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Analysis of Migrating Chemicals and Residues from Plastic, Bioplastic and Recycled Food Contact Materials (FCM) in Food Matrices

A special issue of Applied Sciences (ISSN 2076-3417). This special issue belongs to the section "Food Science and Technology".

Deadline for manuscript submissions: closed (31 July 2024) | Viewed by 11884

Special Issue Editor


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Guest Editor
Department of Food Science, Centre of Innovative Food Research (iFood), Aarhus University, 8200 Aarhus N, Denmark
Interests: analytical chemistry; food contact materials (intentionally added substances (IAS) and non-intentionally added substances (NIAS)); sustainability and recycling of plastics
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Plastic materials, also known as food contact materials (FCM), are widely used in food packaging applications. However, there is increased concern over the possible content of these packaging materials, and the subsequent release of undesirable components into foodstuffs or food simulants due to migration. During the production of these plastics, several compounds can be released, either intentionally added substances (IAS) like monomers and production chemicals (i.e antioxidants) or the so-called non-intentionally added substances (NIAS). These are generated as a result of reaction and degradation processes or due to the presence of impurities in the raw materials used for packaging production. This category of substances might include up to several thousands of compounds, where the vast majority are unknown.

Therefore, any development of new materials, including the increased interest in producing bioplastics (or biopolymers), whether chemical or mechanical (or bioplastics), requires a proper risk and safety assessment.   This includes the safety of new types of materials as well as the safe recycling of plastics. This risk assessment mainly focuses on identifying and quantifying the migrating IAS and NIAS compounds, a task which might also include their structural elucidation in the case of unknown compounds. Hence, the development of appropriate analytical methods is of great importance.

Furthermore, at the moment there is a high interest worldwide to promote the 3R sustainable approach, representing the need to “recycle”, “reuse” and “reduce” plastic materials. Within this framework, the assessment of the materials’ quality is fundamental. Towards this direction, the main research focus is being given to the analysis of what is migrating to respective food simulants, and what is less extended in food per se.

As such, this Special Issue will focus on qualitative and quantitative analysis of these compounds, mainly in food matrices. This includes identification, structural elucidation, method development, and validation, with efforts made to highlight and address any potential scientific and analytical challenges.

Dr. Emmanouil Tsochatzis
Guest Editor

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Keywords

  • food contact materials
  • food matrices
  • recycling of plastic FCM
  • bioplastics and biopolymers
  • fossil fuel plastic FCM
  • intentionally added substances (IAS)
  • non-intentionally added substances (NIAS)
  • analysis, identification, and quantification
  • migration testing
  • specific migration limits
  • analysis in foods
  • toxicity evaluation and assessment
  • exposure studies
  • risk assessment

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Published Papers (7 papers)

