Abstract
A rapid and highly sensitive capillary electrophoresis method was developed combining on-line and off-line sample enrichment techniques that are capable to determine six widely used pharmaceuticals, viz. amoxicillin, carbamazepine, diclofenac, indomethacin, ibuprofen, and paracetamol from various food samples. A new sample preconcentration technique, i.e., in situ aggregated microextraction, was utilized to extract the analytes from various food samples. The process was carried out by the formation of aggregate phase in situ in the aqueous sample by ion association between oppositely charged surfactants, viz. Tiron® and cetyltrimethylammonium bromide. The separation and quantification of analytes were carried out in micellar electrokinetic chromatography mode at −20 kV. In short, the uncoated fused silica capillaries were filled with 80 mM phosphate buffer solution (pH 6.0) to act as leading electrolyte, and the samples were dissolved in 100 mM borate buffer and injected by electrokinetic mode applying −10 kV for 600 s. The method showed good linearity in between 0.06 and 50 μg/L for all six pharmaceuticals. Good repeatability and recoveries were obtained for all analytes in the range of 94.45–106.32% using optimized experimental conditions. The limit of detection ranged from 0.02 to 0.08 μg/L, and the limit of quantification ranged from 0.06 to 0.25 μg/L for six pharmaceuticals. The sensitivity of the developed micellar electrokinetic chromatography method was increased about 2500-folds compared to conventional capillary zone electrophoresis method. Finally, the developed analytical procedure was applied successfully for the detection of selected pharmaceuticals in fruits, urine, and river water samples.
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Amin NC, Blanchin MD, Ake M, Fabre H (2012) Capillary zone electrophoresis as a potential technique for the simultaneous determination of sulfadoxine and pyrimethamine in tablet formulations. J Pharm Biomed Anal 58:168–1671
Aranas AT, Ali A, Anahita N (2011) Sweeping–micellar electrokinetic chromatography for the simultaneous analysis of tricyclic antidepressant and -blocker drugs in wastewater. Talanta 85:86–90
Ashri NY, Rehim MA (2011) Sample treatment based on extraction techniques in biological matrices. Bioanalysis 3:2003–2018
Bhaskar Reddy AV, Yusop Z, Jaafar J, Bin Aris A, Abdul Majid Z, Umar K, Talib J (2016) Simultaneous determination of three organophosphorus pesticides in different food commodities by gas chromatography with mass spectrometry. J Sep Sci 39:2276–2283
Bhaskar Reddy AV, Jaafar J, Aris AB, Majid ZA, Umar K, Talib J, Madhavi G (2015) Development and validation of a rapid ultra-high performance liquid chromatography with tandem mass spectrometry method for the simultaneous determination of darunavir, ritonavir, and tenofovir in human plasma: application to human pharmacokinetics. J Sep Sci 38:2580–2587
Camino SFJ, Rodríguez GR, Zafra GA, Santos FA, Vílchez JL (2014) Stir bar sorptive extraction: recent applications, limitations and future trends. Talanta 130:388–399
Cerqueira MBR, Caldas SS, Primel EG (2014) New sorbent in the dispersive solid phase extraction step of quick, easy, cheap, effective, rugged, and safe for the extraction of organic contaminants in drinking water treatment sludge. J Chromatogr A 1336:10–22
Chevolleau S, Laurent D, Thomas S, Liza V, Issam M, Maria HM, Marina G, Patrick B, Lodovico G (2016) A consolidated method for screening the endocrine activity of drinking water. Food Chem 213:274–283
Endo M, Suzuki K, Abe S (1998) Novel preconcentration technique for trace metal ions by aggregate film formation: spectrophotometric determination of copper (II). Anal Chim Acta 364:13–17
Ferhi S, Marjolaine BD, Jean JD, Sabine H, Sylvie N (2016) Factors influencing the extraction of pharmaceuticals from sewage sludge and soil: an experimental design approach. Anal Bioanal Chem 408:6153–6168
Giróna AM, Antonio LC, Maria JG, Maria LM (2010) Enantiomeric separation of chiral polycyclic musks by capillary electrophoresis: application to the analysis of cosmetic samples. J Chromatogr A 1217:1157–1165
Hamidi S, Abolghasem J (2015) Capillary electrophoresis with UV detection, on-line stacking and off-line dispersive liquid-liquid microextraction for determination of verapamil enantiomers in plasma. Anal Methods 7:5820–5829
Jamali MR, Madadjo A, Rahnama R (2014) Determination of nickel using cold-induced aggregation microextraction based on ionic liquid followed by flame atomic absorption spectrometry. J Anal Chem 69:426–431
Juan LB, Giokas DL, Chisvert A, Salvador A (2015) In-situ suspended aggregate microextraction: a sample preparation approach for the enrichment of organic compounds in aqueous solutions. J Chromatogr A 1408:63–71
Kevin A, Marsh A, Sanger GC (2006) Capillary electrophoresis for the analysis of small-molecule pharmaceuticals. Electrophoresis 27:2263–2282
Khaledi MG, Jenkins SI, Liang L (2013) Perfluorinated alcohols and acids induce coacervation in aqueous solutions of amphiphiles. Langmuir 29:2458–2464
Kim JS, Eun WC, Hai WC, Gyu IK (2006) Effects of Tiron, 4,5-dihydroxy-1,3-benzene disulfonic acid on human promyelotic HL-60 leukemia cell differentiation and death. Toxicology 223:36–45
