Skip to main content

Advertisement

Springer Nature Link
Log in

Liquid Chromatography–Tandem Mass Spectrometry Multiclass Method for 46 Antibiotics Residues in Milk and Meat: Development and Validation

  • Published:
Food Analytical Methods Aims and scope Submit manuscript

Abstract

A screening method for analysis of 46 antibiotics residues, belonging to different classes, such as tetracyclines, sulfonamides, fluoroquinolones, β-lactams, cephalosporins, macrolides and other minority groups was developed and validated for application in bovine milk and bovine, swine, poultry, equine, fish and shrimp meat samples. Sample preparation consists in solvent extraction followed by clean up with C18 bulk and low temperature purification. Instrumental analysis was performed using liquid chromatography coupled to tandem mass spectrometry system. Chromatographic separation was achieved using a C18 column. Mobile phase was composed by methanol and water. The method was validated according to Commission Decision 2002/657/EC criteria. Validation parameters such as specificity and detection capability (CCβ) were determined and considered suitable to the established criteria. Values of CCβ ranged from 1.0 to 50.0 μg L−1 or μg Kg−1, depending on the compound and the matrix. The proposed method has been applied into Brazilian National Residue Control Plan since 2013 for the determination of antibiotic residues. A total of 3833 samples were analyzed until the current date and 13 samples showed positive results with concentrations above the permitted. The method is fast, easy and adequate for high throughput analysis in routine laboratories.

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

Access this article

Log in via an institution

Subscribe and save

Springer+
from $39.99 /Month
  • Starting from 10 chapters or articles per month
  • Access and download chapters and articles from more than 300k books and 2,500 journals
  • Cancel anytime
View plans

Buy Now

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

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2

Similar content being viewed by others

Explore related subjects

Discover the latest articles, books and news in related subjects, suggested using machine learning.

References

  • Arsand JB, Jank L, Martins MT et al (2016) Determination of aminoglycoside residues in milk and muscle based on a simple and fast extraction procedure followed by liquid chromatography coupled to tandem mass spectrometry and time of flight mass spectrometry. Talanta 154:38–45. doi:10.1016/j.talanta.2016.03.045

    Article  CAS  Google Scholar 

  • Berendsen BJA, Stolker LAAM, Nielen MWF, Nielen MWF (2013) Selectivity in the sample preparation for the analysis of drug residues in products of animal origin using LC-MS. TrAC. Trends Anal Chem 43:229–239. doi:10.1016/j.trac.2012.09.019

    Article  CAS  Google Scholar 

  • Bittencourt MS, Martins MT, de Albuquerque FGS et al (2012) High-throughput multiclass screening method for antibiotic residue analysis in meat using liquid chromatography-tandem mass spectrometry: a novel minimum sample preparation procedure. Food Addit Contam Part A 29:508–516. doi:10.1080/19440049.2011.606228

    Article  CAS  Google Scholar 

  • Boscher A, Guignard C, Pellet T et al (2010) Development of a multi-class method for the quantification of veterinary drug residues in feedingstuffs by liquid chromatography-tandem mass spectrometry. J Chromatogr A 1217:6394–6404. doi:10.1016/j.chroma.2010.08.024

    Article  CAS  Google Scholar 

  • Bousova K, Senyuva H, Mittendorf K (2013) Quantitative multi-residue method for determination antibiotics in chicken meat using turbulent flow chromatography coupled to liquid chromatography-tandem mass spectrometry. J Chromatogr A 1274:19–27. doi:10.1016/j.chroma.2012.11.067

    Article  CAS  Google Scholar 

  • Brasil Ministério da Agricultura Pecuária e Abastecimento (2011). Manual de garantia da qualidade analítica

  • Coscollà C, León N, Pastor A, Yusà V (2014) Combined target and post-run target strategy for a comprehensive analysis of pesticides in ambient air using liquid chromatography-Orbitrap high resolution mass spectrometry. J Chromatogr A 1368:132–142. doi:10.1016/j.chroma.2014.09.067

