Food Analytical Methods

, Volume 12, Issue 2, pp 381–393 | Cite as

Rapid and Sensitive Detection of Multi-Class Food Additives in Beverages for Quality Control by Using HPLC-DAD and Chemometrics Methods

  • Xiao-Dong Sun
  • Hai-Long WuEmail author
  • Zhi Liu
  • Yue Chen
  • Qian Liu
  • Yu-Jie Ding
  • Ru-Qin Yu


A rapid and sensitive analytical strategy combining high-performance liquid chromatography-diode array detection (HPLC-DAD) and chemometrics methods was developed for the determination of multi-class food additives in a variety of beverage samples. Different kinds of beverages, which contain diverse unknown interferences, can be directly injected into a chromatographic system after a simple dilution or pretreatment step, and the data were recorded in a short time under a simple gradient elution mode. Although peaks overlapped and changeable interferences existed in the dimension of the chromatographic and spectral in real beverages, all food additives were accurately resolved by using a second-order calibration method based on alternating trilinear decomposition (ATLD) algorithm, and accurate chromatographic profiles, spectral profiles, and concentration profiles were also obtained. Limits of detection for all additives were between 1.40 and 165.1 ng mL−1, while limits of quantitation ranged from 4.20 to 500.2 ng mL−1. The spiked recoveries were in the range of 87.3–103% (except amaranth) with RSDs less than 10.2%. Compared with the results obtained by classic HPLC method, our proposed method was more accurate. In all, the proposed method is fast, sensitive, and universal and could be used as a reliable tool to determine food additives and quality monitoring in different complex beverages.


Alternating trilinear decomposition Beverages Food additives High-performance liquid chromatography-diode array detection Second-order calibration 



Acesulfame potassium




Glycyrrhizic acid


Benzoic acid


Sorbic acid








Sunset yellow


Brilliant blue




China Food and Drug Administration


Alternating trilinear decomposition






Limit of detection


Limit of quantitation



This work was supported by the National Nature Science Foundation of China (Grant No. 21575039 and No. 21775039) and the Foundation for Innovative Research Groups of NSFC (Grant No. 21521063).

Compliance with Ethical Standards

Conflicts of Interest

Xiaodong Sun declares that he has no conflict of interest. Hailong Wu declares that he has no conflict of interest. Zhi Liu declares that he has no conflict of interest. Yue Chen declares that she has no conflict of interest. Qian Liu declares that she has no conflict of interest. Yujie Ding declares that she has no conflict of interest. Ruqin Yu declares that he has no conflict of interest.

Ethical Approval

This article does not contain any studies with animals performed by any of the authors.

Informed Consent

Not applicable.

Supplementary material

12161_2018_1370_MOESM1_ESM.docx (353 kb)
ESM 1 (DOCX 351 kb)


