Skip to main content
SpringerLink
Log in

Simultaneous Screening and Determination of Eight Tetracycline Antibiotics Illegally Adulterated in Herbal Preparations Using HPLC–DAD Combined with LC–MS–MS

  • Original
  • Published:
Chromatographia Aims and scope Submit manuscript

Abstract

In this study, the applicability of high-performance liquid chromatography with diode-array detection (HPLC–DAD) combined with electrospray ionization tandem mass spectrometry (ESI–MS) for the simultaneous screening and determination of tetracycline antibiotic analogues illegally adulterated in herbal preparations was investigated. The HPLC–DAD method could be employed to separate and simultaneously determine eight tetracyclines using an isocratic solvent system. These tetracycline antibiotics include doxycycline, 6-epidoxycycline and tetracycline, which are difficult to identify because they are structural isomers. ESI–MS was used in combination with HPLC–DAD to improve the qualitative accuracy in this study. Method validation included the investigation of linearity, selectivity, stability, limits of detection and quantitation, trueness, precision and ruggedness. The response exhibited a good linear relationship with the analyte concentration. The coefficient of determination (r 2) was greater than 0.9993. The limits of quantification for the examined tetracycline antibiotics ranged from 1.11 to 25.73 µg·mL−1, and the recoveries ranged from 91.0 to 104.0%. The proposed methods were specific, sensitive and accurate, and they could be promising and powerful tools for the routine screening of tetracycline analogues in herbal medicines to ensure food safety and public health.

Graphical abstract

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
Fig. 4
Fig. 5

Similar content being viewed by others

Abbreviations

CTC:

Chlortetracycline

DC:

Doxycycline

DEMC:

Demeclocycline

EDTA:

Ethylenediamine tetraacetic acid

ESI-MS:

Electrospray ionization tandem mass spectrometry

6-epi-DC:

6-Epidoxycycline

HPLC–DAD:

High-performance liquid chromatography with diode-array detection

LOD:

Limit of detection

LOQ:

Limit of quantitation

MNC:

Minocycline

MTC:

Methacycline

OTC:

Oxytetracycline

RSD:

The relative standard deviation

RT:

Retention time

TC:

