Experimental direct evaluation of functional barriers in PET recycled bottles: comparison of migration behaviour of mono‐ and multilayers

Pennarun, Pierre-Yves; Saillard, P.; Feigenbaum, Alexandre; Dole, Patrice

doi:10.1002/pts.680

Cited by 22 publications

(19 citation statements)

References 23 publications

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“…The surrogates used in challenge tests to determine the decontamination efficiency of PET recycling processes are substances with different molecular weights and polarities representative of possible chemical classes of contaminants of concern that were demonstrated to be suitable to monitor the behaviour of PET during recycling (Pennarun et al, 2005;FDA, 2006).…”

Section: Criteria Specific To the Safety Evaluation Of Recycled Hdpe mentioning

confidence: 99%

Scientific Opinion on the safety assessment of the processes ‘Biffa Polymers’ and ‘CLRrHDPE’ used to recycle high‐density polyethylene bottles for use as food contact material

Flavourings¹

2015

EFS2

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This scientific opinion of the EFSA Panel on Food Contact Materials, Enzymes, Flavourings and Processing Aids (CEF Panel) deals with the safety assessment of the recycling processes 'CLRrHDPE' and 'Biffa Polymers'. These processes are used to recycle post-consumer high-density polyethylene (HDPE) bottles which have been in contact with food, mainly milk, to produce recycled HDPE pellets. Post-consumer HDPE bottles are collected in the United Kingdom and processed by conventional recycling including manual sorting into washed and dried HDPE flakes containing no more than 1 % HDPE from non-food consumer applications. The washed and dried HDPE flakes are heated in two successive continuous reactors under vacuum before being extruded under vacuum into pellets. Recycled pellets are blended with virgin HDPE to produce bottles (both processes) and with virgin polypropylene to produce trays (Biffa Polymers). Bottles are intended for storage of milk and fruit juices. Trays are intended for storage of animal products and raw fruits, vegetables and mushrooms. Having examined the challenge tests provided, the Panel noted the limited decontamination efficiency under the conditions of testing and concluded that the processes do not satisfy criteria set for HDPE. Uncertainties and consequent conservatism of the selected criteria could allow the conclusion that a process is safe when these criteria are met but not when they are not met. Therefore, the CEF Panel considered that, for the manufacture of recycled bottles for milks and fruit juices and trays for animal products, additional data should be provided before it can conclude on the safety assessment. For the manufacture of recycled trays intended for contact with whole fruits and vegetables including mushrooms, at room temperature or below, the CEF Panel concluded that recycled HDPE obtained from the process Biffa Polymers is not considered of safety concern under the restriction given in the opinion.

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Section: Criteria Specific To the Safety Evaluation Of Recycled Hdpe mentioning

confidence: 99%

Scientific Opinion on the safety assessment of the processes ‘Biffa Polymers’ and ‘CLRrHDPE’ used to recycle high‐density polyethylene bottles for use as food contact material

Flavourings¹

2015

EFS2

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“…It depends on C* Food Experimental diffusion data have been described in previous papers. 4,5 Averaged values of D* at the plateau (values for M < 130) and straight line equations correlating log D* and M (all values available) are calculated assuming a 90% confidence level using appropriate Student factors (N = 4 S = 1.53; N = 5 S = 1.48; N = 8 S = 1.4, N = 13 S = 1.35; N = 15 S = 1.34). The overestimated equations are obtained by adding the standard deviation (corrected by the adequate Student factor) to the average values or to the straight line regressions.…”

Section: Numerical Simulationsmentioning

confidence: 99%

“…This is why, in a previous study, we generated reference data for PET, 4 for representative sets of molecules and on the basis of diffusion and specific migration tests. 5 In the present paper, we use these experimental data to propose empirical equations for overestimated diffusion coefficients in PET at 40°C. The relationships are then used to predict diffusion/migration behaviour at 40°C, for monolayer bottles and for multilayer (with functional barriers) bottles.…”