    Article  Google Scholar 

  • Croubels S, Daeseleire E (2012) Veterinary drug residues in foods. In: Chemical Contaminants and Residues in Food. pp 148–182

  • de Queiroz Mauricio A, Lins ES (2012) The National Agricultural Laboratories of Brazil and the control of residues and contaminants in food. Food Addit Contam Part A 29:482–489. doi:10.1080/19440049.2011.620987

    Article  Google Scholar 

  • Díaz-Bao M, Barreiro R, Miranda JM et al (2015) Fast HPLC-MS/MS method for determining penicillin antibiotics in infant formulas using molecularly imprinted solid-phase extraction. J Anal Methods Chem. doi:10.1155/2015/959675

    Google Scholar 

  • European Commission (2010) Commission regulation (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 1–72

  • European Commission (2002) Decision (2002/657/EC) of 12 August 2002 implementing council directive 96/23/EC concerning the performance of analytical methods and interpretation of results. Off. J. Eur. Communities 8–36

  • Granelli K, Branzell C (2007) Rapid multi-residue screening of antibiotics in muscle and kidney by liquid chromatography-electrospray ionization-tandem mass spectrometry. Anal Chim Acta 586:289–295. doi:10.1016/j.aca.2006.12.014

    Article  CAS  Google Scholar 

  • Granelli K, Elgerud C, Lundström A et al (2009) Rapid multi-residue analysis of antibiotics in muscle by liquid chromatography-tandem mass spectrometry. Anal Chim Acta 637:87–91. doi:10.1016/j.aca.2008.08.025

    Article  CAS  Google Scholar 

  • Guo X, Yin D, Peng J, Hu X (2012) Ionic liquid-based single-drop liquid-phase microextraction combined with high-performance liquid chromatography for the determination of sulfonamides in environmental water. J Sep Sci 35:452–458. doi:10.1002/jssc.201100777

    Article  CAS  Google Scholar 

  • Hoff RB, Barreto F, Kist TBL (2009) Use of capillary electrophoresis with laser-induced fluorescence detection to screen and liquid chromatography-tandem mass spectrometry to confirm sulfonamide residues: validation according to European Union 2002/657/EC. J Chromatogr A 1216:8254–8261. doi:10.1016/j.chroma.2009.07.074

    Article  Google Scholar 

  • Hoff RB, Barreto F, Melo J et al (2012) Characterization and estimation of sulfaquinoxaline metabolites in animal tissues using liquid chromatography coupled to tandem mass spectrometry. Anal Methods 4:2822–2830. doi:10.1039/c2ay25197c

    Article  CAS  Google Scholar 

  • Hoff RB, Barreto F, Melo J, et al. (2013) Scope extension validation protocol: inclusion of analytes and matrices in an LC-MS/MS sulfonamide residues method. Food Addit Contam Part A 131106185253008. doi: 10.1080/19440049.2013.861082

  • Im M-H (2013) Review of codex Alimentarius and comparison between the US and Korean food classifications for pesticide residues of the US and Korea. J Korean Soc Appl Biol Chem 56:483–495. doi:10.1007/s13765-013-3182-x

    Article  Google Scholar 

  • Jank L, Hoff RB, Tarouco PC et al (2012) β-lactam antibiotics residues analysis in bovine milk by LC-ESI-MS/MS: a simple and fast liquid–liquid extraction method. Food Addit Contam Part A 29:497–507. doi:10.1080/19440049.2011.604044

    Article  CAS  Google Scholar 

  • Jank L, Martins MT, Arsand JB et al (2015a) High-throughput method for macrolides and lincosamides antibiotics residues analysis in milk and muscle using a simple liquid-liquid extraction technique and liquid chromatography-electrospray-tandem mass spectrometry analysis (LC-MS/MS). Talanta 144:686–695. doi:10.1016/j.talanta.2015.06.078

    Article  CAS  Google Scholar 

  • Jank L, Martins MT, Arsand JB et al (2015b) High-throughput method for the determination of residues of β-lactam antibiotics in bovine milk by LC-MS/MS. Food Addit Contam - Part Chem Anal Control Expo Risk Assess 32:1992–2001. doi:10.1080/19440049.2015.1099745

