Journal of Food Composition and Analysis 106 (2022) 104272 Contents lists available at ScienceDirect Journal of Food Composition and Analysis journal homepage: www.elsevier.com/locate/jfca Original Research Article Occurrence and dietary intake of food processing contaminants (FPCs) in Catalonia, Spain Neus González a, Montse Marquès a, Josep Calderón b, Roger Collantes b, Lidia Corraliza b, Isabel Timoner c, Jaume Bosch c, Victòria Castell c, José L. Domingo a, Martí Nadal a, * a Laboratory of Toxicology and Environmental Health, School of Medicine, IISPV, Universitat Rovira i Virgili, Sant Llorenç 21, 43201, Reus, Catalonia, Spain b Laboratory of the Public Health Agency of Barcelona, Chemistry, Avda. Drassanes 13-15, 08001, Barcelona, Catalonia, Spain c Catalan Food Safety Agency, Department of Health, Generalitat de Catalunya, Roc Boronat 81-95, 08005 Barcelona, Catalonia, Spain A R T I C L E I N F O A B S T R A C T Keywords: Food processing contaminants (FPCs) form a wide group of chemicals that are generated during different cooking Food processing contaminants practices. This study was aimed at determining the levels of a number of FPCs (i.e., acrylamide, furans, mono­ Acrylamide chloropropanediols (MCPDs) and glycidyl esters (GEs)) in foodstuffs purchased in Catalonia (Spain), and Furan assessing the human exposure for different population groups. The dietary intake of acrylamide for the adult Monochloropropanediols Glycidyl esters population was estimated in 2.91 μg/day, while that of furan, 2-methylfurans and 3-methylfurans was 4.32, 7.35 Risk assessment and 0.439 μg/day, respectively. Finally, the exposure to 3-MCPD, 2-MCPD, 3-MCPD esters, 2-MCPD esters and Dietary exposure GEs through food consumption was estimated in 0.657, 0.529, 10.7, 5.15 and 8.81 μg/day, respectively. The risk Food composition assessment showed that there is a health concern for developing neoplastic effects derived from the intake of Food analysis acrylamide for all the population groups. In addition, toddlers and infants would exceed the threshold values of 3-MCDP and GEs. The global analysis of these results indicates that a special attention should be paid to the youngest population groups in Catalonia, reinforcing the need of conducting periodical monitoring studies and developing policy measures, especially focused on foodstuffs highly consumed by toddlers, infants and children. 1. Introduction breads or biscuits, among others (Tareke et al., 2002; Deribew and Woldegiorgis, 2021). The toxicological effects of acrylamide include Food processing contaminants (FPCs) include a wide range of com­ neurotoxicity, genotoxicity and reproductive toxicity (EFSA, 2015). pounds that can be formed during cooking practices (Mogol and Therefore, the International Agency for Research on Cancer (IARC) Gökmen, 2016). Heating treatment is by far the most widely method for classified acrylamide as a probably carcinogenic to humans (Group 2A) food process in the industry or at home, covering up to 80–90 % of the (IARC, 1994). consumed food (Nerín et al., 2016). This group of chemicals include a MCPDs are formed by the reaction of lipids and chlorines at high variety of toxicants, such as acrylamide, furans and mono­ temperatures, mainly during the deodorization process (Nguyen and chloropropanediols (MCPDs), with different physico-chemical and Fromberg, 2020). In the late 1970s, 2- and 3-MCPDs were identified in toxicological properties. Their consumption has been also linked to the composition of hydrolyzed vegetable protein (HVP), which is used as adverse health effects (Kettlitz et al., 2019), although accurate exposure a flavoring condiment (EFSA, 2016). However, the presence of MCPDs in estimates for FPCs may be particularly challenging (Rietjens et al., foodstuffs was firstly observed in 2004 (Svejkovská et al., 2004), while 2018). their occurrence in edible oils and soy/oyster sauces was reported Acrylamide is formed during heating processes above 120 ◦ C, when shortly after (Wong et al., 2006; Zelinková et al., 2006). In turn, as the free asparagines react with reducing sugars, such as glucose and fruc­ presence of chlorinated compounds is not required, glycidol can be also tose, according to the Maillard reaction (Mesías and Morales, 2016; Abt formed by different routes, but under the same conditions as MCPDs et al., 2019; Rifai and Saleh, 2020). Acrylamide has been found to be (FAO/WHO, 2017; Nguyen and Fromberg, 2020). The IARC classified contained in a wide variety of starch-based foods, including potatoes, 3-MCPD as possibly carcinogenic and GEs as probably carcinogenic to * Corresponding author. E-mail address: marti.nadal@urv.cat (M. Nadal). https://doi.org/10.1016/j.jfca.2021.104272 Received 17 June 2021; Received in revised form 5 November 2021; Accepted 8 November 2021 Available online 10 November 2021 0889-1575/© 2021 The Author(s). Published by Elsevier Inc. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/). N. González et al. Journal of Food Composition and Analysis 106 (2022) 104272 humans (Group 2B and 2A, respectively) (IARC, 2013, 2000). cookies, margarine, roasted coffee, instant coffee, baby food, Furan and methylfurans are lipophilic oxygen heterocycles of high cereal-based baby food and breakfast cereals (wheat-based and others). volatility (Kettlitz et al., 2019). They are formed by different pathways, For MCPDs, their content was determined in potato chips, potato snacks, such as degradation of carbohydrates, ascorbic acid and its derivatives sliced bread, toasts and crackers, white bread, cookies, margarine, and thermal oxidation of lipids (Frank et al., 2020). They are detected in sunflower oil, pomace oil, refined olive oil, infant formula, follow-on a wide range of food products including coffee or canned and jarred formulae, cereals and milk, cereal-based baby food, mayonnaise, soy foods, as well as baby food containing meat, vegetables, breakfast ce­ sauce, salad sauce, bakery products, chocolate spreads, palm oil cookies reals or cookies (EFSA, 2017). Based on the reported adverse health and frying oil. Finally, furan and methylfurans was determined in effects derived from the exposure to furans, the IARC classified them as ground coffee, coffee beans, instant coffee, coffee substitutes, fruit jui­ possibly carcinogenic to humans (Group 2B) (IARC, 1995). ces, breakfast cereals, baby food and cereal-based baby food. The aim of this study was to determine the levels of several FPCs in For determining acrylamide and MCPDs, three composites contain­ food products from the Catalan (Spain) market, where these data are ing 8 individual units were prepared for each food group. Since furan currently inexistent. In addition, health risks derived from the con­ and methylfurans are very volatile compounds, instead of composites, 8 sumption of FPC-containing foodstuffs were assessed for various popu­ units of each foodstuff were directly analyzed. Only edible parts of the lation groups. The dietary intakes were compared with toxicological foods were included. Samples were homogenized and stored at -20 ◦ C endpoints in order to establish the potential health risks for the until analysis. consumers. 