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Research

17 pages, 443 KiB  
Article
Toxic Metals Migration from Plastic Food Contact Materials in Romania: A Health Risk Assessment
by Gabriel Mustatea, Andreea L. Mocanu, Corina A. Stroe and Elena L. Ungureanu
Appl. Sci. 2024, 14(23), 10985; https://doi.org/10.3390/app142310985 - 26 Nov 2024
Viewed by 492
Abstract
Food packaging plays an essential role in preserving food quality. However, heavy metals found in packaging materials—whether intentionally incorporated or not—can migrate into food. This study aims to evaluate the migration of specific heavy metals (Ba, Co, Cu, Zn, Al, Ni, Li, Fe, [...] Read more.
Food packaging plays an essential role in preserving food quality. However, heavy metals found in packaging materials—whether intentionally incorporated or not—can migrate into food. This study aims to evaluate the migration of specific heavy metals (Ba, Co, Cu, Zn, Al, Ni, Li, Fe, Pb, Cd, Cr, Sb) from plastic food packages (films and bags) obtained from various materials (PE, PP, PVC, composite materials) into food simulant B (3% acetic acid) using inductively coupled plasma mass spectrometry (ICP-MS). Migration tests was conducted according to EU regulations, using OM2 conditions (10 days at 40 °C). The obtained results were lower than the specific migration limits set by EU Regulation no. 10/2011 (Annex II). Both carcinogenic and non-carcinogenic risk assessments were carried out based on the specific migration data, estimating the exposure, average daily dose (ADD), hazard quotient (HQ), hazard index (HI), cancer risk (CR), and total cancer risk (TCR). The exposure values were found to be below the recommended tolerable daily intake (TDI) levels for each metal tested. Both HQ and HI values were under the limit value of 1. The average total cancer risk was 1.73 × 10−4, indicating that approximately 1.73 consumers out of 10,000 may develop a type of cancer due to chronic exposure to the tested metals. These results highlight the importance of continuous monitoring of chemical migrants from food contact materials. Full article
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13 pages, 520 KiB  
Article
Styrene Migration from Polystyrene for Food Contact: A Case Study on the Processing Chain of Yoghurt Pots
by Valeria Guazzotti, Veronika Hendrich, Anita Gruner, Dominik Fiedler, Angela Störmer and Frank Welle
Appl. Sci. 2024, 14(19), 9056; https://doi.org/10.3390/app14199056 - 7 Oct 2024
Viewed by 923
Abstract
A precautionary specific migration limit of 40 µg/kg for styrene from food contact materials is currently under evaluation in Europe. In the ongoing discussion about applicable methods to demonstrate compliance, testing with food instead of simulants or total transfer calculations has been proposed. [...] Read more.
A precautionary specific migration limit of 40 µg/kg for styrene from food contact materials is currently under evaluation in Europe. In the ongoing discussion about applicable methods to demonstrate compliance, testing with food instead of simulants or total transfer calculations has been proposed. In this study, the residual styrene levels in high-impact polystyrene (HIPS) blended with general-purpose polystyrene (GPPS) were determined at several levels of the processing chain of yoghurt pots (from pellets to sheets, then to pots). The styrene migration from extruded sheets and thermoformed pots was analyzed in food simulants at 10 days/20 °C and 40 °C, as well as in yoghurt after storage at 8 °C after 50 days. The obtained results show that the residual styrene content in the PS materials correlates with migration. However, the migration of styrene was far below the total transfer assumption. Styrene migration from the sheets into food simulants and into yoghurt exceeded that migrating from the pots. Styrene migration into food simulants in 20% ethanol at 10 days/20 °C and 40 °C and, more clearly, in 50% ethanol at 10 days/40 °C, was higher than that into yoghurt tested on the best-before date. Styrene migration from PS pots into yoghurt after storage at 8 °C for 50 days reached up to 15 µg/kg (applying the EU cube model), which would be conservatively covered by testing the PS pots with 20% ethanol at 10 days/20 °C. Full article
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16 pages, 1013 KiB  
Article
Determination of Diffusion Coefficients of Bisphenol A (BPA) in Polyethylene Terephthalate (PET) to Estimate Migration of BPA from Recycled PET into Foods
by Mladen Juric, Roland Franz and Frank Welle
Appl. Sci. 2024, 14(17), 7704; https://doi.org/10.3390/app14177704 - 31 Aug 2024
Viewed by 1231
Abstract
Bisphenol A (BPA) is a known substance that is found in food contact materials as an intentionally added as well as a non-intentionally added substance. Traces of BPA were found as a non-intentionally added substance in recycled PET (rPET). In 2023, the EFSA [...] Read more.