Lee YT, Breadmore MC, Hong HS (2016) Electrokinetic supercharging in nonaqueous capillary electrophoresis for online preconcentration and determination of tamoxifen and its metabolites in human plasma. J Chromatogr A 461:185–191
Mataa J, Varadea D, Bahadurb P (2005) Aggregation behavior of quaternary salt based cationic surfactants. Thermochim Acta 428:147–155
Merkle S, Kleeberg KK, Fritsche J (2015) Recent developments and applications of solid phase microextraction (SPME) in food and environmental analysis—a review. Chromatography 2:293–381
Mons MN, Heringa MB, Genderen VJ, Puijker LM, Brand W, Leeuwen CJ, Stoks P, Hoek JPV, Kooij DV (2013) Use of the threshold of toxicological concern (TTC) approach for deriving target values for drinking water contaminants. Water Res 47:1666–1678
Murphy EA, Post GB, Buckley BT, Lippincott RL, Robson MG (2012) Future challenges to protecting public health from drinking-water contaminants. Annu Rev Public Health 33:209–224
Nerin C, Salafranca J, Aznar M, Batlle R (2009) Critical review on recent developments in solventless techniques for extraction of analytes. Anal Bioanal Chem 393:809–833
Nicolini C, Anna C, Enrico G, Roland W (2006) Pressure tuning of the morphology of heterogeneous lipid vesicles: a two-photon-excitation fluorescence microscopy study. Biophys J 91:2936–2942
Pakade YB, Tewary DK (2010) Development and applications of single-drop microextraction for pesticide residue analysis: a review. J Sep Sci 33:3683–3691
Pallabi S, Sen K (2014) Cloud point extraction: a sustainable method of elemental preconcentration and speciation. J Indus Eng Chem 20:1209–1219
Pavlovic DM, Sandra B, Alka JMH, Marija KM (2007) Sample preparation in analysis of pharmaceuticals. Tr Anal Chem 26:1062–1075
Reddy Ambavaram VB, Venugopal N, Madhavi V, Gangadhara RK, Madhavi G (2013) Liquid chromatography–tandem mass spectrometry method for simultaneous quantification of urapidil and aripiprazole in human plasma and its application to human pharmacokinetic study. Biomed Chromatogr 27:916–923
Reijenga JC, Verheggen PEMT, Johannes HPAM, Frans ME (1996) Buffer capacity, ionic strength and heat dissipation in capillary electrophoresis. J Chromatogr A 744:147–153
Saraji M, Boroujeni MK (2014) Recent developments in dispersive liquid–liquid microextraction. Anal Bioanal Chem 406:2027–2066
Schulzki G, Nublein B, Sievers H (2017) Transition rates of selected metals determined in various types of teas (Camellia sinensis L. Kuntze) and herbal/fruit infusions. Food Chem 215:22–30
Sharifi V, Abbasi A, Anahita N (2016) Application of hollow fiber liquid phase microextraction and dispersive liquid–liquid microextraction techniques in analytical toxicology. J Food Drug Anal 24:264–276
Siddiqui MR, Al-Othman ZA, Rahman N (2016) Analytical techniques in pharmaceutical analysis: a review. Arab J Chem https://doi.org/10.1016/j.arabjc.2013.04.016
Tatiana GC (2016) In-situ suspended aggregate microextraction of gold nanoparticles from water samples and determination by electrothermal atomic absorption spectrometry. Talanta 151:91–99
Wang M, Wang Y (2014) Development of surfactant co-acervation in aqueous solution. Soft Matter 10:7909–7919
Wainright A (1990) Capillary electrophoresis applied to the analysis of pharmaceutical compounds. J Microcolumn Sep 2:166–175
Wojciech G, Michał JM, Quirino PJ (2016) Different detection and stacking techniques in capillary electrophoresis for metabolomics. Anal Methods 8:1216–1221
Acknowledgements
The postdoctoral fellowship to one of the authors Dr. A. Vijaya Bhaskar Reddy by Universiti Teknologi Malaysia through Research University Grant is highly acknowledged. Further, the authors are thankful to the Ministry of Higher Education Malaysia for providing LRGS Grant on Water Security entitled Protection of Drinking Water: Source Abstraction and Treatment (203/PKT/6720006) and Universiti Teknologi Malaysia (R.J 130000.7809.4L810) as financial support of this project. Additionally, the authors would like to thank UTM GUP J130000.2517.12H03 on ‘Removal of Chemical of Emerging Concern Using in-situ Suspended Aggregate Microextraction from River Water’. Finally, the authors gratefully acknowledged the support of UIRL for providing instrumentation facilities.
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A. Vijaya Bhaskar Reddy declares that he has no conflict of interest. Zulkifli Yusop declares that he has no conflict of interest. Jafariah Jaafar declares that she has no conflict of interest. Nur Hidayati Jamil declares that she has no conflict of interest. Z. A. Majid declares that he has no conflict of interest. Azmi B. Aris declares that he has no conflict of interest.
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Vijaya Bhaskar Reddy, A., Yusop, Z., Jaafar, J. et al. Development and Validation of Capillary Electrophoresis Method for Simultaneous Determination of Six Pharmaceuticals in Different Food Samples Combining On-line and Off-line Sample Enrichment Techniques. Food Anal. Methods 11, 533–545 (2018). https://doi.org/10.1007/s12161-017-1024-x
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DOI: https://doi.org/10.1007/s12161-017-1024-x