2.2. Analytical determination 2. Materials and methods The analysis of acrylamide was performed after a water extraction 2.1. Sampling and a clean-up using two types of cartridges. One g of each food was extracted with 10 mL of purified water. Samples were subjected for 30 s Sampling was carried out in three different periods: July 2015, to vortex, 45 min to orbital shaking and finally 20 min to centrifugation September 2016 and September 2019, according to the surveillance at 12,000 rpm and 10 ◦ C. Two mL of the supernatant were then passed program established by the Catalan Food Safety Agency (ACSA). Details through an Oasis HLB cartridge (Waters, Milford, MA, USA). After on the food products purchased in each campaign are given in Table 1. drying, 3 mL of methanol were used to elute the acrylamide, which was In order to get a good representativeness, samples were bought at subsequently cleaned using an Oasis MCX cartridge (Waters, Milford, different markets, supermarkets and grocery stores across Catalonia. MA, USA). The elute was collected in a test tube for evaporation, softly Food products were selected as those containing high levels of the dried under nitrogen at 50 ◦ C for 40 min, and finally redissolved with contaminants assessed in the present study, according to the scientific 400 μL of water. The determination of acrylamide was performed by literature (EFSA, 2017, 2016, 2015). Acrylamide was analyzed in potato UHPLC coupled to a high-resolution mass spectrometer by using a chips, potato snacks, sliced bread, toasts and crackers, white bread, HRMS-Orbitrap q-Exactive system (Thermofisher Scientific, Waltharm, MA, USA). The limit of quantification (LOQ) was defined as the concentration of Table 1 the lowest point of the calibration, being set at 10 μg/kg. A nine-level Food products purchased in the three different sampling periods. calibration curve was established by plotting the average response fac­ Food product July September 2016 September 2019 tor against concentration (μg/L) for each standard level. The recovery 2015 (n = 336) (n = 120) study for the method validation in the range 10.0− 3000 μg/kg of (n = acrylamide showed an accuracy of 101.7 %, with a precision, expressed 264) as percentage of the relative standard deviation (%RSD), of 12.7 %, Potato chips X considering a sample size of N = 58. Quality control/quality assurance Potato snacks X of the analytical procedure was ensured by analyzing spiked samples Sliced bread X and participating in proficiency testing experiments. Toasts and crackers X White bread X The concentration of free MCPD was determined by gas Cookies X X chromatograph-mass spectrometry (GC–MS) using on a previous Margarine X method developed by Wenzl et al. (2015). For the determination of Wheat-based breakfast cereals X 3-MCPD and 2-MCPD, samples were dissolved in n-hexane:acetone Other breakfast cereals X X Roasted coffee X Sigma-Aldrich (St. Louis, MO, USA) (1:1 v/v) and spiked with a surro­ Instant coffee X X gate standard containing d5-3-MCPD and d5-2-MCPD (both from Sunflower oil X Sigma-Aldrich, St. Louis, MO, USA). The supernatant was collected and Pomace oil X water was added, being vortex and the organic phase discarded. The Refined olive oil X aqueous phase was collected and completely evaporated under vacuum Infant formula X Follow-on formulae X and nitrogen. The residue was dissolved in ethyl acetate and the analytes Cereals and milk X were derivatised with phenylboronic acid (Sigma-Aldrich, St. Louis, MO, Cereal-based baby food X X USA). The extract was then evaporated under a nitrogen stream and Mayonnaise X reconstituted with isooctane. GC–MS was carried out on a 7890 A Agi­ Soy sauce X Salad sauce X lent gas chromatograph equipped with a 5977B mass spectrometer Bakery products (milk bread, X (Agilent, Santa Clara, CA, USA). A HP 5 MS capillary column (Agilent) puff pastry and muffins) 30 m ×0.25 mm, 0.25 μm) was used for separation. Helium with a flow Chocolate spreads X of 1.2 mL/min was used. GC oven temperature was programmed from an Palm oil cookies X initial temperature of 60 ◦ C (for 1 min), with 6 ◦ C/min to 150 ◦ C, and Frying oil X Ground coffee X final step up to 300 ◦ C. Characteristic fragment ions of m/z for 3-MCPD Coffee beans X and 2-MCPD were 147 and 196, respectively. The quantitation was Coffee substitutes X performed using the quantifier ions for the selected compounds. The Fruit juices X ratio of the quantifier / qualifier was similar between standards and Baby food X samples, with maximum ranges of 20 %. A six-level calibration curve 2 N. González et al. Journal of Food Composition and Analysis 106 (2022) 104272 was established by plotting the average response factor against con­ methylfuan showed an accuracy of 92.4 %, 88.9 % and 92.6 %, centration (μg/L) for each standard level. The slope and the intercept respectively, while precision results were 9.3 %, 8.2 % and 15 %, were calculated by linear regression for each analyte. The recovery respectively. study for the method validation between 10 and 100 μg/kg showed an accuracy of 91.5 % for 3-MCDP (N = 58) and 86.2 % for 2-MCPD (N = 65), while precision results were 12.6 % and 10.5 %, respectively. 