Bisphenol A (BPA) is a known substance that is found in food contact materials as an intentionally added as well as a non-intentionally added substance. Traces of BPA were found as a non-intentionally added substance in recycled PET (rPET). In 2023, the EFSA proposed a new TDI of 0.0002 µg/kg bw/d, which is lower than the previous (temporary) TDI of 4 µg/kg bw/d by a factor of 20,000. The TDI of 0.0002 µg/kg bw/d would translate for a default 60 kg person eating one kilogram of food into a migration limit of 0.012 µg/kg in the food. This very low migration limit is a challenge to measuring BPA levels in food. A solution is to use migration modeling to establish maximum concentrations in rPET for different food contact applications. Precise diffusion coefficients for BPA in PET were determined within this study by use of migration kinetics. In June 2024, the European Commission proposed a new migration threshold limit for BPA of 1 µg/kg, which should be understood as a detection limit. From the results of this study, it can be concluded that a BPA concentration in the PET bottle wall of 297 mg/kg (3% acetic acid), 255 mg/kg (10% ethanol), and 192 mg/kg (20% ethanol) after storage for 365 d at 25 °C is in compliance with the migration threshold limit of 1 µg/kg. These maximum concentrations are far above the measured BPA concentrations on rPET bottles in Europe between 2019 and 2023. Therefore, the new proposed migration threshold limit for BPA cannot be exceeded. Full article
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20 pages, 6237 KiB  
Article
Microplastics’ Detection in Honey: Development of Protocols in a Simulation
by Klytaimnistra Katsara, Zacharias Viskadourakis, Eleftherios Alissandrakis, Nikos Kountourakis, George Kenanakis and Vassilis M. Papadakis
Appl. Sci. 2024, 14(11), 4720; https://doi.org/10.3390/app14114720 - 30 May 2024
Viewed by 1318
Abstract
Honey, renowned for its nutritional and therapeutic properties, has recently come under scrutiny due to its contamination by microplastics, in multiple ways. Bees’ exposure to plastic pollution impacts the whole hive’s ecosystem, and plastic tends to accumulate in hive products. Plastic packaging as [...] Read more.
Honey, renowned for its nutritional and therapeutic properties, has recently come under scrutiny due to its contamination by microplastics, in multiple ways. Bees’ exposure to plastic pollution impacts the whole hive’s ecosystem, and plastic tends to accumulate in hive products. Plastic packaging as polyethylene terephthalate (PET) is used to store honey in small flexible packages, which also increases the risk of microplastic migration. This study aims to establish three practical detection methods for PET microplastics and nanoplastics in honey, using readily available laboratory equipment without the need for chemical digestion or costly pretreatment protocols, in a laboratory-based simulation. The first method utilizes Raman micro-spectroscopy, offering high-resolution identification of PET microplastics on cellulose acetate filters with Raman mapping, eliminating the need for organic solvents or dyes. The second method employs optical microscopic observation under fluorescence with the aid of 4-dimethylamino-4′-nitrostilbene dye and ultraviolet radiation to enhance microplastic visibility, making it suitable for laboratories with standard optical microscopes. To isolate MPs from the solid honey particles, a density separator has been introduced using pentane. Lastly, the third method employs the use of electrospray ionization mass spectrometry for the detection of nanoplastics (<200 nm) in honey samples, through the examination of the different extraction phases of density separation. All the aforementioned methods contribute to efficient microplastic detection in honey, ensuring its quality and safe consumption. Full article
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13 pages, 2569 KiB  
Article
Odd-Even Effect of Polyesters‘ Cyclic Oligomers and the Definition of Oligomers Based on Physicochemical Properties
by Joao Alberto Lopes, Fabiano Reniero, Claude Guillou and Emmanouil Tsochatzis
Appl. Sci. 2024, 14(5), 2085; https://doi.org/10.3390/app14052085 - 1 Mar 2024
Viewed by 1281
Abstract
This work explores the definition and characterization of synthetic polymeric oligomers, chemical substances comprising a small number of repeated organic molecules. It highlights the lack of clarity surrounding the range of repeated units that can be classified as an oligomer, and how this [...] Read more.
This work explores the definition and characterization of synthetic polymeric oligomers, chemical substances comprising a small number of repeated organic molecules. It highlights the lack of clarity surrounding the range of repeated units that can be classified as an oligomer, and how this definition is field-dependent. The present study focused on PET cyclic oligomers and revealed that the progression of the ring length from smaller to longer oligomers followed the well-known odd-even effect. This phenomenon affects the physical and chemical properties of oligomers and can also be observed with analytical techniques such as differential scanning calorimetry (DSC), high resolution mass spectrometry (HR-MS) and NMR. Similarities between PET and PBT oligomers were also observed, and an alternative potential definition for oligomers in the polymeric field is suggested based on physical behaviour of the longer cyclic oligomers. Full article
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13 pages, 1910 KiB  
Article
Quantification of Microplastics in Plastic-Bottled Chinese Baijiu Using Micro-FTIR in Imaging Mode
by Xuejun Zhou, Qian Wang, Jin Wang, Hongyan Li, Jiefang Ren and Shali Tang
Appl. Sci. 2023, 13(20), 11142; https://doi.org/10.3390/app132011142 - 10 Oct 2023
