Dispersive liquid-liquid microextraction/HPLC techniques for determination of oxytetracycline and doxycycline residues in beef samples: method developments and statistical analysis

Muinat Aliu; Abibat Junaid; Abdulrahman Ibraheem; Aisha Ishaq; Abubakar Lawal; Kikelomo Ayeni`; Amudalat Lawal; Lukman Abdulra'uf

doi:10.46481/asr.2023.2.1.87

Authors

M. A. Aliu
Department of Chemistry and Industrial Chemistry, Faculty of Pure and Applied Sciences, Kwara State University, Malete, P.M.B 1530, Ilorin, Nigeria.
A. M. Junaid
Department of Chemistry and Industrial Chemistry, Faculty of Pure and Applied Sciences, Kwara State University, Malete, P.M.B 1530, Ilorin, Nigeria.
A. Ibraheem
Department of Chemistry and Industrial Chemistry, Faculty of Pure and Applied Sciences, Kwara State University, Malete, P.M.B 1530, Ilorin, Nigeria
A. Ishaq
Department of Chemistry and Industrial Chemistry, Faculty of Pure and Applied Sciences, Kwara State University, Malete, P.M.B 1530, Ilorin, Nigeria
A. Lawal
Department of Pure and Industrial Chemistry, Umaru Musa Yar’adua University Katsina, Nigeria
K. E. Ayeni
Department of Chemistry and Industrial Chemistry, Faculty of Pure and Applied Sciences, Kwara State University, Malete, P.M.B 1530, Ilorin, Nigeria
A. R. Lawal
Department of Biology, School of Sciences, Kwara State College of Education, Ilorin, Nigeria
L. B. Abdulrauf
[email protected]

Department of Chemistry and Industrial Chemistry, Faculty of Pure and Applied Sciences, Kwara State University, Malete, P.M.B 1530, Ilorin, Nigeria.

Keywords:

beef, liquid chromatography, microextraction, tetracyclines, validation`

Abstract

A rapid, cost-effective and environment-friendly sample pre-treatment method involving dispersive liquid-liquid microextraction (DLLME) and high-performance liquid chromatography (HPLC) was developed and applied for the extraction of oxytetracycline and doxycycline residues in beef samples (liver, kidney and muscle). Several influencing factors associated with the extraction and separation of these antibiotics residues, such as sample size, type and volume of disperser and extraction solvents, centrifugation speed and time, were optimized using Plackett-Burman design and central composite design, while insignificant factors were fixed at values determined using univariate analysis. Figures of merit of the analytical methodology including the limit of detection (LOD), the limit of quantification (LOQ), accuracy (in terms of average recoveries), precision and calibration functions were established according to the European Union commission decision 2002/657/EC. Linearity, in the range of 5–500 µg/kg, was obtained with regression coefficients ranging from 0.9983 – 0.9999. Inter-day repeatability, intra-day precision, LODs and LOQs obtained were 3.81 – 14.90%, 3.80 – 8.70%, 4.21 – 4.69 µg/kg and 14.02 – 15.65 µg/kg respectively. Samples with detectable drug residues have oxytetracycline being the most commonly detected. The developed method was successfully established and the concentration levels of drug residues detected were lower than the European Union set maximum residue level (MRL).

Dimensions

REFERENCES

M. R. Prashanthy, S. Shreelakshmi, D. Prabu, M. Rajmohan, V. V. Bharathwaj, R. Sindhu, D. Dinesh, P. Suganya, “A comparative analysis of cost and affordability between veterinary and human pharmaceutical drugs in India”, International Journal of Science and Healthcare Research 6 (2021) 170.

T. Beyene, “Veterinary Drug Residues in Food-animal Products: Its risk factors and potential effects on public health”, Journal of Veterinary Science & Technology 7 (2016) 1.

B. Er, F. Kaynak, B. Demirhan, & S. Ö. Özgacar, “Screening of quinolone antibiotic residues in chicken meat and beef sold in the markets of Ankara, Turkey”, Poultry Science 92 (2013) 2212.

V. Goetting, K. A. Lee, & L. A. Tell, “Pharmacokinetics of veterinary drugs in laying hens and residues in eggs: A review of the literature”, Journal of Veterinary Pharmacology and Therapeutics 34 (2011) 521.

N. Kemper, “Veterinary antibiotics in the aquatic and terrestrial environment”, Ecological Indicator 8 (2008) 1.

A. B. Saba, L. O. Olatoye, & O. A. Oridupa, “Spectrophotometric analysis of oxytetracycline brands available over-the-counter for veterinary use in South western Nigerian”, Nigerian Veterinary Journal 33 (2011) 533.

