Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Lingli Huang
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. Guyue Cheng
    View author publications

    You can also search for this author in PubMed Google Scholar

  10. Wei Qu
    View author publications

    You can also search for this author in PubMed Google Scholar

  11. Zhenli Liu
    View author publications

    You can also search for this author in PubMed Google Scholar

  12. Yanfei Tao
    View author publications

    You can also search for this author in PubMed Google Scholar

  13. Zonghui Yuan
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Yanfei Tao.

Ethics declarations

Conflict of Interest

The authors declare that there is no conflict of interest.

Ethical Approval

This article does not contain any studies with human participants or animals performed by any of the authors.

Informed Consent

Not applicable.

Additional information

Publisher’s Note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Wang, Y., Ou, Y., Xie, S. et al. Magnetic Graphene Solid-Phase Extraction for the Determination of 47 Kinds of Non-steroidal Anti-inflammatory Drug Residues in Animal Food with Liquid Chromatography Tandem Mass Spectrometry. Food Anal. Methods 12, 1346–1368 (2019). https://doi.org/10.1007/s12161-019-01440-8

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s12161-019-01440-8

Keywords

Search

Navigation