  1. Alothman ZA, Aqel A, Mke A, Yacine BA, Alwarthan AA (2012) Fast chromatographic determination of caffeine in food using a capillary hexyl methacrylate monolithic column. Food Chem 132:2217–2223CrossRefGoogle Scholar
  2. Amigo JM, Skov T, Bro R (2010) ChroMATHography: solving chromatographic issues with mathematical models and intuitive graphics. Chem Rev 110:4582–4605CrossRefPubMedGoogle Scholar
  3. Bazzucchi I, Felici F, Montini M, Figura F, Sacchetti M (2011) Caffeine improves neuromuscular function during maximal dynamic exercise. Muscle Nerve 43:839–844CrossRefPubMedGoogle Scholar
  4. Belguidoum K, Amira-Guebailia H, Boulmokh Y, Houache O (2014) HPLC coupled to UV–vis detection for quantitative determination of phenolic compounds and caffeine in different brands of coffee in the Algerian market. J Taiwan Inst Chem Eng 45:1314–1320CrossRefGoogle Scholar
  5. Bergamo AB, Da Silva JAF, De Jesus DP (2011) Simultaneous determination of aspartame, cyclamate, saccharin and acesulfame-K in soft drinks and tabletop sweetener formulations by capillary electrophoresis with capacitively coupled contactless conductivity detection. Food Chem 124:1714–1717CrossRefGoogle Scholar
  6. Berger TA, Berger BK (2013) Rapid, direct quantitation of the preservatives benzoic and Sorbic acid (and salts) plus caffeine in foods and aqueous beverages using supercritical fluid chromatography. Chromatographia 76:393–399CrossRefGoogle Scholar
  7. Boeris V, Arancibia JA, Olivieri AC (2014) Determination of five pesticides in juice, fruit and vegetable samples by means of liquid chromatography combined with multivariate curve resolution. Anal Chim Acta 814:23–30CrossRefPubMedGoogle Scholar
  8. Bonan S, Fedrizzi G, Menotta S, Elisabetta C (2013) Simultaneous determination of synthetic dyes in foodstuffs andbeverages by high-performance liquid chromatography coupledwith diode-array detector. Dyes & Pigments 99:36–40CrossRefGoogle Scholar
  9. Bro R, Andersson CA, Kiers HA (1999) PARAFAC2-part II. Modeling chromatographic data with retention time shifts. J Chemom 13:295–309CrossRefGoogle Scholar
  10. Bro R, Kiers HAL (2003) A new efficient method for determining the number of components in PARAFAC models. J Chemom 17:274–286CrossRefGoogle Scholar
  11. Chen Z-P, Liu Z, Cao Y-Z, Yu R-Q (2001) Efficient way to estimate the optimum number of factors for trilinear decomposition. Anal Chim Acta 444:295–307CrossRefGoogle Scholar
  12. Demiralay EC, Özkan G, Guzel-Seydim Z (2006) Isocratic separation of some food additives by reversed phase liquid chromatography. Chromatographia 63:91–96CrossRefGoogle Scholar
  13. Feng F, Yang S, Ling Y, Jiang GB, Chu XG (2011) Simultaneous screening of 14 illegal food additives in wines using ultra performance liquid chromatography tandem mass spectrometry. Chin J Anal Chem 39:1732–1737Google Scholar
  14. Fernandes VNO, Fernandes LB, Vasconcellos JP, Jager AV, Tonin FG, de Oliveira MAL (2013) Simultaneous analysis of aspartame, cyclamate, saccharin and acesulfame-K by CZE under UV detection. Anal Methods 5:1524–1532CrossRefGoogle Scholar
  15. Fjm M, Implvo F, Cunha SC, Mbpp O (2003) Optimisation of extraction procedures for analysis of benzoic and sorbic acids in foodstuffs. Food Chem 82:469–473CrossRefGoogle Scholar
  16. Gao H, Yang M, Wang M, Zhao Y, Cao Y, Chu X (2013) Determination of 30 synthetic food additives in soft drinks by HPLC/electrospray ionization-tandem mass spectrometry. J AOAC Int 96:110–115CrossRefPubMedGoogle Scholar
  17. Gemperline P (2006) Practical guide to chemometrics. CRC pressGoogle Scholar
  18. Kamankesh M, Mohammadi A, Tehrani ZM, Ferdowsi R, Hosseini H (2013) Dispersive liquid–liquid microextraction followed by high-performance liquid chromatography for determination of benzoate and sorbate in yogurt drinks and method optimization by central composite design. Talanta 109:46–51CrossRefGoogle Scholar
  19. Kiers HA, Ten Berge JM, Bro R (1999) PARAFAC2-part I. a direct fitting algorithm for the PARAFAC2 model. J Chemom 13:275–294CrossRefGoogle Scholar
  20. Lee Y, Do B, Lee G, Lim HS, Yun SS, Kwon H (2017) Simultaneous determination of sodium saccharin, aspartame, acesulfame-K and sucralose in food consumed in Korea using high-performance liquid chromatography and evaporative light-scattering detection. Food Addit Contam: Part A 34:666–677CrossRefGoogle Scholar
  21. Ling DS, Xie HY, He YZ, Gan WE, Yong G (2010) Determination of preservatives by integrative coupling method of headspace liquid-phase microextraction and capillary zone electrophoresis. J Chromatogr A 1217:7807–7811CrossRefPubMedGoogle Scholar
  22. Liu Z, Cai W, Shao X (2009) High-throughput approach for analysis of multicomponent gas chromatographic–mass spectrometric signals. J Chromatogr A 1216:1469–1475CrossRefPubMedGoogle Scholar
  23. Liu Z, Wu HL, Xie LX, Hu Y, Fang H, Sun XD, Wang T, Xiao R, Yu RQ (2017) Direct and interference-free determination of thirteen phenolic compounds in red wines using a chemometrics-assisted HPLC-DAD strategy for authentication of vintage year. Anal Methods 9:3361–3374CrossRefGoogle Scholar
  24. Ma J, Zhang B, Wang Y, Hou X (2014) Comparison of six sample preparation methods for analysis of food additives in milk powder. Food Anal Methods 7:1345–1352CrossRefGoogle Scholar
