Analytical and Bioanalytical Chemistry

, Volume 410, Issue 16, pp 3789–3803 | Cite as

Identification of intentionally and non-intentionally added substances in plastic packaging materials and their migration into food products

  • Verónica García Ibarra
  • Ana Rodríguez Bernaldo de Quirós
  • Perfecto Paseiro Losada
  • Raquel Sendón
Research Paper


Plastic materials are widely used in food packaging applications; however, there is increased concern because of the possible release of undesirable components into foodstuffs. Migration of plastic constituents not only has the potential to affect product quality but also constitutes a risk to consumer health. In order to check the safety of food contact materials, analytical methodologies to identify potential migrants are required. In the first part of this work, a GC/MS screening method was developed for the identification of components from plastic packaging materials including intentionally and “non-intentionally added substances” (NIAS) as potential migrants. In the second part of this study, the presence of seven compounds (bis (2-ethylhexyl) phthalate (DEHP), diethyl phthalate (DEP), diisobutyl phthalate (DIBP), dibutyl phthalate (DBP), butylated hydroxytoluene (BHT), acetyl tributyl citrate (ATBC), benzophenone (BP)) previously identified in packaging materials were investigated in food products (corn and potatoes snacks, cookies, and cakes). For this purpose, a suitable extraction method was developed and quantification was performed using GC-MS. The developed method was validated in terms of linearity, recovery, repeatability, and limits of detection and quantification. The spiked recoveries varied between 82.7 and 116.1%, and relative standard deviation (RSD) was in the range of 2.22–15.9%. The plasticizer ATBC was the most detected compound (94% samples), followed by DEP (65%), DEHP (47%), BP (44%), DBP (35%), DIBP (21%), and BHT (12%). Regarding phthalates, DEP and DEHP were the most frequently detected compounds in concentrations up to 1.44 μg g−1. In some samples, only DBP exceeded the European SML of 0.3 mg kg−1 established in Regulation 10/2011.

Graphical abstract

Chemical migration from plastic packaging into food


Screening method Food packaging materials NIAS Migration studies GC-MS 



The study was financially by the “Ministerio de Economía y Competitividad” and by “Fondo Europeo de Desarrollo Regional (FEDER), Ref. No. AGL2015-69609-P “MIGRAEXPO,” (MINECO/FEDER,UE). V. García Ibarra is grateful for her grant from SENESCYT-Ecuador.

Compliance with ethical standards

Conflict of interest

The authors declare that there are no conflicts of interest.