2.3. Dietary exposure Ester bound MCPD and glycidyl esters in food samples were analyzed by means of Gas Chromatography – Triple quadrupole Mass Spectrom­ Consumption data for the analyzed foodstuffs were obtained from etry (GC–MS/MS). Fat from infant or nutritional formulas was extracted ENALIA and ENALIA2, which are the most recent consumption surveys by liquid-liquid extraction using ethyl acetate. Fat from the rest of the performed in Spain. ENALIA covers data for infants and adolescents, samples was extracted by Accelerated Solvent Extraction (ASE) using while ENALIA2 includes data for the adult population and pregnant tertbutylmethylether (Sigma-Aldrich, St. Louis, MO, USA). The extrac­ women (AECOSAN, 2016a, b). These surveys were performed by ted fat and oil samples were analyzed for bound MCPD and Glycidyl following the recommendations guide developed by EFSA (2009). They esters (GE) following the AOCS (2013) official method CD29a-13. GE are consumption data studies representative of different Spanish sub­ were converted to 3-monobromopropanediol (3-MBPD) monoesters in populations, which are based on a random selection of 1862 children an acid solution containing a bromide salt. 3-MBPD esters, together with and adolescents, 623 adults, 310 seniors, and 157 pregnant women. The 2- and 3-MCPD esters, were then converted into the free (nonesterified) method included a 24-h recall in two non-consecutive days (at least 14 form in an acid methanolic solution. The fatty acid methyl esters days in between) and a food frequency questionnaire. For coffee, a generated during the reaction were extracted from the sample, and special assumption was made, taking into consideration that three 2-MCPD, 3-MCPD, and 3-MBPD were derivatized with phenylboronic different types of coffee (roasted, ground and beans) were analyzed but acid (Sigma-Aldrich, St. Louis, MO, USA) prior to GC-tandem MS only consumption data on “liquid coffee” is available. Therefore, the (GC–MS/MS) analysis. GC–MS/MS was carried out on a 7890B Agilent consumption of each type of coffee was assumed as 1/3 of the total for gas chromatograph equipped with a 7010B mass spectrometer triple the “liquid coffee”. quadrupole detector (Agilent, Santa Clara, CA, USA). A HP 5 MS capil­ The population under study was divided into 7 groups according to lary column (30 m ×0.25 mm, 0.25 μm) (Agilent, Santa Clara, CA, USA) age: toddlers (6–11 months), infants (1–3 years), children (3–9 years), was used for separation. Helium was used as carrier gas with a flow of 16 adolescents (10–17 years), young adults (18− 39 years), adults (40− 64 psi. GC oven temperature was programmed from an initial temperature years), seniors (65− 74 years). The age bands were selected according to of 60 ◦ C (for 1 min), 10 ◦ C/min up to 200 ◦ C, and finally at 25 ◦ C/min up the ENALIA surveys (AECOSAN, 2016a, b). The total exposure to to 250 ◦ C. Quantitative analysis was carried out by monitoring the acrylamide, free- and ester-bound-MCPDs, GEs and furan and methyl­ transitions specified in previous studies (Dubois et al., 2019; Wenzl furans was calculated by multiplying the concentration of each chemical et al., 2015). in food and the average consumption of that food. The total dietary The LOQ was set at 2.0 μg/kg for infant formula, and 50 μg/kg for the intake of each compound was finally obtained by summing the respec­ rest of food commodities. Quantification was performed using the tive intakes from each food group. quantifier ions for the selected compounds. A ten-level calibration curve Finally, the intake was also estimated according to the respective was established by plotting the average response factor against con­ average body weight (bw) of each population group, whose values were centration (μg/L) for each standard level. The slope and the intercept gathered from the scientific literature (Carrascosa et al., 2010; were calculated by linear regression for each analyte. The recovery López-Sobaler et al., 2016; Martínez et al., 2017; WHO, 2003). For study for the method validation was conducted in the range 2.0− 35 μg/ calculation purposes, mean body weights of 8.4, 12.3, 24, 51, 72, 77, kg for infant formula, and between 50 and 1000 μg/kg for the rest of 70.5 and 65 kg were used for toddlers, infants, children, adolescents, food commodities. Bound 3-MCPD, bound 2-MCPD and glycidil esters adults aged 18− 39, adults aged 40− 64, seniors, and pregnant women, showed an accuracy of 97.8 % (N = 16), 96.3 % (N = 16) and 104.8 % (N respectively. When estimating the dietary intake, for those chemicals = 16), respectively, being precision results 11.9 %, 10.3 % and 11.7 % with levels under their respective limit of detection (LOD), their con­ respectively. Quality control/quality assurance of the analytical pro­ centration was assumed equal to one-half of the LOD (medium-bound; cedure was ensured by analyzing spiked samples and participating in MB). The dietary exposure was also calculated under 2 additional sce­ proficiency testing experiments. narios: upper-bound (UB) and lower-bound (LB). To estimate the UB and For the furan determination, food samples were analyzed using Head LB exposures, the values corresponding to the highest and lowest con­ Space (HS) gas chromatography–mass spectrometry (GC–MS) with centrations were used, respectively. When a chemical was under their isotope dilution. The HS method applied was based on the FDA (2004) respective LOD, their concentration was assumed as the LOD, under the method. One-half gram of sample was weighted into a 20 mL HS vial, UB scenario, or 0, under the LB scenario. Furthermore, for the exposure and 10 mL of a 30 % sodium chloride solution were added. For coffee, assessment of acrylamide, furan and methylfurans, specific dilution and 0.25 g of sample and 10 mL of water were used. Fifty μL of a d4-furan loss factors were applied to coffee (Becalski et al., 2016). For acryl­ solution internal standard (Sigma-Aldrich, St. Louis, MO, USA) was amide, a dilution factor of 19.6 was considered because non-brewed used, being added to the HS vial before capping it. The extraction into coffee was analyzed. In turn, for furan the following reduction (dilu­ the HS was done for 20 min at 50 ◦ C before injecting it the the GC. The tion + loss) factors, related to coffee brewing, were applied: 26.8 for determination was done with an Agilent HeadSpace (7697A, Agilent), furan, 47 for 2-methylfuran and 46 for 3-methylfuran. GC (Agilent 7890) and a MS (Agilent 5977) (Agilent, Santa Clara, CA, USA). The GC column used was a HP-Plot/Q (15 m x0.32 mm; id 20 μm film). Ions for furan (m/z 68 and 39) and methylfurans (m/z 82 and 53) 2.4. Risk characterization were monitored, being target compounds quantified with external calibration curves. Two different approaches for the risk characterization were used in The LOQ for baby foods and juices was determined at 5 μg/kg, while the present study. The first one consisted of the comparison of the that for the remaining foodstuffs was 20 μg/kg. A seven-level calibration estimated daily intake (EDI) with the tolerable daily intake (TDI). curve was established by plotting the average response factor against However, this approach is not valid for carcinogenic substances because concentration (in ng per vial) for each standard level. The slope and the there cannot be threshold values associated to cancer effects. In that intercept were calculated by linear regression for each analyte. The re­ case, the margin of exposure (MOE) approach was used by applying this covery study for the method validation of furan, 2-methylfuran and 3- equation: 3 N. González et al. Journal of Food Composition and