  25. Ma K, Li XJ, Wang HF, Zhao M (2015) Rapid and sensitive method for the determination of eight food additives in red wine by ultra-performance liquid chromatography tandem mass spectrometry. Food Anal Methods 8:203–212CrossRefGoogle Scholar
  26. Ma K, Yang YN, Jiang XX, Zhao M, Cai YQ (2012) Simultaneous determination of 20 food additives by high performance liquid chromatography with photo-diode array detector. Chin Chem Lett 23:492–495CrossRefGoogle Scholar
  27. McCann D, Barrett A, Cooper A, Crumpler D, Dalen L, Grimshaw K, Kitchin E, Lok K, Porteous L, Prince E, Sonuga-Barke E, Warner JO, Stevenson J (2007) Food additives and hyperactive behaviour in 3-year-old and 8/9-year-old children in the community: a randomised, double-blinded, placebo-controlled trial. Lancet 370:1560–1567CrossRefPubMedGoogle Scholar
  28. Meinhart AD, Bizzotto CS, Ballus CA, Prado MA, Bruns RE, Filho JT, Godoy HT (2010) Optimisation of a CE method for caffeine analysis in decaffeinated coffee. Food Chem 120:1155–1161CrossRefGoogle Scholar
  29. Olivieri AC (2012) Recent advances in analytical calibration with multi-way data. Anal Methods 4:1876–1886CrossRefGoogle Scholar
  30. Olivieri AC (2014) Analytical figures of merit: from univariate to multiway calibration. Chem Rev 114:5358–5378CrossRefPubMedGoogle Scholar
  31. Olivieri AC, Faber NM (2005) A closed-form expression for computing the sensitivity in second-order bilinear calibration. J Chemom 19:583–592CrossRefGoogle Scholar
  32. Pérez RL, Escandar GM (2015) Multivariate calibration-assisted high-performance liquid chromatography with dual UV and fluorimetric detection for the analysis of natural and synthetic sex hormones in environmental waters and sediments. Environ Pollut 209:114CrossRefPubMedGoogle Scholar
  33. Prado MA, Boas LFV, Bronze MR, Godoy HT (2006) Validation of methodology for simultaneous determination of synthetic dyes in alcoholic beverages by capillary electrophoresis. J Chromatogr A 1136:231–236CrossRefPubMedGoogle Scholar
  34. Ruxton C (2009) Health aspects of caffeine: benefits and risks. Nurs Stand 24:41–48CrossRefPubMedGoogle Scholar
  35. Shin JY, Jung MY (2017) Ultra-High-Throughput Analytical Strategy Based on UHPLC-DAD in Combination with Syringe Filtration for the Quantification of 9 Synthetic Colorants in Beverages: Impacts of Syringe Membrane Types and Sample pH on Recovery Journal of Agricultural & Food ChemistryGoogle Scholar
  36. Soponar F, Moţ AC, Sârbu C (2008) Quantitative determination of some food dyes using digital processing of images obtained by thin-layer chromatography. J Chromatogr A 1188:295–300CrossRefPubMedGoogle Scholar
  37. Swithers SE (2013) Artificial sweeteners produce the counterintuitive effect of inducing metabolic derangements. Trends Endocrinol Metab 24:431–441CrossRefPubMedPubMedCentralGoogle Scholar
  38. Tauler R (1995) Multivariate curve resolution applied to second order data. Chemometr Intell Lab Syst 30:133–146CrossRefGoogle Scholar
  39. Wasik A, Mccourt J, Buchgraber M (2007) Simultaneous determination of nine intense sweeteners in foodstuffs by high performance liquid chromatography and evaporative light scattering detection--development and single-laboratory validation. J Chromatogr A 1157:187–196CrossRefPubMedGoogle Scholar
  40. Wu HL, Shibukawa M, Oguma K (1998) An alternating trilinear decomposition algorithm with application to calibration of HPLC–DAD for simultaneous determination of overlapped chlorinated aromatic hydrocarbons. J Chemometr 12:1–26CrossRefGoogle Scholar
  41. Xiang SX, Kang C, Xie LX, Yin XL, Gu HW, Yu RQ (2015) Fast quantitative analysis of four tyrosine kinase inhibitors in different human plasma samples using three-way calibration-assisted liquid chromatography with diode array detection. J Sep Sci 38:2781–2788CrossRefPubMedGoogle Scholar
  42. Yin X-L, Wu HL, Gu HW, Hu Y, Wang L, Xia H, Xiang SX, Yu RQ (2016) Chemometrics-assisted high performance liquid chromatography-diode array detection strategy to solve varying interfering patterns from different chromatographic columns and sample matrices for beverage analysis. J Chromatogr A 1435:75–84CrossRefPubMedGoogle Scholar
  43. Yin X-L, Wu HL, Gu HW, Zhang XH, Sun YM, Hu Y, Liu L, Rong QM, Yu RQ (2014) Chemometrics-enhanced high performance liquid chromatography-diode array detection strategy for simultaneous determination of eight co-eluted compounds in ten kinds of Chinese teas using second-order calibration method based on alternating trilinear decomposition algorithm. J Chromatogr A 1364:151–162CrossRefPubMedGoogle Scholar
  44. Yoshikawa K, Saito S, Sakuragawa A (2011) Simultaneous analysis of acidulants and preservatives in food samples by using capillary zone electrophoresis with indirect UV detection. Food Chem 127:1385–1390CrossRefPubMedGoogle Scholar
  45. Zhang Y, Wu H-L, Xia A-L, Hu L-H, Zou H-F, Yu R-Q (2007) Trilinear decomposition method applied to removal of three-dimensional background drift in comprehensive two-dimensional separation data. J Chromatogr A 1167:178–183CrossRefPubMedGoogle Scholar

Copyright information

© Springer Science+Business Media, LLC, part of Springer Nature 2018

Authors and Affiliations

  1. 1.State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical EngineeringHunan UniversityChangshaChina
  2. 2.Institute of Quality and Standards for Agricultural ProductsZhejiang Academy of Agricultural SciencesHangzhouChina

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