  1. 1.
    Guart A, Bono-Blay F, Borrell A, Lacorte S. Migration of plasticizers, phthalates, bisphenol A and alkylphenols from plastic containers and evaluation of risk. Food Addit Contam. 2011;28:676–85.CrossRefGoogle Scholar
  2. 2.
    Bhunia K, Sablani S, Tang J, Rasco B. Migration of chemical compounds from packaging polymers during microwave, conventional heat treatment, and storage. Compr Rev Food Sci Food Saf. 2013;12:523–45.CrossRefGoogle Scholar
  3. 3.
    Piringer OG, Baner AL. Plastic packaging: interactions with food and pharmaceuticals. 2nd ed. Weinheim: Wiley-VCH Verlag GmbH; 2007.Google Scholar
  4. 4.
    European Commission. Commission Regulation 10/2011 on plastic materials and articles intended to come into contact with food. Off J Eur Communities 2011; L12: 1–89 and amendments.Google Scholar
  5. 5.
    Nerin C, Alfaro P, Aznar M, Domeño C. The challenge of identifying non-intentionally added substances from food packaging materials: a review. Anal Chim Acta. 2013;775:14–24.CrossRefPubMedGoogle Scholar
  6. 6.
    Cherta L, Portolés T, Pitarch E, Beltran J, López FJ, Calatayud C, et al. Analytical strategy based on the combination of gas chromatography coupled to time-of-flight and hybrid quadrupole time-of-flight mass analyzers for non-target analysis in food packaging. Food Chem. 2015;188:301–8.CrossRefPubMedGoogle Scholar
  7. 7.
    Nerin C, Canellas E, Aznar M, Silcock P. Analytical methods for the screening of potential volatile migrants from acrylic-base adhesives used in food-contact materials. Food Addit Contam. 2009;26:1592–601.CrossRefGoogle Scholar
  8. 8.
    Isella F, Canellas E, Bosetti O, Nerin C. Migration of non intentionally added substances from adhesives by UPLC-Q-TOF/MS and the role of EVOH to avoid migration in multilayer packaging materials. J Mass Spectrom. 2013;48:430–7.CrossRefPubMedGoogle Scholar
  9. 9.
    Rothenbacher T, Schwack W. Nontargeted multicomponent analytical screening of plastic food contact materials using fast interpretation of deliverables via expert structure-activity relationship software. J AOAC Int. 2009;92:941–50.PubMedGoogle Scholar
  10. 10.
    Skjevrak I, Brede C, Steffensen IL, Mikalsen A, Alexander J, Fjeldal P, et al. Non-targeted multi-component analytical surveillance of plastic food contact materials: identification of substances not included in EU positive lists and their risk assessment. Food Addit Contam. 2005;22:1012–22.CrossRefPubMedGoogle Scholar
  11. 11.
    Félix JS, Isella F, Bosetti O, Nerín C. Analytical tools for identification of non-intentionally added substances (NIAS) coming from polyurethane adhesives in multilayer packaging materials and their migration into food simulants. Anal Bioanal Chem. 2012;403:2869–82.CrossRefPubMedGoogle Scholar
  12. 12.
    Fromme H, Gruber L, Schlummer M, Wolz G, Böhmer S, Angerer J, et al. Intake of phthalates and di (2-ethylhexyl) adipate: results of the Integrated Exposure Assessment Survey based on duplicate diet samples and biomonitoring data. Environ Int. 2007;33:1012–20.CrossRefPubMedGoogle Scholar
  13. 13.
    Serôdio P, Nogueira JMF. Considerations on ultra-trace analysis of phthalates in drinking water. Water Res. 2009;40:2572–82.CrossRefGoogle Scholar
  14. 14.
    Carrillo JD, Salazar C, Moreta C, Tena MT. Determination of phthalates in wine by headspace solid-phase microextraction followed by gas chromatography–mass spectrometry: fibre comparison and selection. J Chromatogr A. 2007;1164:248–61.CrossRefPubMedGoogle Scholar
  15. 15.
    He J, Lv R, Zhu J, Lu K. Selective solid-phase extraction of dibutyl phthalate from soybean milk using molecular imprinted polymers. Anal Chim Acta. 2010;661:215–21.CrossRefPubMedGoogle Scholar
  16. 16.
    Nara K, Nishiyama K, Natsugari H, Takeshita A, Takahashi H. Leaching of the plasticizer, acetyl tributyl citrate:(ATBC) from plastic kitchen wrap. J Health Sci. 2009;55:281–4.CrossRefGoogle Scholar
  17. 17.
    Badeka AB, Kontominas MG. Effect of microwave heating on the migration of dioctyladipate and acetyltributylcitrate plasticizers from food-grade PVC and PVDC/PVC films into olive oil and water. Z Lebensm Unters Forsch. 1996;202:313–7.CrossRefPubMedGoogle Scholar
  18. 18.
    Anderson WAC, Castle L. Benzophenone in cartonboard packaging materials and the factors that influence its migration into food. Food Addit Contam. 2003;20:607–18.CrossRefPubMedGoogle Scholar
  19. 19.
    Lago MA, Sendón R, Rodríguez-Bernaldo de Quirós A. Photocured materials. In Tiwari A, Polykarpov A, editors. Analytical methods for determining photoinitiators in food-contact materials. Cambridge R Soc Chem; 2015. pp. 1–9.Google Scholar
  20. 20.
    Patlewicz G, Jeliazkova N, Safford RJ, Worth AP, Aleksiev B. An evaluation of the implementation of the Cramer classification scheme in the Toxtree software. SAR QSAR Environ Res. 2008;19:495–524.CrossRefPubMedGoogle Scholar
  21. 21.
    Toxtree. Toxtree—Toxic Hazard Estimation by decision tree approach. 2015. Accessed 16 March 2015.
  22. 22.
    Gil N, Saska M, Negulescu I. Evaluation of the effects of biobased plasticizers on the thermal and mechanical properties of poly (vinyl chloride). J Appl Polym Sci. 2006;102:1366–73.CrossRefGoogle Scholar