Analysis 106 (2022) 104272 BMDL10 orT25 European Commission. (2013). The results found in this study are in MOE = EDI accordance to those reported in the literature for a number of countries. For instant coffee, the levels observed in Catalonia are very similar to Where BMDL10 is the 95 % lower confidence limit for this benchmark those reported by Arisseto et al. (2007) in Brazil (582 μg/kg), while dose for 10 % extra risk of carcinogenic effects, T25 is the dose corre­ values for roasted coffee are also similar to those previously found in the sponding to a 25 % incidence of tumors, and EDI is the estimated daily USA (272.4 μg/kg) (Abt et al., 2019). For potato chips, our results are intake. also in the same order of magnitude than those observed in Colombia, USA, Brazil and North Macedonia (635, 498, 591 and 390 μg/kg, 3. Results and discussion respectively) (Abt et al., 2019; Arisseto et al., 2007; Barón Cortés et al., 2021; Dimitrieska-Stojkovikj et al., 2019), but notably lower than values 3.1. Concentrations of FPCs from Lebanon (Hariri et al., 2015). The food levels of acrylamide were also lower than those reported in a number of food products (e.g., salted The mean concentrations of the nine food processing contaminants snacks, biscuits and wafers, breakfast cereals, coffee and toasts and here analyzed in a number of foodstuffs are summarized in Table 2. bread) purchased in Slovenia (Mencin et al., 2020). Similarly, mean Instant coffee showed the highest concentrations of acrylamide (594 μg/ levels in potato chips and snacks (range: 243− 435 μg/kg) were also kg), followed by potato chips and potato snacks (435 and 243 μg/kg, lower than (but of the same order of magnitude as) the values reported respectively). Relatively high levels of acrylamide were also noted in by Mesías et al. (2020) in Spain (664 μg/kg). In a previous study, these cookies and roasted coffee (209 and 202 μg/kg, respectively). None of researchers found an average acrylamide content of 630 μg/kg in the foodstuffs exceeded the recommended limits established by the commercial potato crisps (Mesías and Morales, 2015). In addition, Table 2 Concentrations of FPCs (μg/kg) in different foodstuffs purchased from Catalonia (Spain). Food samples Acrylamide Furan 2- 3- 3-MCPD 2-MCPD 3-MCPD 2-MCPD GE methylfurans methylfurans ester ester Potato chips (n = 24) 435 ± 110 n.a. n.a. n.a. <10 <10 102 ± 40 50.7 ± 25 68 ± 5.3 Potato snacks (n = 24) 243 ± 140 n.a. n.a. n.a. <10 <10 389 ± 190 152 ± 69 138 ± 44 Sliced bread (n = 24) 14.7 ± 4.2 n.a. n.a. n.a. 15.1 ± 1.5 <10 21 ± 9.2 5±2 1 ± 1.7 Toasts and crackers (n = 24) 43.4 ± 17 n.a. n.a. n.a. 4.67 ± <10 68.3 ± 37 24.3 ± 24 61.7 ± 31 0.58 White bread (n = 24) 9.6 ± 8 n.a. n.a. n.a. 4.87 ± <10 0.67 ± 1.2 1±1 3±0 0.23 Breakfast cereals (wheat) (n = 86 ± 21 n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. 24) Breakfast cereals (other) (n = 59.7 ± 6 n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. 24) Roasted coffee (n = 24) 202 ± 76 n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. Instant coffee* 594 ± 160 380 ± 330 869 ± 640 62.1 ± 40 n.a. n.a. n.a. n.a. n.a. Margarine (n = 24) <40 n.a. n.a. n.a. <20 <20 287 ± 38 174 ± 32 294 ± 160 Cereal-based baby food* 11.3 ± 3.1 4.70 ± 6.5 2.65 ± 1.4 <1 <10 <10 2.33 ± 1.5 1.17 ± 0.76 <1 Cookies (n = 24) 209 ± 49 n.a. n.a. n.a. 4.47 ± 0.7 <10 191 ± 95 91.3 ± 42 305 ± 110 Baby food* 9.27 ± 6.9 1.13 ± <1 <1 n.a. n.a. n.a. n.a. n.a. 0.36 Ground coffee (n = 8) n.a. 1670 ± 5210 ± 1100 261 ± 32 n.a. n.a. n.a. n.a. n.a. 170 Coffee beans (n = 8) n.a. 2410 ± 7130 ± 1100 373 ± 29 n.a. n.a. n.a. n.a. n.a. 260 Coffee substitutes (n = 8) n.a. 257 ± 190 380 ± 230 12.6 ± 8.5 n.a. n.a. n.a. n.a. n.a. Fruit juices (n = 8) n.a. <1 <1 <1 n.a. n.a. n.a. n.a. n.a. Breakfast cereals (n = 8) n.a. 21.6 ± 29 8.13 ± 9.6 1.26 ± 0.73 n.a. n.a. n.a. n.a. n.a. Sunflower oil (n = 24) n.a. n.a. n.a. n.a. <10 <10 617 ± 190 321 ± 100 407 ± 140 Pomace oil (n = 24) n.a. n.a. n.a. n.a. <10 <10 2270 ± 210 733 ± 220 737 ± 400 Refined olive oil (n = 24) n.a. n.a. n.a. n.a. <10 <10 397 ± 210 198 ± 130 267 ± 29 Infant formula (n = 24) n.a. n.a. n.a. n.a. <10 <10 304 ± 180 101 ± 61 <68 Follow-on formulae (n = 24) n.a. n.a. n.a. n.a. <10 <10 171 ± 120 73 ± 36 <54 Cereals and milk (n = 24) n.a. n.a. n.a. n.a. <20 <20 <6 1.83 ± 1.3 <7 Mayonnaise (n = 24) n.a. n.a. n.a. n.a. 34.1 ± 20 5.7 ± 245 ± 96 102 ± 47 246 ± 37 0.58 Soy sauce (n = 24) n.a. n.a. n.a. n.a. 18.8 ± 7.6 46 ± 71 n.a. n.a. n.a. Salad sauce (n = 24) n.a. n.a. n.a. n.a. 12.3 ± 1.2 12.3 ± 229 ± 130 97.3 ± 58 95.3 ± 21 1.2 Bakery products (n = 24) n.a. n.a. n.a. n.a. 7.23 ± 3.9 <10 388 ± 310 107 ± 110 265 ± 380 Chocolate spreads (n = 24) n.a. n.a. n.a. n.a. <10 <10 457 ± 160 207 ± 49 617 ± 140 Palm oil cookies (n = 24) n.a. n.a. n.a. n.a. 4.50 ± <10 297 ± 15 114 ± 13 343 ± 15 0.87 Frying oil (mixture) (n = 24) n.a. n.a. n.a. n.a. n.a. n.a. 727 ± 58 313 ± 32 700 ± 53 n.a.: not analyzed; *different number of analyzed samples, depending on the target chemicals: n = 24 for acrylamide, 3-MCPD, 2-MCPD, 3-MCPD ester, 2-MCPD ester and GE, and n = 8 for furan, 2-methylfutran and 3-methylfuran. 4 N. González et al. Journal of Food Composition and Analysis 106 (2022) 104272 cookies contained comparable levels of acrylamide to those reported in Table 3 the USA or North Macedonia (181.8 and 231 μg/kg, respectively) (Abt Dietary intake of acrylamide by the adult population of Catalonia (Spain). et al., 2019; Dimitrieska-Stojkovikj et al., 2019), but lower levels in Food samples Consumption (g) Exposure (μg/day) cookies marketed in Spain (423 μg/kg) (Rufian-Henares et al., 2007). In Potato chips 0.46 0.198 (7) 2015, EFSA released an opinion on acrylamide in food, indicating that Potato snacks 0.46 0.111 (4) higher levels are found in coffee and potato-based products, as well as Sliced bread 11.4 0.167 (6) biscuits and cereals, which could also contain notable levels of acryl­ Toasts and crackers 0.64 0.028 (1) amide. Moreover, EFSA (2015) reported low levels in baby food, in White bread 62.3 0.311 (11) Breakfast cereals (wheat) 1.31 0.113 (4) agreement to the findings here presented. Breakfast cereals (other) 0.98 0.058 (2) The highest levels of furan, 2-methylfurans and 3-methylfurans were Roasted coffee 27.2 0.280 (10) found in coffee beans (2410, 7130 and 373 μg/kg, respectively). In Soluble coffee 0.17 0.101 (3) general, the levels of 2-methylfuran in all the foodstuffs were higher Margarine 0.85 0.017 (1) Baby cereals n.d n.d than those of furan and 3-methylfuran. Kettlitz et al. (2019) had previ­ Cookies 7.31 1.53 (53) ously observed that 2-methylfuran was the contaminant with the highest Baby food n.d n.d concentrations in ground coffee (18,300 μg/kg), being followed by furan TOTAL 113 2.91 and 3-methyfuran (3140 and 690 μg/kg, respectively). Moreover, n.d.: not determined. In brackets, contribution percentage of each food sample instant coffee followed the same pattern (4030, 730 and 210 μg/kg for to total exposure. 