Liquid chromatography – tandem mass spectrometry method for the determination of ten tetracycline residues in muscle samples

Open access

Abstract

A liquid chromatography – tandem mass spectrometry (LC-MS/MS) method for the determination of oxytetracycline (OTC), 4-epi oxytetracycline (4-epi OTC), tetracycline (TC), 4-epi tetracycline (4-epi TC), chlortetracycline (CTC), 4-epi chlortetracycline (4-epi CTC), doxycycline (DC), minocycline (MINO), methacycline (META) and rolitetracycline (ROLI) residues in muscles was developed. The procedure consisted of an oxalic acid extraction followed by protein removal with trichloroacetic acid. Further solid phase clean-up on polymeric (Strata X) reversed phase columns was performed to obtain an extract suitable for LC-MS/MS analysis. The tetracyclines were separated on a C 18 analytical column with mobile phase consisting of 0.01% formic acid in acetonitrile and 0.01% formic acid in water in gradient mode. The method was validated according to the Commission Decision 2002/657/EC. The recoveries of all target compounds were 91.8% – 103.6%. The decision limits were from 109.0 to 119.8 μg/kg and detection capability varied within the range of 122.2 to 137.6 μg/kg, depending on the analyte.

1. Anderson C.R., Rupp H.S., Wu W-H.: Complexities in tetracycline analysis – chemistry, matrix extraction, cleanup and liquid chromatography. J Chromatogr A 2005, 1075, 23–32.

2. Biswas A.K., Rao G.S., Kondaiah N., Anjaneyulu A.S.R., Mendiratta S.K., Prasad R., Malik J.K.: A simple multi-residue method for determination of oxytetracycline, tetracycline and chlorotetracycline in export buffalo meat by HPLC-Photodiode Array Detector. J Food Drug Anal 2007, 15, 278–284.

3. Blasco C., Di Corcia A., Pico Y.: Determination of tetracyclines in multi-specie animal tissues by pressurized liquid extraction and liquid chromatography – tandem mass spectrometry. Food Chem 2009, 116, 1005–1012.

4. Bogialli S., Curini R., Di Corcia A., Lagana A., Rizzuti G.: A rapid confirmatory method for analyzing tetracycline antibiotics in bovine, swine and poultry muscle tissues: matrix solid-phase dispersion with heated water as extractant followed by liquid chromatography-tandem mass spectrometry. J Agr Food Chem 2006, 54, 1564–1570.

5. Brandsteterova E., Kubalec P., Bovanova L., Simko P., Bednarikowa A., Machackova L.: SPE and MSPD as pre-separation techniques for HPLC of tetracyclines in meat, milk and cheese. Lebensm Unters Forsch A 1997, 205, 311–315.

6. Carrasco-Pancorbo A., Casado-Terrones S., Segura-Carretero A., Fernandez-Gutierrez A.: Reversed-phase high performance liquid chromatography coupled to ultraviolet and electrospray time-of-flight mass spectrometry on-line detection for the separation of eight tetracyclines in honey samples. J Chromatogr A 2008, 1195, 107–116.

7. Castellari M., Garcia-Regueiro J.A.: HPLC determination of tetracyclines in lamb muscle using an RP-C18 monolithic type column. Chromatographia 2003, 58, 789–792.

8. Cherlet M., Schelkens M., Croubels S., De Backer P.: Quantitative multi-residue analysis of tetracyclines and their 4-epimers in pig tissues by high-performance liquid chromatography combined with positive-ion electrospray ionization mass spectrometry. Anal Chim Acta 2003, 492, 199–213.

9. Cinquina A.L., Longo F., Anastasi G., Giannetti L., Cozzania R.: Validation of a high – performance liquid chromatography method for the determination of oxytetracycline, tetracycline, chlortetracycline and doxycycline in bovine milk and muscle. J Chromatogr A 2003, 987, 227–233.

10. Commission Decision 2002/657/EC of 12 August 2002 implementing Council Directive 96/23/EC concerning the performance of analytical methods and the interpretation of results. OJ 2002, L 221, pp. 8–36

11. 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 Commun 2010, L15, 1–72.

12. Cooper A.D., Stubbings G.W.F., Kelly M., Tarbin J.A., Farrington W.H.H., Shearer G.: Improved method for the on-line metal chelate affinity chromatography – high performance liquid chromatographic determination of tetracycline antibiotics in animal products. J. Chromatogr A 1998, 812, 321–326.

13. Cooper A.D., Tarbin J.A., Farrington W.H.H., Shearer G.: Effect of extraction and spiking procedures on the determination of incurred residues of oxytetracycline in cattle kidney. Food Addit Contam 1998, 15, 645–650.

14. Croubels S.M., Vanoosthuyze K.EI., Van Pethegem C.H.: Use of metal chelate affinity chromatography and membrane-based ion-exchange as clean-up procedure for trace analysis of tetracyclines in animal tissues and egg. J Chromatogr B 1997, 690, 173–179.