    CAS  Google Scholar 

  • Johnson D, Boyes B, Orlando R (2013) The use of ammonium formate as a mobile-phase modifier for LC-MS/MS analysis of tryptic digests. J Biomol Tech JBT 24:187–197. doi:10.7171/jbt.13-2404-005

    Article  Google Scholar 

  • Kaufmann A, Butcher P, Maden K (2012) Determination of aminoglycoside residues by liquid chromatography and tandem mass spectrometry in a variety of matrices. Anal Chim Acta 711:46–53. doi:10.1016/j.aca.2011.10.042

    Article  CAS  Google Scholar 

  • Kaufmann A, Walker S (2013) Post-run target screening strategy for ultra high performance liquid chromatography coupled to Orbitrap based veterinary drug residue analysis in animal urine. J Chromatogr A 1292:104–110. doi:10.1016/j.chroma.2012.09.019

    Article  CAS  Google Scholar 

  • Kivrak İ, Kivrak Ş, Harmandar M (2016) Development of a rapid method for the determination of antibiotic residues in honey using UPLC-ESI-MS/MS. Food Sci Technol 36:90–96. doi:10.1590/1678-457X.0037

    Google Scholar 

  • KuKanich B, Gehring R, Webb AI et al (2005) Effect of formulation and route of administration on tissue residues and withdrawal times. J Am Vet Med Assoc 227:1574–1577. doi:10.2460/javma.2005.227.1574

    Article  CAS  Google Scholar 

  • Lara FJ, del Olmo-Iruela M, Cruces-Blanco C et al (2012) Advances in the determination of β-lactam antibiotics by liquid chromatography. TrAC - Trends Anal Chem 38:52–66. doi:10.1016/j.trac.2012.03.020

    Article  CAS  Google Scholar 

  • Le Bizec B (2012) Brazilian Ministry of Agriculture, livestock and food supply (MAPA): strategies to tackle chemical food safety issues. Food Addit Contam Part A 29:481–481. doi:10.1080/19440049.2012.662768

    Article  CAS  Google Scholar 

  • Li N, Feng F, Yang B, et al. (2014) Simultaneous determination of β-lactam antibiotics and β-lactamase inhibitors in bovine milk by ultra performance liquid chromatography-tandem mass spectrometry. J Chromatogr B Analyt Technol Biomed Life Sci 945–946:110–114. doi: 10.1016/j.jchromb.2013.11.044

  • Lins ES, Conceição ES, Mauricio ADQ (2012) Evolution of a residue laboratory network and the management tools for monitoring its performance. Food Addit Contam Part A 29:490–496. doi:10.1080/19440049.2011.653988

    Article  CAS  Google Scholar 

  • Ma S, Chowdhury SK (2013) Data acquisition and data mining techniques for metabolite identification using LC coupled to high-resolution MS. Bioanalysis 5:1285–1297. doi:10.4155/bio.13.103

    Article  CAS  Google Scholar 

  • Martins MT, Barreto F, Hoff RB et al (2015) Determination of quinolones and fluoroquinolones, tetracyclines and sulfonamides in bovine, swine and poultry liver using LC-MS/MS. Food Addit Contam - Part Chem Anal Control Expo Risk Assess 32:333–341. doi:10.1080/19440049.2015.1007091

    CAS  Google Scholar 

  • Martins MT, Barreto F, Hoff RB et al (2016) Multiclass and multi-residue determination of antibiotics in bovine milk by liquid chromatography-tandem mass spectrometry: combining efficiency of milk control and simplicity of routine analysis. Int Dairy J 59:44–51. doi:10.1016/j.idairyj.2016.02.048

    Article  CAS  Google Scholar 

  • Martins MT, Melo J, Barreto F et al (2014) A simple, fast and cheap non-SPE screening method for antibacterial residue analysis in milk and liver using liquid chromatography-tandem mass spectrometry. Talanta 129:374–383. doi:10.1016/j.talanta.2014.04.049