2-methylfuran, furan and 3-methylfuran, respectively). Finally, the levels of furans in breakfast cereals from Catalonia are similar to those previously found by Kettlitz et al. (2019) (21.6 vs. 27 μg/kg). However, Table 4 our results are, in general, notably lower than those typically found in Dietary intake of furan, 2-methylfurans and 3-methylfurans by the adult popu­ the scientific literature. Thus, furan mean levels reported by EFSA lation of Catalonia (Spain). (2017) were higher in coffee beans (4580 vs 2410 μg/kg) and ground Exposure (μg/day) coffee (2360 vs 1670 μg/kg), but similar in instant coffee (310 vs 380 Food samples Consumption (g) Furan 2- 3- μg/kg). In turn, lower concentrations (range: 20–57 μg/kg) were found methylfurans methylfurans in other types of food, such as breakfast cereals, ready-to-eat meals for Soluble coffee 0.17 0.065 0.148 (2) 0.011 (3) infants or bread and rolls, among others (EFSA, 2017). (2) Mayonnaise showed the highest concentration of 3-MCPD (34.1 μg/ Cereal-based n.d n.d n.d n.d kg), while salad sauce presented the greatest levels of 2-MCPD (12.3 μg/ baby food kg). Regarding ester-bound MCPDs, pomace oil was the food item Baby food n.d n.d n.d n.d Ground coffee 27.2 1.69 3.01 (41) 0.154 (35) showing the highest levels of 3-MCPD and 2-MCPD esters (2270 and 733 (39) μg/kg, respectively). Accordingly, pomace oil also showed the highest Coffee beans 27.2 2.44 4.12 (56) 0.220 (50) concentrations of GEs (737 μg/kg). Infant and follow-on formulae also (57) contained notable levels of 3-MCPD and 2-MCPD esters. Results for es­ Coffee n.d. n.d n.d n.d ters in refined oils are lower than those found in commercialized sam­ substitutes Fruit juices 49.6 0.05 (1) 0.050 (1) 0.050 (11) ples of extra virgin olive oils, olive oils and oil blends (Kamikata et al., Breakfast cereals 3.26 0.07 (2) 0.027 (0) 0.004 (1) 2018), where levels of 3-MCPD, 2-MCPD esters and glycidyl ester were TOTAL 107 4.32 7.36 0.439 as high as 3770, 1910 and 1600 μg/kg, respectively. In another study n.d.: not determined. In brackets, contribution percentage of each food sample conducted in China, Zhang et al. (2020) analyzed the presence of 3- and to total exposure. 2-MCPD esters in vegetable oils and related products. Vegetable oils contained 3-MCPD and 2-MCPD esters values of 760 and 330 μg/kg, respectively, being similar to those found in the present study for sun­ estimated in 2.91 μg/day (0.042 μg/kg bw/day, considering a body flower oil (617 and 321 μg/kg, respectively). In samples of the USA, weight of 70 kg), being cookies the main contributor (53 %). Because of Beekman et al. (2019) found higher concentrations of 3-MCPD esters its high consumption (62.3 g/day), the second most important contri­ and GEs in refined olive oil (560 and 480 μg/kg, respectively), and bution corresponded to white bread (11 %) (Table 3). The mean dietary similar levels in sunflower oil (550 and 390 μg/kg, respectively) than the intakes of furan, 2-methylfurans and 3-methylfurans by the adults was concentrations observed here. calculated in 4.32, 7.36 and 0.439 μg/day (0.0617, 0.105 and 0.0063 In contrast to other foodstuffs, the levels of MCDPs and GEs in infant μg/kg bw/day), respectively. For the three contaminants, coffee (beans formulas from Catalonia were higher than those found in Denmark, + ground) was the main contributor, with exposure percentage ranges where concentration ranges were the following: 2-MCPD esters: 1.3–29 between 85 % and 97 % of the total exposure to furans (Table 4). In μg/kg; 3-MCPD esters: 8.6–65 μg/kg; GEs: 3.1–32 μg/kg (Nguyen and relation to MCPDs, the mean dietary exposure was found to be 0.657, Fromberg, 2020). They were also higher than the concentrations of 0.529, 10.7, 5.15 and 8.81 μg/day for 3-MCPD, 2-MCPD, 3-MCPD esters, 2-MCPD and 3-MCPD in infant formula from the Canadian market, 2-MCPD esters and GEs, respectively (Table 5). Considering a body where maximum values of 47 and 89 μg/kg, respectively, were reported weight of 70 kg, these values would mean an exposure of 0.0094, in samples collected in 2013 (Becalski et al., 2015). However, the con­ 0.0076, 0.153, 0.074 and 0.126 μg/kg bw/day, respectively. White centrations are within the same range of magnitude than those found in bread was the greatest contributor to the intake of free 3- and 2-MCPDs other countries, such as the USA (3-MCPD esters: 93–620 μg/kg; GE: (46 % and 58 %, respectively), due to the high consumption associated 8–360 μg/kg) (Beekman et al., 2020) and the Czech Republic (3-MCPD to this food item (62.3 g/day). In turn, the greatest contribution of the esters: 62–588 μg/kg) (Zelinková et al., 2009). ester-bound MCPDs and GEs corresponded to refined olive oil (range: 48 %–60 %), which is a highly consumed food item in the Mediterranean diet (15.7 g/day). 3.2. Dietary intake of FPC Data on the exposure assessment of the current study were compared to those reported in the literature. For acrylamide, our results were The estimated mean dietary intake of acrylamide, furan, 2-methyl­ lower than those observed in Japan (Kito et al., 2020), where an expo­ furan, 3-methylfuran, 3-MCPD, 2-MCPD, ester-bound 3- and 2-MCPDs sure for the adult population of 0.15 μg/kg bw/day was reported. and GEs by the adult population (18–74 years) of Catalonia is summa­ Moreover, higher intakes were also found in the USA (0.36 μg/kg rized in Tables 3–5. The mean dietary exposure of acrylamide was 5 N. González et al. Journal of Food Composition and Analysis 106 (2022) 104272 Table 5 Dietary intake of 3-MCPD, 2-MCPD, 3-MCPD and 2-MCPD esters and GEs by the adult population of Catalonia (Spain). Exposure (μg/day) Food samples Consumption (g) 3-MCPD 2-MCPD 3-MCPD esters 2-MCPD esters GE Potato chips 0.46 0.00228 (0.4) 0.00228 (0.4) 0.0464 (0.43) 0.0230 (0.4) 0.0309 (0.4) Potato snacks 0.46 0.00228 (0.4) 0.00228 (0.4) 0.177 (2) 0.0690 (1.3) 0.0628 (0.7) Sliced bread 11.4 0.172 (26) 0.0570 (11) 0.239 (2.22) 0.0570 (1.1) 0.0114 (0.1) Toasts and crackers 0.64 0.00299 (0.5) 0.00320 (0.6) 0.0437 (0.4) 0.0156 (0.3) 0.0395 (0.4) White bread 62.3 0.303 (46) 0.311 (58) 0.0415 (0.4) 0.0623 (1.2) 0.187 (2) Margarine 0.85 0.00850 (1.3) 0.00850 (1.6) 0.244 (2.3) 0.148 (3) 0.250 (3) Cereal-based baby food n.d n.d n.d n.d n.d n.d Cookies 7.31 0.0327 (5) 0.0366 (6.9) 1.39 (13) 0.668 (13) 2.23 (25) Sunflower oil 1.82 0.00910 (1.4) 0.00910 (2) 1.12 (10) 0.585 (11) 0.740 (8.4) Pomace oil n.d. n.d n.d n.d n.d n.d Refined olive oil 15.7 0.0785 (12) 0.0785 (15) 6.22 (58) 3.11 (60) 4.18 (48) Infant formula n.d. n.d n.d n.d n.d n.d Follow-on formulae n.d. n.d n.d n.d n.d n.d Cereals and milk n.d. n.d n.d n.d n.d n.d Mayonnaise n.d. 0.0273 (4.2) 0.00456 (0.85) 0.196 (1.83) 0.0819 (2) 0.197 (2) Soy sauce 0.8 0.00128 (0.2) 0.00313 (0.59) n.d n.d n.d Salad sauce 0.068 0.00037 (0.1) 0.00037 (0.06) 0.00687 (0.1) 0.00292 (0.1) 0.00286 (0.03) Bakery products 0.03 0.0132 (2) 0.00910 (2) 0.707 (6.6) 0.195 (4) 0.482 (5.5) Chocolate spreads 1.82 0.00320 (0.5) 0.00320 (0.6) 0.292 (2.72) 0.132 (2.6) 0.395 (4.5) Palm oil cookies 0.64 n.d n.d n.d n.d n.d Frying oil (mixture) n.d. n.d n.d n.d n.d n.d TOTAL 104 0.657 0.529 10.7 5.15 8.81 n.d.: not determined. In brackets, contribution percentage of each food sample to total exposure. bw/day) and in North Macedonia (0.643 μg/kg bw/day) (Abt et al., 2019; Dimitrieska-Stojkovikj et al., 2019). The estimated intake of acrylamide by the Catalan adult population (2.91 μg/day) was notably lower than the estimated values reported in other Spanish regions (range: 15.3–18.7 μg/day), according to Freisling et al. (2013). More­ over, it was lower than the dietary intake by Spanish women (0.3 μg/kg bw/day) given by Obón-Santacana et al. (2014), who estimated a value of 0.3 μg/kg bw/day (equivalent to 18 μg/day for a 60 kg-body weight woman). Finally, the intake was similar to the values found by Mesías and Morales (2015), considering only the consumption of potatoes (0.035 μg/kg bw/day). Regarding furans, the estimated exposure in the current study was well below that reported in Austria (range: 0.312 – 0.498 μg/kg bw/day) (Mayerhofer et al., 2019) and Belgium (0.38 μg/kg bw/day) (Scholl Fig. 1. Dietary intake of acrylamide for several population groups living in et al., 2012). In Canada, the average furan and total furan (including 2- Catalonia (Spain). and 3-methylfuran) intakes by adults (≤20 years) were estimated at approximately 0.37 and 0.71 μg/kg bw/day (Becalski et al., 2010). In China, Zhang et al. (2020) analyzed the content of MCPDs in vegetable oils and related products from Zhejiang market. They esti­ mated a dietary exposure of 3-MCPD esters and 2-MCPD esters of 0.62 and 0.26 μg/kg bw/day, respectively, which are notably higher than those here found. Also in China, Li et al. (2015) estimated the 3-MCPD esters exposure levels for the adult population (18–49 years), which was estimated in 0.71 μg/kg bw/day. Our results are also lower than those found by Chung et al. (2013) in Hong Kong (range: 0.20− 0.53 μg/kg bw/day). As for free MCPDs, our levels are notably lower than those found in Brazil (range: 0.06− 0.51 μg/kg bw/day) and in the Netherlands (0.674 μg/kg bw/day) (Arisseto et al., 2013; Boon and Te Biesebeek, 2016). The dietary intake of acrylamide, furans and MCPDs for different Fig. 2. Dietary intake of furan, 2-methylfurans and 3-methylfurans for several population groups are depicted in Figs. 1–3. Children aged 3–9 years population groups living in Catalonia (Spain). presented the highest exposure level of acrylamide (5.41 μg/day). However, taking into account the body weight, toddlers (6–11 months) groups (toddlers, infants, children and adolescents), among these three were the most exposed group (0.405 μg/kg bw/day). For all the age contaminants, furan was the most important contributor in comparison groups, the highest contribution to acrylamide corresponded to cookies, to 2-methylfurans and 3-methylfurans, with ranges of 45 %–63 %. In with the only exception of toddlers, whose main contributor was turn, adults and senior people presented a higher intake of 2-methylfur­ breakfast cereals. ans than that of furan and 3-methylfurans (Fig. 2). For the latter popu­ The adult population (40–64 years) was the group showing the lation groups, 2-methylfurans meant 72 % of the total exposure to highest exposure to furan, 2-methylfurans and 3-methylfurans (5.33, furans. Breakfast cereals were the main contributor to furan exposure for 15.9 and 0.856 μg/day, respectively). For the youngest population the young population groups (toddlers, infants, children and 6 N. González et al. Journal of Food Composition and Analysis 106 (2022) 104272 acrylamide for toddlers, infants, children and adolescents ranged be­ tween 0.65 and 1.70 μg/kg bw/day, while for young adults, adults, se­ niors and pregnant women, the range was between 0.15 and 0.23 μg/kg bw/day. For furan, the exposure of the youngest population (toddlers, infants, children and adolescents) was estimated in 0.034− 0.32 μg/kg bw/day, while the intake for the adults was between 0.17 and 0.22 μg/ kg bw/day. The daily exposure to 2-methylfuran and 3-methylfuran for the youngest people ranged 0.018− 0.17 and 0.010− 0.089 μg/kg bw/ day, respectively, while for the older groups, these values were within the range 0.048− 0.63 μg/kg bw/day, for 2-methylfuran, and 0.030− 0.036 μg/kg bw/day, for 3-methylfuran. Finally, the exposure Fig. 3. Dietary intake of 3-MCPD, 2-MCPD, 3-MCPD and 2-MCPD esters and ranges of 3-MCPD, 2-MCPD, 3-MCPD ester, 2-MCPD ester, and GE were GEs for several population groups living in Catalonia (Spain). 0.078− 0.15, 0.057− 0.14, 1.40–4.42, 0.64–2.06, and 1.40–2.81 μg/kg bw/day, respectively, for the youngest groups, and 0.029− 0.040, adolescents), while the greatest intake of furan by adults and seniors 0.022− 0.028, 0.50− 0.59, 0.24− 0.28, and 0.42− 0.50 μg/kg bw/day, corresponded to coffee beans. Regarding 2-methylfurans, the intake respectively, for the adults. In all the cases, the P95 of the dietary intake pattern was different according to the age. The foodstuffs with the of FPC were lower than typical intake data reported by EFSA (2015, highest contribution were breakfast cereals in toddlers and infants, fruit 2016, 2017). juices in children and adolescents, and coffee beans in adults, seniors and pregnant women. The food pattern was more varied for 3-methyl­ 3.3. Health risk assessment furans. Toddlers were primarily exposed to this contaminant through baby food consumption, while fruit juices were the main intake of 3- In order to be compared with threshold values, either MOE or TDI methylfurans in infants, children and adolescents. As for most FPCs, (Table 7), data on dietary intake according to the body weight were coffee beans were the main contributors to exposure of 3-methylfurans considered. For acrylamide, the risk characterization for neoplastic ef­ for adult groups. fects was derived from the BMDL10 of 170 μg/kg bw/day, taken from Adolescents (10–17 years old) and children (3–9 years old) were the data on Harderian gland adenomas and adenocarcinomas in