A. Ogwuche, A. B. Ekiri, I. Endacott, B. V. Maikai, E. S. Idoga, R. Alafiatayo, & A. J. C. Cook, “Antibiotic use practices of veterinarians and para-veterinarians and the implications for antibiotic stewardship in Nigeria”, Journal of the South African Veterinary Association 92 (2021) 1.

M. O. Emeje, S. Olye, M. Bubakari, & M. Adeyeye, “Use of antibiotics in livestock in Nigeria: curbing antimicrobial resistance and developing a national regulatory Guideline towards monitoring antibiotic use in animal and animal foods”, International Research Journal of Public and Environmental Health 9 (2022) 55.

T. Ma, L. Zhou, L. Chen, Z. Li, L. Wu, P. Christie, & Y. Luo, “Oxytetracycline toxicity and its effect on phytoremediation by Sedum plumbizincicola and Medicago sativa in metal contaminated soil”, Journal of Agricultural and Food Chemistry 64 (2016) 8045.

A. S. Lorenzetti, C. E. Domini, & A. G. Lista, “A simple and new reverse liquid–liquid microextraction for the automated spectrometric determination of doxycycline in chicken fat”, Food Chemistry 237 (2017) 506.

A. Kazek, A. Nosol, P. Joanna, S. Monika, S. Student, S., & M. Brzychczyw, Physico-chemical and biological evaluation of doxycycline loaded into hybrid oxide-polymer layer on Ti–Mo alloy”, Bioactive Materials 5 (2017) 553.

H. Sereshti, G. Abdolhosseini, S. Soltani, F. Jamshidi, & N. Nouri, “Natural thymol-based ternary deep eutectic solvents: application in air-bubbles assisted-dispersive liquid liquid microextraction for analysis of tetracyclines in water”, Journal of Separation Science 44 (2021) 3626.

G. Lai, G. Chen, T. Chen, & Q. Li, “Rapid screening of oxytetracycline residue in fish muscle by dispersive liquid-liquid microextraction and europium-sensitized luminescence”, Food Analytical Methods 8 (2015) 2052.

Y. Fang, W. Tian, F. Pei, P. Li, X. Shao, Y. Fan, &,Q. Hu, “Simultaneous determination of pesticide residues and antioxidants in blended oil using a liquid-liquid extraction combined with dispersive solid phase extraction method”, Food Chemistry 229 (2017) 347.

C. Stalikas, Y. Fiamegos, V. Sakkas, & T. Albanis, “Developments on chemometric approaches to optimize and evaluate microextraction”, Journal of Chromatography A 1216 (2009) 175.

L. B. Abdulra’uf, A. Y. Sirhan, & G. H. Tan, “Applications of experimental design to the optimization of microextraction sample preparation parameters for the Analysis of pesticides residues in fruits and vegetables”, Journal of AOAC International 98 (2015) 1171.

ICH-Topic Q2(R2) “Validation of analytical procedures: text and methodology”, International Council for Harmonisation of Technical Re- quirements for Pharmaceuticals for Human Use, ICH Harmonised Tripartite Guideline. U. S Department of Health and Human Services

B. J. Winer, Statistical Principles in Experimental Design (3rd ed.). New York: McGraw-Hill, 1991.

A. Lawal, R. C. S. Wong, G. H. Tan, L. B. Abdulra’uf, & A. M. A. Alsharif, “Multi-pesticides determination in samples of fruits and vegetables using chemometrics approach to QuEChERS – dSPE coupled with ionic liquid –based DLLME and LC-MS/MS”, Chromatographia 81 (2018) 759.

G. A. M. Curbelo, M. Asensio–Ramos, V. A. Herrera–Herrere, & J. Harnardez-Borges “Pesticide residue analysis in cereal based baby foods using multi – walled carbon nanotubes dispersive solid–phase extraction”, Analytical Bioanalytical Chemistry 404 (2012) 83.

European Commission. 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, as amended by Decision 2003/181/EC (4). Official Journal of the European Communities 8 (2002) 36.

S. O. S. Mookantsa, S. Dube, & M. M. Nindi, “Development and application of a dispersive liquid – liquid microextraction method for the determination of tetracyclines in beef by liquid chromatography mass spectrometry”, Talanta 148 (2016) 321.

D. Moema, M. M. Nindi, & S. Dube, “Development of a dispersive liquid-liquid microextraction method for the determination of fluoro-quinolones in chicken liver by high performance liquid chromatography”, Analytica Chimica Acta 730 (2012) 80.

SANCO, “Method validation and quality control procedures for pesticide residues analysis in food and feed”, SANCO/12571/2013 Brussel: European Commission, Directorate of General Health and Consumer Protection.

A. Lawal, & L. B. Abdulra’uf, “Chemometrics approach to QuEChERS-dSPE for multi standard determination of pesticides in blank samples of Milli-Q-Water using high performance liquid chromatography-tandem mass spectrometry (LC-MS/MS)”, Chemsearch 11 (2020) 66.