    Article  CAS  Google Scholar 

  • Mauricio ADQ, Lins ES, Alvarenga MB (2009) A National Residue Control Plan from the analytical perspective-the Brazilian case. Anal Chim Acta 637:333–336. doi:10.1016/j.aca.2008.09.061

    Article  CAS  Google Scholar 

  • Nonaka CKY, Oliveira AMG, Paiva CR et al (2012) Occurrence of antimicrobial residues in Brazilian food animals in 2008 and 2009. Food Addit Contam Part A 29:526–534. doi:10.1080/19440049.2011.625649

    Article  CAS  Google Scholar 

  • Prestes OD, Martins ML, Do A, Friggi C et al (2013) The state of the art in determination of veterinary drug residues in foods of animal origin using chromatographic techniques coupled to mass spectrometry. Quim Nov. 36:697–710. doi:10.1590/S0100-40422013000500015

  • Woodward K (2004) The evolution of safety assessments for veterinary medicinal products the European Union. Vet Hum Toxicol 46:199–205

    CAS  Google Scholar 

Download references

Acknowledgments

The authors would like to thank the CAPES for the fellowships provided for Juliana Bazzan Arsand, and to National Council for Scientific and Technological Development (CNPq) for the fellowship provided to Magda Targa Martins, Tanara Magalhães Campos Motta and Tiago Corrêa Feijó.

Author information

Authors and Affiliations

  1. Instituto de Química, Universidade Federal do Rio Grande do Sul – UFRGS, Av. Bento Gonçalves 9500, Porto Alegre, RS, ZIP91501-970, Brazil

    Louise Jank, Juliana Bazzan Arsand, Tanara Magalhães Campos Motta & Tânia Mara Pizzolato

  2. Laboratório Nacional Agropecuário – LANAGRO/RS, Ministério da Agricultura, Pecuária e Abastecimento do Brasil, Estrada da Ponta Grossa 3036, Porto Alegre, RS, ZIP91780-580, Brazil

    Louise Jank, Magda Targa Martins, Juliana Bazzan Arsand, Tanara Magalhães Campos Motta, Tiago Corrêa Feijó, Tamara dos Santos Castilhos, Rodrigo Barcellos Hoff & Fabiano Barreto

Authors
  1. Louise Jank
    View author publications

    Search author on:PubMed Google Scholar

  2. Magda Targa Martins
    View author publications

    Search author on:PubMed Google Scholar

  3. Juliana Bazzan Arsand
    View author publications

    Search author on:PubMed Google Scholar

  4. Tanara Magalhães Campos Motta
    View author publications

    Search author on:PubMed Google Scholar

  5. Tiago Corrêa Feijó
    View author publications

    Search author on:PubMed Google Scholar

  6. Tamara dos Santos Castilhos
    View author publications

    Search author on:PubMed Google Scholar

  7. Rodrigo Barcellos Hoff
    View author publications

    Search author on:PubMed Google Scholar

  8. Fabiano Barreto
    View author publications

    Search author on:PubMed Google Scholar

  9. Tânia Mara Pizzolato
    View author publications

    Search author on:PubMed Google Scholar

Corresponding author

Correspondence to Louise Jank.

Ethics declarations

Conflict of Interest

Louise Jank declares that they have no conflict of interest. Juliana Bazzan Arsand that they have no conflict of interest. Tanara Magalhães Campos Motta that they have no conflict of interest. Tiago Corrêa Feijó that they have no conflict of interest. Tamara dos Santos Castilhos that they have no conflict of interest. Rodrigo Barcellos Hoff that they have no conflict of interest. Fabiano Barreto that they have no conflict of interest. Tânia Mara Pizzolato that they have 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.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Jank, L., Martins, M.T., Arsand, J.B. et al. Liquid Chromatography–Tandem Mass Spectrometry Multiclass Method for 46 Antibiotics Residues in Milk and Meat: Development and Validation. Food Anal. Methods 10, 2152–2164 (2017). https://doi.org/10.1007/s12161-016-0755-4

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s12161-016-0755-4

Keywords