mice. The most exposed groups for the MCPDs and GEs, respectively (34.6 μg/day CONTAM Panel established that a MOE of 10,000 or higher would be of for both). The chemical profile was dominated by 3-MCPD, with a low concern for the public health. On the other hand, the BMDL10 value contribution range to total exposure of 40 %–55 %. In contrast, free 3- of 430 μg/kg bw/day was used to perform the risk characterization for and 2-MCPDs were the contaminants showing the lowest levels of non-neoplastic effects (neurotoxicity). In this case, a MOE of 100 or exposure (Fig. 3). For free MCPDs, follow-on formula was the food item higher is considered sufficient to conclude that there is no health mainly contributing to their exposure in toddlers and infants, due to concern (EFSA, 2015). In the present study, none of the population their high consumption. On the other hand, white bread was the main groups was at risk of suffering non-neoplastic effects, being all MOEs contributor for adolescents, adults and seniors, as well as pregnant above 100 for the three scenarios considered (UB, MB and LB). However, women. Ester-bound MCPDs followed a similar pattern in young popu­ the MOEs for all the population groups (except seniors and adults be­ lation groups, with the main contribution corresponding to follow-on tween 40 and 64 years) were below 10,000 for the neoplastic effects; formula consumed by toddlers and infants. By contrast, refined olive therefore, there would be a health concern for that type of effects oil was the food product with the highest contribution to exposure of derived from the exposure to acrylamide. In addition, under the UB, all ester-bound MCPDs in the remaining population groups. Finally, tod­ the population groups were below 10,000, indicating a health risk for dlers, young adults, adults, seniors and pregnant women, were mainly neoplastic effects. In fact, some studies have observed an increased risk exposed to GEs through refined olive oil consumption, while infants, of suffering some specific types of cancer (endometrial and ovarian), children and adolescents were mostly exposed through cookies when the exposure to acrylamide overcomes 20 μg/day, while no as­ consumption. sociation is found with some of the common types of cancers (Adani The 95th percentile (P95) of the FPC dietary intake by the Catalan et al., 2020; Pelucchi et al., 2014). population is summarized in Table 6. The estimated exposure of Regarding furan, the CONTAM Panel selected the BMDL10 of 64 μg/ Table 6 Mean and P95 exposure to acrylamide, furans and MCPDs by selected groups of population of Catalonia (Spain). Compound Exposure (μg/kg Adults Toddlers Infants Children Adolescents Adults Adults Seniors Pregnant bw/day) (18− 74 y) (18− 39 y) (40− 64 y) (65− 74 y) women Mean 0.042 0.41 0.35 0.23 0.097 0.045 0.036 0.032 0.054 Acrylamide P95 0.17 1.70 1.52 1.30 0.65 0.23 0.15 0.15 0.19 Mean 0.062 0.090 0.033 0.014 0.0089 0.045 0.069 0.057 0.039 Furan P95 0.22 0.32 0.17 0.062 0.034 0.19 0.22 0.22 0.17 Mean 0.11 0.040 0.019 0.011 0.008 0.13 0.21 0.17 0.11 2-MF P95 0.63 0.17 0.10 0.033 0.018 0.54 0.63 0.63 0.48 Mean 0.006 0.014 0.011 0.0055 0.0030 0.0076 0.011 0.0093 0.0071 3-MF P95 0.036 0.089 0.057 0.019 0.010 0.031 0.035 0.036 0.030 Mean 0.0094 0.054 0.047 0.031 0.019 0.0099 0.0081 0.0081 0.011 3-MCPD P95 0.034 0.13 0.15 0.12 0.078 0.040 0.030 0.029 0.047 Mean 0.0076 0.054 0.044 0.024 0.015 0.0074 0.0069 0.0068 0.0078 2-MCPD P95 0.025 0.13 0.14 0.095 0.057 0.027 0.022 0.023 0.028 3-MCPD Mean 0.153 1.96 1.08 0.58 0.27 0.15 0.14 0.14 0.17 ester P95 0.55 4.42 3.78 2.72 1.40 0.59 0.51 0.50 0.54 2-MCPD Mean 0.074 0.83 0.49 0.27 0.13 0.073 0.067 0.067 0.080 ester P95 0.26 2.06 1.75 1.25 0.64 0.28 0.25 0.24 0.26 Mean 0.126 0.68 0.71 0.54 0.25 0.13 0.11 0.11 0.14 GE P95 0.48 2.31 2.47 2.81 1.40 0.50 0.44 0.42 0.49 7 N. González et al. Journal of Food Composition and Analysis 106 (2022) 104272 Table 7 Risk assessment of acrylamide, furan and 3-MCPD (free + esters) for several population groups living in Catalonia (Spain). MOE or TDI Exposure Toddlers Infants Children Adolescents Adults Adults Seniors Pregnant women (18− 39 y) (40− 64 y) Acrylamide UB 338 368 548 1176 2507 2997 3339 2187 Neoplastic effects 170 μg/kg/day MB 419 481 755 1747 3740 4709 5371 3154 LB 600 694 1059 2572 5512 7157 8360 4604 UB 856 930 1386 2975 6341 7580 8445 5531 No neoplastic effects 430 μg/kg/day MB 1061 1217 1909 4418 9459 11,912 13,587 7977 LB 1518 1756 2678 6506 13,492 18,104 21,145 11,645 Furan UB 3670 11,073 27,552 45,435 22,696 15,488 17,972 25,560 Neoplastic effects 1310 μg/kg/day MB 14,527 39,730 91,046 146,987 29,403 18,929 22,802 33,556 LB -a -a 20,993,490 1,712,126 37,691 23,377 28,752 43,648 UB 179 541 1346 2220 1109 757 878 1249 No neoplastic effects 64 μg/kg/day MB 710 1941 4448 7181 1436 925 1114 1639 LB -a -a 102,277 83,646 1841 1142 1405 2132 3-MCPD (free + esters)* UB 3.37 1.82 0.914 0.440 0.247 0.228 0.225 0.271 TDI 0.8 μg/kg/day MB 2.01 1.13 0.610 0.290 0.164 0.147 0.146 0.179 LB 1.00 0.607 0.335 0.152 0.086 0.075 0.074 0.095 GEs UB 10,527 10,441 14,125 31,336 60,435 69,911 74,799 55,467 Neoplastic effects 10,200 μg/kg/day MB 15,042 14,367 18,944 41,577 78,380 90,730 95,188 71,120 LB 29,464 22,908 27,599 57,950 105,126 117,824 120,928 93,342 MOE: Margin of exposure; TDI: Tolerable daily intake; UB: Upper-bound; MB: Medium-bound; LB: Lower-bound. * Results are given in μg/kg/day; athe estimated exposure was zero; therefore, a MOE could not be calculated. kg bw/day as a reference point for the risk characterization of non- carcinogenic effects derived from glycidyl esters exposure. In turn, neoplastic effects. In turn, the risk characterization for neoplastic ef­ under the LB exposure scenario, none of the groups was above a MOE of fects was derived from the BMDL10 of 1310 μg/kg bw/day. Again, a 25,000. MOE of 100 or higher and a MOE of 10,000 or higher for non-neoplastic When the MOE according to the P95 dietary exposure was calcu­ and neoplastic effects, respectively, would be enough to conclude that lated, it was concluded that all the population groups were at risk for there is no health concern (EFSA, 2017). The calculated MOEs showed neoplastic effects derived from acrylamide exposure for the three sce­ that no group is at risk of developing non-neoplastic effects, being the narios considered (MOE < 10,000), while no risk was determined for the exposure levels for all the population groups above 100, for the three non-neoplastic effects (MOE > 100) (Table 8). For furan, most of the scenarios considered. With the calculation of the MOE for the neoplastic groups were at risk of suffering neoplastic effects in the three scenarios, effects, it