  23. 23.
    Sheftel VO. Indirect food additives and polymers: migration and toxicology. London: Boca Raton: Lewis Publishers; 2000.Google Scholar
  24. 24.
    Sheftel VO. Handbook of toxic properties of monomers and additives. Florida: Boca Raton: Lewis Publishers; 1995.Google Scholar
  25. 25.
    Heudorf U, Mersch-Sundermann V, Angerer J. Phthalates: toxicology and exposure. Int J Hyg Environ Health. 2007;210:623–34.CrossRefPubMedGoogle Scholar
  26. 26.
    Serrano SE, Braun J, Trasande L, Dills R, Sathyanarayana S. Phthalates and diet: a review of the food monitoring and epidemiology data. Environ Health. 2014;13:1–13.CrossRefGoogle Scholar
  27. 27.
    Lahimer MC, Ayed N, Horriche J, Belgaied S. Characterization of plastic packaging additives: food contact, stability and toxicity. Arab J Chem. 2017;10:S1938–S54.CrossRefGoogle Scholar
  28. 28.
    Ash M, Ash I. Handbook of preservatives. New York: Synapse Information Resources Inc; 2004.Google Scholar
  29. 29.
    Lago MA, Ackerman LK. Identification of print-related contaminants in food packaging. Food Addit Contam Part A. 2016;33:518–29.CrossRefGoogle Scholar
  30. 30.
    Clemente I, Aznar M, Nerín C, Bosetti O. Migration from printing inks in multilayer food packaging materials by GC-MS analysis and pattern recognition with chemometrics. Food Addit Contam Part A. 2016;33:703–14.Google Scholar
  31. 31.
    Llop C, Manrique A, Navarro R, Mijangos C, Reinecke H. Control of the migration behavior of slip agents in polyolefin-based films. Polym Eng Sci. 2011;51:1763–9.CrossRefGoogle Scholar
  32. 32.
    Dupáková Z, Dobiáš J, Votavová L, Klaudisová K, Voldrich M. Occurrence of extractable ink residuals in packaging materials used in the Czech Republic. Food Addit Contam. 2010;27:97–106.CrossRefGoogle Scholar
  33. 33.
    American Chemical Society (ACS). Subcommittee of environmental analytical chemistry. Anal Chem. 1980;52:2242–80.CrossRefGoogle Scholar
  34. 34.
    Poças MF, Oliveira JC, Pereira JR, Hogg T. Consumer exposure to phthalates from paper packaging: an integrated approach. Food Addit Contam. 2010;27:1451–9.CrossRefGoogle Scholar
  35. 35.
    Zygoura PD, Paleologos EK, Kontominas MG. Changes in the specific migration characteristics of packaging–food simulant combinations caused by ionizing radiation: effect of food simulant. Radiat Phys Chem. 2011;80:902–10.CrossRefGoogle Scholar
  36. 36.
    Cao XL, Zhao W, Dabeka R. Di-(2-ethylhexyl) adipate and 20 phthalates in composite food samples from the 2013 Canadian Total Diet Study. Food Addit Contam Part A. 2015;32:1893–901.CrossRefGoogle Scholar
  37. 37.
    Bradley EL, Burden RA, Leon I, Mortimer DN, Speck DR, Castle L. Determination of phthalate diesters in foods. Food Addit Contam Part A. 2013;27:722–34.CrossRefGoogle Scholar
  38. 38.
    Pastorelli S, Sanches-Silva A, Cruz JM, Simoneau C, Losada PP. Study of the migration of benzophenone from printed paperboard packages to cakes through different plastic films. Eur Food Res Technol. 2008;227:1585–90.CrossRefGoogle Scholar
  39. 39.
    Xu D, Deng X, Fang E, Zheng X, Zhou Y, Lin L, et al. Determination of 23 phthalic acid esters in food by liquid chromatography tandem mass spectrometry. J Chromatogr A. 2014;1324:49–56.CrossRefPubMedGoogle Scholar
  40. 40.
    Guo Y, Zhang Z, Liu L, Li Y, Ren N, Kannan K. Occurrence and profiles of phthalates in foodstuffs from China and their implications for human exposure. J Agric Food Chem. 2012;60:6913–9.CrossRefPubMedGoogle Scholar
  41. 41.
    Fierens T, Servaes K, Van Holderbeke M, Geerts L, De Henauw S, Sioen I, et al. Analysis of phthalates in food products and packaging materials sold on the Belgian market. Food Chem Toxicol. 2012;50:2575–83.CrossRefPubMedGoogle Scholar
  42. 42.
    Tsumura Y, Ishimitsu S, Kaihara A, Yoshii K, Tonogai Y. Phthalates, adipates, citrate and some of the other plasticizers detected in Japanese retail foods: a survey. J Health Sci. 2002;48:493–502.CrossRefGoogle Scholar
  43. 43.
    Van Den Houwe K, Van Heyst A, Evrard C, Van Loco J, Bolle F, Lynen F, et al. Migration of 17 photoinitiators from printing inks and cardboard into packaged food—results of a Belgian market survey. Packag Technol Sci. 2016;29:121–31.CrossRefGoogle Scholar
  44. 44.
    Xu Q, Yin X, Wang M, Wang H, Zhang N, Shen Y, et al. Analysis of phthalate migration from plastic containers to packaged cooking oil and mineral water. J Agric Food Chem. 2010;58:11311–7.CrossRefPubMedGoogle Scholar
  45. 45.
    Rodríguez-Bernaldo de Quirós A, Paseiro-Cerrato R, Pastorelli S, Koivikko R, Simoneau C, Paseiro-Losada P. Migration of photoinitiators by gas phase into dry foods. J Agric Food Chem. 2009;57:10211–5.CrossRefPubMedGoogle Scholar

Copyright information

© Springer-Verlag GmbH Germany, part of Springer Nature 2018

Authors and Affiliations

  • Verónica García Ibarra
    • 1
  • Ana Rodríguez Bernaldo de Quirós
    • 1
  • Perfecto Paseiro Losada
    • 1
  • Raquel Sendón
    • 1
  1. 1.Faculty of Pharmacy, Department of Analytical Chemistry, Nutrition and Food ScienceUniversity of Santiago de CompostelaSantiago de CompostelaSpain

Personalised recommendations