Migration of toxic elements from recycled paper food contact materials to food simulants
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barium were exclusively identified in the dried pellet and were below the LOR of the diluted solutions. The LORs for all analyzed elements per sample are provided as Supplementary Material. The number and quantity of elements detected by DFM and DE were frequently similar in the dried pellets, with no elements detected above the LOR in the diluted solution. Magnesium, aluminum, copper, zinc, and barium were de- tected at comparable concentrations in the dried pellets of both FFM and FE. Cerium was exclusively detected in the dried pellet form of the DFM sample, the concentration of which was below the LOR for the diluted solution. Similarly, lead was detected in the dried pellet form of DE; however, this was below the LOR for the diluted solution form. The number of detected elements was greater with AFM than with LFM, FFM, and DFM in the descending order. In the first three samples, a greater number and concentration of elements were typically detected in the migration samples than in the corresponding extracts, LAE and FE. The food simulant compositions for the AFM, LFM, and FFM samples were 3% acetic acid, 10% ethanol, and 50% ethanol (volume fraction), respectively, while the solvent for the exhaustive extraction equivalents was acetone/methanol (1:1, volume ratio). For DFM and DE, which share the same solvent com- position, there were no significant differences in the profile of detected elements regarding the number and concentration. In addition, the required dilution of solutions to reduce the or- ganic content increased the LOR of the samples by five times for the AFM and LFM samples, 25 times for the FFM sam- ples, and 50 times for the DFM, DE, LAE, and FE samples compared with the LOR of the dried pellets. Comparison of detected elemental levels to regulatory SMLs and tolerable intake values The migration samples and extracts exhibited elevated levels of toxic elements. Specifically, migration samples—AFM, LFM, and FFM—contained concentrations of numerous elements that exceeded regulatory SMLs and tolerable intake values. Table 4 presents the SMLs for various toxic elements as stipulated by EU and Dutch legislation. In addition, toler- able intake values, including tolerable weekly intake (TWI), tolerable daily intake (TDI), tolerable upper intake level (UL), and reference threshold values such as NOAEL, LOAEL, and BDML, were identified using the OpenFoodTox database. These threshold values are accompanied by their respective toxicological endpoints. cTDI values were determined by dividing the reference threshold values by a UF of 100. Compared with the regulatory SMLs, greater quantities and tolerable intake values were detected in AFM for 12 elements, LFM for nine elements, FFM for eight elements, and DFM for four elements. The extraction counterparts of the samples, LAE, FE, and DE, contained higher levels of alu- minum, copper, zinc, and barium compared with the safety reference values, whereas DE additionally contained a large quantity of lead. Specifically, aluminum was detected in extremely large quantities in the FFM and AFM samples, approximately 10 and 8 g/kg of food simulant, respectively. These quantities ex- ceed the SMLs of 1 mg/kg of food established by the Dutch Commodities Act regulation of 2014 by factors of 10 000 and 8000, respectively. In addition, elevated levels of aluminum were detected in the LFM and DFM samples, which were
and in the dried pellet form (26 elements), compared with the LAE sample, where only one element in solution and nine elements in the dried pellet form were identified. Toxic elem- ents exclusively detected in AFM include chromium, cobalt, barium, lead, and cadmium. This trend is similar to that ob- served in the LFM samples, where nine elements were found in the solution and 15 elements were found in the dried pel- lets, in contrast to the corresponding LAE samples. Beryllium, manganese, and molybdenum were exclusively detected in LFM. In addition, more elements were detected in AFM than in the LFM samples regardless of the form of the ana- lyzed samples. Elements, such as lanthanum, cerium, praseo- dymium, neodymium, samarium, dysprosium, and uranium, were exclusively detected in AFM. The concentrations of elements were consistently higher in the AFM and LFM samples than in the LAE samples, irre- spective of their physical form. These elements include lithium, aluminum, magnesium, manganese, iron, zinc, copper, stron- tium, and barium. Specifically, these elements were only de- tected in the dried pellet form of the LAE samples and not in the diluted solution. Furthermore, element migration to AFM generally exhibited higher quantities compared with that to LFM. For instance, the concentrations of lithium, alu- minum, calcium, strontium, barium, and lead were at least 3.5 times higher in the AFM samples than in the LFM samples. Particularly noteworthy are calcium and strontium, which were detected at concentrations 21 and 27.5 times higher in AFM, respectively, compared with LFM in pellet form. Exceptions to this trend were observed for sodium and mo- lybdenum, whose concentrations were higher in LFM than in AFM. More elements were consistently detected in the dried pellets than in the dissolved solutions for AFM, LFM, and LAE. In many cases, the quantities of elements detected in the pellets were below the LOR of the diluted solutions. For in- stance, cadmium was quantified at 1.47 mg/kg of food simu- lant in the dried pellet of AFM, whereas the LOR in the diluted sample was 4.99 mg/kg of food simulant. Another example is cobalt in LFM samples, which was quantified at 0.99 mg/kg of food simulant in the dried pellet, which is below the LOR of 5.11 mg/kg of food simulant for the diluted solution. The quantities of elements above the LOR in both the dried pellets and the diluted solutions did not present notable differences with respect to the detected amounts regardless of their form. Similar trends to the abovementioned ones are encountered regarding the number of detected elements between the FFM and FE samples. A higher number of elements were detected in the dried pellets of FFM than in those of FE, with 16 and six elements detected, respectively. While six elements were detected in the diluted form of FFM, no elements were de- tected in the diluted form of FE. Magnesium, iron, calcium, strontium, molybdenum, and uranium were exclusively de- tected in FFM. The quantity of elements was, in some cases, higher in the FFM sample regardless of the physical form of the samples; for instance, aluminum, copper, and sodium ex- hibited higher quantities in the FFM sample. Copper, zinc, and barium presented similar quantities in both FFM and FE in both the dried pellet and the dissolved solution form. Similar to the AFM, LFM, and LAE samples, the elements detected in the dried pellets of FFM were often below the LOR of the diluted solutions. This was observed for lithium, vanadium, chromium, manganese, cobalt, nickel, and barium in the FFM samples. Sodium, aluminum, copper, zinc, and
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