Tetracycline

References

  1. Li SP, Zhao J, Yang B (2011) J Pharm Biomed Anal 55:802–809

    Article  CAS  Google Scholar 

  2. Feng Y, Lei D, Hu C (2014) Spectrochim Acta Part A Mol Biomol Spectrosc 125:363–374

    Article  CAS  Google Scholar 

  3. Guo C, Shi F, Jiang S, Gong L et al (2014) J Chromatogr B Anal Technol Biomed Life Sci 967:174–182

    Article  CAS  Google Scholar 

  4. Liang Q, Qu J, Luo G, Wang Y (2006) J Pharm Biomed Anal 40:305–311

    Article  CAS  Google Scholar 

  5. Yao J, Shi YQ, Li ZR, Jin SH (2007) J Chromatogr B Anal Technol Biomed Life Sci 853:254–259

    Article  CAS  Google Scholar 

  6. Shi F, Guo C, Gong L, Li J et al (2014) J Chromatogr A 1344:91–98

    Article  CAS  Google Scholar 

  7. Liu F, Xie Y, Li Y, Niu C, Ling X (2008) Chin J Pharm Anal 28:1276–1279

    CAS  Google Scholar 

  8. Deconinck E, Cauwenbergh T, Bothy JL, Custers D et al (2014) J Pharm Biomed Anal 100:279–283

    Article  CAS  Google Scholar 

  9. Fejos I, Neumajer G, Beni S, Jankovics P (2014) J Pharm Biomed Anal 98:327–333

    Article  CAS  Google Scholar 

  10. Holzgrabe U, Malet-Martino M (2011) J Pharm Biomed Anal 55:679–687

    Article  CAS  Google Scholar 

  11. Johansson M, Fransson D, Rundlof T, Huynh NH, Arvidsson T (2014) J Pharm Biomed Anal 100:215–229

    Article  CAS  Google Scholar 

  12. Lee ES, Lee JH, Han KM, Kim JW et al (2013) J Pharm Biomed Anal 83:171–178

    Article  CAS  Google Scholar 

  13. Poplawska M, Blazewicz A, Bukowinska K, Fijalek Z (2013) J Pharm Biomed Anal 84:232–243

    Article  CAS  Google Scholar 

  14. Glette J, Sandberg S (1986) Biochem Pharmacol 35:2883–2885

    Article  CAS  Google Scholar 

  15. Douglas AC (1963) Br J Dis Chest 57:44–47

    Article  Google Scholar 

  16. Karageorgou E, Armeni M, Moschou I, Samanidou V (2014) Food Chem 150:328–334

    Article  CAS  Google Scholar 

  17. Cristofani E, Antonini C, Tovo G, Fioroni L et al (2009) Anal Chim Acta 637:40–46

    Article  CAS  Google Scholar 

  18. Tolgyesi A, Tolgyesi L, Bekesi K, Sharma VK, Fekete J (2014) Meat Sci 96:1332–1339

    Article  CAS  Google Scholar 

  19. Shalaby AR, Salama NA, Abou-Raya SH, Emam WH, Mehaya FM (2011) Food Chem 124:1660–1666

    Article  CAS  Google Scholar 

  20. Ben W, Qiang Z, Adams C, Zhang H, Chen L (2008) J Chromatogr A 1202:173–180

    Article  CAS  Google Scholar 

  21. Lillenberg M, Yurchenko S, Kipper K, Herodes K et al (2009) J Chromatogr A 1216:5949–5954

    Article  CAS  Google Scholar 

  22. O’Connor S, Aga DS (2007) Trends Anal Chem 26:456–465

    Article  Google Scholar 

  23. USFDA (2001). http://www.fda.gov/downloads/Drugs/GuidanceComplianceRegulatoryInformation/Guidances/ucm070107.pdf

Download references

Acknowledgements

This work was supported by the Shandong Public Service Platform for new drug safety and pharmacology evaluation, Shandong Provincial Research Fund for Outstanding Young Scholars (BS2015YY037).

Author information

Authors and Affiliations

  1. School of Pharmaceutical Sciences, Shandong University, Jinan, 250012, China

    Fuyan Liu, Peixue Ling, Qixin Chen, Aibin Ma, Mei Li & Fengshan Wang

  2. Shandong Provincial Key Laboratory of Biopharmaceuticals, Shandong Academy of Pharmaceutical Science, Jinan, 250101, China

    Fuyan Liu, Peixue Ling, Qixin Chen, Aibin Ma & Huarong Shao

  3. Shandong Institute for Food and Drug Control, Jinan, 250101, China

    Fuyan Liu, Hui Gao & Xiaoyan Li

  4. School of Life Sciences, Lanzhou University, Lanzhou, 730000, China

    Xiaofeng Zhang

  5. Shandong University of Traditional Chinese Medicine, Jinan, 250355, China

    Yuqiu Li

Authors
  1. Fuyan Liu
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Xiaofeng Zhang
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Yuqiu Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Hui Gao
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Peixue Ling
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Xiaoyan Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Qixin Chen
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Aibin Ma
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. Huarong Shao
    View author publications

    You can also search for this author in PubMed Google Scholar

  10. Mei Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  11. Fengshan Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding authors

Correspondence to Peixue Ling or Fengshan Wang.

Ethics declarations

Conflict of interest

The authors declare that they have no conflicts of interest.

Electronic supplementary material

Below is the link to the electronic supplementary material.

Supplementary material 1 (DOCX 327 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Liu, F., Zhang, X., Li, Y. et al. Simultaneous Screening and Determination of Eight Tetracycline Antibiotics Illegally Adulterated in Herbal Preparations Using HPLC–DAD Combined with LC–MS–MS. Chromatographia 81, 303–314 (2018). https://doi.org/10.1007/s10337-017-3450-8

Download citation

  • Received:

  • Revised:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10337-017-3450-8

Keywords

Search

Navigation