Cited by 1 | Viewed by 1679
Abstract
Microplastics (MPs) are prevalent in our environment, being present in the air we breathe and in the food we consume. Due to the widespread use of plastic materials in everyday life, the amount of microplastics being released into the biosphere has become increasingly [...] Read more.
Microplastics (MPs) are prevalent in our environment, being present in the air we breathe and in the food we consume. Due to the widespread use of plastic materials in everyday life, the amount of microplastics being released into the biosphere has become increasingly apparent in recent years. This study provides the first documentation of the presence of microplastics in Chinese baijiu, a popular alcoholic beverage in China, bottled in plastic. It is essential to note the significance of this discovery and potential implications for human health. Analysis of samples collected from the Chinese market showed the presence of microplastics in all six Chinese baijiu brands tested. Concentrations ranged from 172 MPs/500 mL to 944 MPs/500 mL with an average concentration of 436 MPs/500 mL. Cellulose and PA accounted for 70.4% and 17.8% of all microplastics detected, respectively. These were the most commonly detected types. Other types of microplastics were also found, including PET, PP, PVC, and PE. PET accounted for 2.7%, PP for 2.2%, PVC for 1.2%, and PE for 0.1% of all microplastics. The possible sources of contamination include raw materials, ambient air, and equipment and vessels that shed microplastics. Therefore, this study emphasizes the requirement for further research to mitigate the potential hazards associated with human exposure to microplastics. Additionally, it presents significant findings on the presence of microplastics in Chinese baijiu sold in plastic bottles. Full article
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23 pages, 5991 KiB  
Article
Screening of Microplastics in Aquaculture Systems (Fish, Mussel, and Water Samples) by FTIR, Scanning Electron Microscopy–Energy Dispersive Spectroscopy and Micro-Raman Spectroscopies
by Kleopatra Miserli, Christos Lykos, Angelos G. Kalampounias and Ioannis Konstantinou
Appl. Sci. 2023, 13(17), 9705; https://doi.org/10.3390/app13179705 - 28 Aug 2023
Cited by 10 | Viewed by 4070
Abstract
In the last decade, plastic waste has become one of the main threats to marine ecosystems and their biodiversity due to its abundance and increased persistence. Microplastics can be classified as either primary, i.e., fabricated for commercial use, or secondary, i.e., resulting from [...] Read more.
In the last decade, plastic waste has become one of the main threats to marine ecosystems and their biodiversity due to its abundance and increased persistence. Microplastics can be classified as either primary, i.e., fabricated for commercial use, or secondary, i.e., resulting from the fragmentation/weathering processes of larger plastic pieces in the environment. In general, microplastics are detected in a number of aquatic organisms (e.g., fish, bivalves, mollusks, etc.) with alarming effects on their health. Therefore, the present work focuses on the detection and identification of microplastics in fish species (Dicentrarchus labrax, Sparus aurata) and mussels (Mytilus galloprovincialis) from aquaculture systems since these aquatic organisms are largely commercially available for consumption. In addition, seawater was also screened for the types of polymers present as well as their aging. The experimental protocol for biota samples contains a digestion step using Fenton’s reagent (0.05 M FeSO4⋅7H2O with 30% H2O2 at a volume ratio of 1:1) to remove organic material followed by filtration and a density separation step where the sample material was mixed with a saturated ZnCl2 solution to separate microplastic particles from heavier material. For seawater samples (sampled by a microplastic net sampler), only sieving on stainless steel sieves followed by filtration on silica filters was applied. Detection of microplastics and identification of their polymeric composition was achieved through the combined use of micro-Raman analysis, Attenuated Total Reflectance–Fourier Transform Infrared spectroscopy, and Scanning Electron Microscopy in tandem with Energy Dispersive X-ray spectroscopy. Microplastic abundance was 16 ± 1.7 items/individual in mussels and 22 ± 2.1 items/individual in sea bass, and 40 ± 3.9 items/individual in sea bream, with polyethylene (74.4%) being the most detected polymer type, while polyethylene-co-vinyl acetate (65%), polyvinyl-butyral (36.8%), polyvinyl alcohol (20%), and polybutyl methacrylate (15.8%) were also detected to a lesser extent. The microplastics isolated from seawater samples were films (30%), fragments (30%), and fibers (20%), while some of them were derived from foams (20%). Also, in most of these seawater-recovered microplastics, a relatively high degree of oxidation (carbonyl index > 0.31) was observed, which was further confirmed by the results of Energy Dispersive X-ray spectroscopy. Finally, the Scanning Electron Microscopy images showed various morphological characteristics (cracks, cavities, and burrs) on the surfaces of the microplastics, which were attributed to environmental exposure. Full article
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