Section: Introductionmentioning

confidence: 99%

“…Actual (D) and overestimated (D*) diffusion coefficients are lower for PET/PET than for PET/ethanol tests, which is consistent with the strong plasticizing effect of ethanol. 4,5 The slope for the overestimated (0.0148) diffusion coefficients is lower with ethanol than without solvent (0.0289) (equation 1). This is also in agreement with general knowledge on swelling and thermal effects described for other polymers.…”

mentioning

confidence: 96%

“…5,11,[13][14][15][16] Propylene glycol (M = 64 g/mol) is the only compound we found in these references with molecular weight below 80 g/mole; however its strong capacity to form hydrogen bonds with PET strongly reduces its volatility and most likely also its diffusion coefficient.…”

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confidence: 99%

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Overestimated diffusion coefficients for the prediction of worst case migration from PET: application to recycled PET and to functional barriers assessment

2004

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This paper defines parameters that can be used to predict worst-case migration from recycled PET bottles, with and without a functional barrier. Starting with a set of diffusion coefficients determined in well-defined experimental conditions (temperature, presence or not of a solvent, with and without swelling effect), empirical equations for the diffusion coefficient of a migrant or a pollutant in PET at 40°C are given as a function of its molecular weight. An equation is also derived for migration from PET into water. Surrogates representative of worst-case migrants are identified and are discussed in terms of molecular weight, structure and interaction with the PET matrix. In the second part of the paper, the empirical equations have been used to simulate the migration from monolayer bottles and from multilayer bottles with different geometries of functional barrier, as a function of the pollutants' molecular weight. Since the diffusion coefficients are overestimated, the calculated migration is also overestimated, which provides a margin of safety. The advantage of the functional barrier technology is compared to the direct food contact route, as a function of food contact time. In the last part of the paper, the effect of testing temperature is investigated. Based on a literature survey, the activation energy of pollutants is shown to increase roughly with their molecular weights. A worst-case activation energy of 80 kJ/mol is proposed, allowing extrapolation of migration data from a higher temperature (values calculated at 40°C or determined at 60°C) to room temperature. The possible use of this activation energy to design tests for functional barriers is discussed. Copyright

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Functional barriers in PET recycled bottles. Part I. Determination of diffusion coefficients in bioriented PET with and without contact with food simulants

Pennarun¹,

Dole²,

Feigenbaum³

2004

J of Applied Polymer Sci

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A major outcome for recycled plastics consists of making food packaging materials. However, any contamination of collected plastics with chemicals may then be of concern for public health. A solution to mind migration is to use a layer of virgin polymer, named functional barrier, intercalated between the recycled layer and the food. This article aims to provide experimental values of diffusion coefficients (D) of model pollutants (surrogates) in poly(ethylene terephthalate) (PET) to be used for modeling migration through functional barriers. Diffusion coefficients of a large set of surrogates at low concentrations in PET were measured in various conditions. A solid-to-solid diffusion test was designed to avoid the use of a solvent that may induce plasticizing of the material and partitioning effects at the interface. Using [Log D ϭ f(molecular weight)] correlations, the values of diffusion coefficients and activation energies of the surrogates measured by this method were shown to be consistent with the literature data obtained for gases, in permeation experiments, where no plasticization occurred. Migration from PET into food simulants was then studied. Migration into an aqueous medium is largely influenced by the solubility of the surrogates, the less soluble ones being not detected, despite high D values. With ethanol solvent, there were no partitioning effects, and the high plasticization effect of PET by ethanol considerably increases the apparent diffusion coefficients. The effects of temperature and plasticization on the relationship between diffusion coefficients and molecular weight are discussed.

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Experimental direct evaluation of functional barriers in PET recycled bottles: comparison of migration behaviour of mono‐ and multilayers

Cited by 22 publications

References 23 publications

Scientific Opinion on the safety assessment of the processes ‘Biffa Polymers’ and ‘CLRrHDPE’ used to recycle high‐density polyethylene bottles for use as food contact material

Scientific Opinion on the safety assessment of the processes ‘Biffa Polymers’ and ‘CLRrHDPE’ used to recycle high‐density polyethylene bottles for use as food contact material

Overestimated diffusion coefficients for the prediction of worst case migration from PET: application to recycled PET and to functional barriers assessment

Functional barriers in PET recycled bottles. Part I. Determination of diffusion coefficients in bioriented PET with and without contact with food simulants

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