can be concluded that none of the groups are at risk of suffering with the exception of adolescents (UB and MB), children (MB) and neoplastic effects, since the MOE was above 10,000, for LB and MB es­ pregnant women (LB). For the non-neoplastic effects, only toddlers were timates. However, for the UB, toddlers are at risk for neoplastic effects, at risk, with a MOE of 54 (Table 8). In addition, the TDI set for 3-MCPD as the calculated MOE was less than 10,000. Because of the lack of in­ (free + esters) was exceeded by most of the population groups in the UB, formation, the health risks associated to the dietary intake of 2-methyl­ with the exception of the seniors, while at the MB and LB, only the furans and 3-methylfurans could not be characterized. youngest population groups (aged <17) surpassed the threshold value. With respect to free- and ester-bound 3-MCPD, the CONTAM Panel Finally, the MOE calculated for the GE was below 25,000 for all the established a TDI of 0.8 μg/kg bw/day. No TDI could be established for population groups in the UB and MB scenarios, while in the LB, only the 2-MCPD and its fatty esters due to the lack of toxicological information youngest groups were at risk of suffering neoplastic effects (Table 8). (EFSA, 2016). The mean exposure levels estimated for different popu­ lation groups living in Catalonia showed that toddlers and infants in­ 4. Conclusions takes are above the TDI (2.01 and 1.13 μg/kg bw/day, respectively), while those of the remaining population groups are below that threshold To the best of our knowledge, this is the first study reporting the (range: 0.146− 0.61 μg/kg bw/day). Under the UB scenario, children, occurrence and the exposure and risk assessment of several FPCs in along with toddlers and infants, also exceeded the TDI (0.914, 3.37 and Spain. The highest concentrations of acrylamide and furan were found in 1.82 μg/kg bw/day, respectively). Differently, under the LB exposure different types of coffee (roasted, ground and beans), while the greatest scenario, only toddlers are above the established TDI (1.00 μg/kg levels of MCPDs were found in edible oils, including sunflower, pomace bw/day), meaning that toddlers, even at a low exposure scenario, are at and frying oils. The exposure assessment identified cookies, coffee, risk for the potential effects derived from MCPD exposure. bread and refined olive oil as the main contributors to the exposure of Since glycidol is genotoxic and carcinogenic, the CONTAM Panel acrylamide, furan, MCPDs and GEs, respectively. Moreover, this pattern considered that it was not appropriate to establish a TDI for glycidol. of contribution was similar irrespective of the population group. How­ Thus, the MOE approach was used to characterize the risk. Moreover, it ever, some specific foodstuffs, such as breakfast cereals or infant for­ was assumed that the complete hydrolysis of the esters to free glycidol is mulas, showed a remarkable contribution in the dietary intake of some achieved upon ingestion. In this case, a T25 approach (25 % increase in FPCs by toddlers and infants. According to risk assessment calculations, incidence of a specific tumor above background incidence in the lifespan all the population groups are currently at risk of suffering neoplastic of the species) was used, instead the BMD. The reference point used for effects derived from the exposure to acrylamide. Moreover, the human glycidol was 10,200 μg/kg bw/day. Moreover, the CONTAM Panel exposure to total 3-MCPD (free + ester-bound) and GEs by toddlers and considered that a MOE of 25,000 or higher was enough to conclude that infants exceeds the threshold values set by international organizations. there was not a health concern (EFSA, 2016). Toddlers, infants and In contrast, the current exposure to furans is not associated to health children had MOEs below 25,000, under the UB and MB exposure sce­ risks, for both neoplastic and non-neoplastic effects. Our findings clearly narios, which means that they may be at risk for the genotoxic and indicate that the current dietary exposure to FPCs in Catalonia (Spain) 8 N. González et al. Journal of Food Composition and Analysis 106 (2022) 104272 Table 8 Risk assessment of acrylamide, furan and 3-MCPD (free + esters) for several population groups living in Catalonia (Spain) in the P95 dietary exposure. MOE or TDI Exposure Toddlers Infants Children Adolescents Adults Adults Seniors Pregnant women (18− 39 y) (40− 64 y) Acrylamide UB 76 84 97 192 510 789 779 621 Neoplastic effects 170 μg/kg/day MB 100 112 130 263 726 1141 1134 875 LB 176 168 179 366 1042 1678 1693 1269 UB 192 211 246 486 1291 1996 1970 1570 No neoplastic effects 430 μg/kg/day MB 253 283 330 664 1837 2885 2869 2213 LB 446 425 453 927 2637 4244 4283 3209 Furan UB 1110 2153 5879 10,586 5251 4595 4245 5557 Neoplastic effects 1310 μg/kg/day MB 4050 7681 21,226 38,742 6970 6071 5930 7629 LB -a -a -a -a 8956 7844 7912 10,106 UB 54 105 287 517 257 224 207 271 No neoplastic effects 64 μg/kg/day MB 198 375 1037 1893 341 297 290 373 LB -a -a -a -a 438 383 387 494 3-MCPD (free + esters)* UB 7.38 6.23 4.20 2.20 0.94 0.81 0.78 0.86 TDI 0.8 μg/kg/day MB 4.54 3.93 2.85 1.48 0.63 0.54 0.53 0.58 LB 2.55 2.17 1.58 0.80 0.35 0.30 0.29 0.35 GEs UB 3279 2983 2663 5328 14,821 16,917 17,581 16,217 Neoplastic effects 10,200 μg/kg/day MB 4410 4124 3635 7268 20,217 23,095 24,134 20,790 LB 6958 6495 5509 10,809 29,673 33,580 35,663 28,852 MOE: Margin of exposure; TDI: Tolerable daily intake; UB: Upper-bound; MB: Medium-bound; LB: Lower-bound. * Results are given in μg/kg/day; athe estimated exposure was zero; therefore, a MOE could not be calculated. may be a health concern for some groups of the population, especially AECOSAN, 2016a. Encuesta Nacional De Alimentación En La Población Infantil Y Adolescente (2012-2015). Agencia Estatal De Consumo, Seguridad Alimentaria Y toddlers, infants and children, who are the most vulnerable. Therefore, Nutrición (AECOSAN). Ministerio De Sanidad, Servicios Sociales E Igualdad, food monitoring studies should be performed periodically to see the Gobierno De España. trends of FPCs and to assure that their exposure by young people follows AECOSAN, 2016b. Encuesta Nacional De Alimentación En Población Adulta, Mayores Y a decreasing trend. In parallel, specific policy measures should be Embarazadas (2014-2015). Agencia Estatal De Consumo, Seguridad Alimentaria Y Nutrición (AECOSAN). Ministerio De Sanidad, Servicios Sociales E Igualdad, adopted to minimize the intake of FPCs in Catalonia. Gobierno De España. AOCS, 2013. Official Methods and Recommended Practices of the AOCS (2013), 7th ed. 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