15. Ding X., Mou S.: Ion chromatographic analysis of tetracyclines using polymeric column and acidic eluent. J Chromatogr A 2000, 897, 205–214.

16. Gajda A., Posyniak A, Tomczyk G.: LC-MS/MS analysis of doxycycline residues in chicken tissues after oral administartion. Bull Vet Inst Pulawy, 2014, 58, 573–579.

17. Gajda A., Posyniak A., Żmudzki J., Tomczyk G.: Determination of doxycycline in chicken fat by liquid chromatography with UV detection and liquid chromatography - tandem mass spectrometry. J Chromatogr B – Analytical Technologies in the Biomedical and Life Sciences. 2013, 928, 113–120

18. Haagsma N., Scherpenisse P.: High-performance liquid chromatographic determination of tetracyclines in animal tissue and eggs. Euroresidue II, Veldhoven, the Netherlands, 1993.

19. Kamel A.M., Fouda H.G., Brown P.R., MunsonB.: Mass spectral characterization of tetracyclines by electrospray ionization, H/D/ exchange, and multiple stage mass spectroametry. J Am Soc Mass Spectrom 2002, 13, 543–557.

20. Liang Y., Denton M.B., Bates R.B.: Stability studies of tetracycline in methanol solution. J Chromatogr A 1998, 827, 45–55.

21. Majors R.E., Carr P.W.: Glossary of liquid-phase separation terms. LC – GC N Am 2001, 2, 124–162.

22. McCracken R.J., Blanchflower W.J., Haggan S.A., Kennedy D.G.: Simultaneous determination of oxytetracycline, tetracycline and chlortetracycline in animal tissues using liquid chromatography, post-column derivatisation with alumninium and fluorescence detection. Analyst 1995, 120, 1763–1766.

23. Mulders E.J., Van De Lagemaat D.: Determination of residues of tetracycline antibiotics in animal tissues by high-performance liquid chromatography. J Pharm Biomed Anal 1989, 7, 1829–1835.

24. Nakazawa H., Ino S., Kato K., Watanabe T., Ito Y., Oka H.: Simultaneous determination of residual tetracyclines in foods by high-performance liquid chromatography with atmospheric pressure chemical ionization tandem mass spectrometry. J Chromatogr B 1999, 732, 55–64.

25. Oka H., Ikai Y., Ito Y., Hayakawa J., Harada K., Suzuki M., Odani H., Maeda K.: Improvement of chemical analysis of antibiotics XXIII. Identification of residual tetracyclines in bovine tissues by electrospray high-performance liquid chromatography – tandem mass spectrometry. J Chromatogr B 1997, 693, 337–344.

26. Oka H., Ito Y., Ikai Y., Kagami T., Harada K.: Mass spectrometric analysis of tetracycline antibiotics in food. J Chromatogr A 1998, 812, 309–319.

27. Oka H., Ito Y., Matsumoto H.: Chromatographic analysis of tetracycline antibiotics in foods. J Chromatogr A 2000, 882, 109–133.

28. Pena A.L.S., Lino C.M., Silveira I.M.: Determination of tetracycline antibiotics in salmon muscle by liquid chromatography using post-column derivatization with fluorescence detection. J AOAC Int 2003, 86, 925–929.

29. Posyniak A., Żmudzki J., Semeniuk S., Niedzielska J., Ellis R.: Determination of tetracycline residues in animal tissues by liquid chromatography. Biomed Chromatogr 1998, 12, 294–299.

30. Shalaby A.R., Salama N.A., Abou-Raya S.H., Emam W.H., Mehaya F.M.: Validation of HPLC method for determination of tetracycline residues in chicken meat and liver. Food Chem 2011, 124, 1660–1666.

31. Wen Y., Wang Y., Feng Y-Qi.: Simultaneous residue monitoring of four tetracycline antibiotics in fish muscle by in-tube solid-phase microextraction coupled with high-performance liquid chromatography. Talanta 2006, 70, 153–159.

32. Yu H., Tao Y., Chen D., Wang Y., Yuan Z.: Development of an HPLC – UV method for the simultaneous determination of tetracyclines in muscle and liver of porcine, chicken and bovine with accelerated solvent extraction. Food Chem. 2011, 124, 1131–1138.

Bulletin of the Veterinary Institute in Pulawy

The Journal of National Veterinary Research Institute in Pulawy

Journal Information


IMPACT FACTOR 2017: 0.811
5-year IMPACT FACTOR: 0.973

CiteScore 2017: 0.68


SCImago Journal Rank (SJR) 2017: 0.287
Source Normalized Impact per Paper (SNIP) 2017: 0.484

Cited By

Metrics

All Time Past Year Past 30 Days
Abstract Views 0 0 0
Full Text Views 128 128 10
PDF Downloads 48 48 6