Occurence of Benzene As Heat-Induced Contaminant of Carrot
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Occurence of benzene as heat-induced contaminant of carrot juice for babies in a general survey of beverages Dirk W Lachenmeier, Helmut Reusch, Constanze Sproll, Kerstin Schoeberl, Thomas Kuballa To cite this version: Dirk W Lachenmeier, Helmut Reusch, Constanze Sproll, Kerstin Schoeberl, Thomas Kuballa. Oc- curence of benzene as heat-induced contaminant of carrot juice for babies in a general survey of bever- ages. Food Additives and Contaminants, 2008, 25 (10), pp.1216-1224. 10.1080/02652030802036230. hal-00577446 HAL Id: hal-00577446 https://hal.archives-ouvertes.fr/hal-00577446 Submitted on 17 Mar 2011 HAL is a multi-disciplinary open access L’archive ouverte pluridisciplinaire HAL, est archive for the deposit and dissemination of sci- destinée au dépôt et à la diffusion de documents entific research documents, whether they are pub- scientifiques de niveau recherche, publiés ou non, lished or not. The documents may come from émanant des établissements d’enseignement et de teaching and research institutions in France or recherche français ou étrangers, des laboratoires abroad, or from public or private research centers. publics ou privés. Food Additives and Contaminants For Peer Review Only Occurence of benzene as heat-induced contaminant of carrot juice for babies in a general survey of beverages Journal: Food Additives and Contaminants Manuscript ID: TFAC-2008-015.R1 Manuscript Type: Original Research Paper Date Submitted by the 28-Feb-2008 Author: Complete List of Authors: Lachenmeier, Dirk; Chemisches und Veterinäruntersuchungsamt Karlsruhe Reusch, Helmut; Chemisches und Veterinäruntersuchungsamt Karlsruhe Sproll, Constanze; Chemisches und Veterinäruntersuchungsamt Karlsruhe Schoeberl, Kerstin; Chemisches und Veterinäruntersuchungsamt Karlsruhe Kuballa, Thomas; Chemisches und Veterinäruntersuchungsamt Karlsruhe Chromatography - GC/MS, Chromatography - Headspace, Market Methods/Techniques: basket survey, Survey Additives/Contaminants: Benzene, Additives general, Metals, Process contaminants Food Types: Baby food, Beer, Beverages, Fruit juices http://mc.manuscriptcentral.com/tfac Email: [email protected] Page 1 of 21 Food Additives and Contaminants 1 2 3 4 5 1 Occurrence of benzene as heat-induced contaminant of carrot 6 7 8 2 juice for babies in a general survey of beverages 9 10 11 3 12 13 14 4 Dirk W. Lachenmeier ∗∗∗, Helmut Reusch, Constanze Sproll, Kerstin Schoeberl, Thomas 15 16 For Peer Review Only Kuballa 17 5 18 19 6 20 21 7 Chemisches und Veterinäruntersuchungsamt (CVUA) Karlsruhe, Weißenburger Str. 3, 22 23 8 D-76187 Karlsruhe, Germany 24 25 26 9 27 28 ∗ 10 To whom correspondence should be addressed. e-mail: [email protected] 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 1 http://mc.manuscriptcentral.com/tfac Email: [email protected] Food Additives and Contaminants Page 2 of 21 1 2 3 4 5 11 6 7 12 Abstract 8 9 10 13 A survey of benzene contamination of 451 beverage samples using headspace sampling 11 12 14 in combination with gas chromatography and mass spectrometry (HS-GC/MS) with a 13 14 -1 15 15 quantification limit of 0.13 µg l was conducted. Artefactual benzene formation during 16 For Peer Review Only 17 16 headspace sampling was excluded by only mildly heating at 50°C and adjustment of 18 19 20 17 sample pH to 10. The incidence of benzene contamination in soft drinks, beverages for 21 22 18 babies, alcopops and beer-mixed drinks was relatively low with average concentrations 23 24 19 below the EU drinking water limit of 1 µg l-1. Significantly higher concentrations were 25 26 27 20 only found in carrot juices, with the highest levels in carrot juices specifically intended 28 29 21 for infants. About 94% of 33 carrot juices for infants had detectable benzene levels with 30 31 -1 32 22 an average concentration of 1.86 ± 1.05 µg l . The benzene contamination of beverages 33 34 23 was significantly correlated to iron and copper concentrations, which act as catalyst in 35 36 37 24 benzene formation. The formation of benzene in carrot juices was predominantly caused 38 39 25 by a heat-induced mechanism, which explains the higher occurrence in infant carrot 40 41 26 juices that are considerably heated to exclude microbiological contamination. 42 43 44 27 45 46 28 Keywords: Benzene, benzoic acid, beverages, soft drinks, fruit juice, carrot juice, baby 47 48 49 29 food 50 51 52 53 54 55 56 57 58 59 60 2 http://mc.manuscriptcentral.com/tfac Email: [email protected] Page 3 of 21 Food Additives and Contaminants 1 2 3 4 5 30 Introduction 6 7 31 Benzene is one of the contaminants with the highest level of evidence for 8 9 10 32 carcinogenicity. For example, it was classified as carcinogenic to humans (Group 1) by 11 12 33 the International Agency for Research on Cancer (IARC 1987). Active as well as 13 14 15 34 passive smoking, automobile exhaust, and driving or riding in automobiles are 16 For Peer Review Only 17 35 postulated as the most important pathways for benzene exposure (Wallace 1996). Since 18 19 20 36 high levels of benzene metabolites are frequently reported among children and non- 21 22 37 smoking workers without occupational exposure, Johnson et al. (2007) hypothesize that 23 24 38 there may significant sources of benzene that are hitherto unidentified. 25 26 27 39 28 29 40 Since early 1990s, concerns about benzene contamination of food have been raised. 30 31 32 41 Several sources can contribute to the occurrence of benzene in foods. Benzoic acid, a 33 34 42 widely used food preservative, may decarboxylate to benzene in the presence of ascorbic 35 36 37 43 acid (Gardner and Lawrence 1993). The formation of benzene from benzoic acid is 38 39 44 influenced by the presence of transition-metal catalysts (for example, Cu(II) or Fe(III) 40 41 45 ions) and is dependent on pH, UV light or temperature (Gardner and Lawrence 1993; 42 43 44 46 McNeal et al. 1993; Chang and Ku 1993; Barshick et al. 1995). Benzene may be 45 46 47 introduced into foods through leaching from various packaging materials or storage 47 48 49 48 environments, from contamination of water supplies, or may be formed during 50 51 49 irradiation processes (Barshick et al. 1995). Another source of benzene in soft drinks 52 53 54 50 and beer is contaminated carbon dioxide used for carbonation (Long 1999; Wu et al. 55 56 51 2006). 57 58 52 59 60 3 http://mc.manuscriptcentral.com/tfac Email: [email protected] Food Additives and Contaminants Page 4 of 21 1 2 3 4 5 53 Methods for determination of benzene in food usually apply GC/MS and different 6 7 54 sample clean-up techniques like liquid-liquid extraction (Carrillo-Carrión et al. 2007), 8 9 55 static or purge and trap headspace sampling (Page et al. 1992; Gardner and Lawrence 10 11 12 56 1993; McNeal et al. 1993; Chang and Ku 1993; Barshick et al. 1995; Fabietti et al. 13 14 57 2001; Cao et al. 2007) or headspace solid-phase dynamic extraction (Ridgway et al. 15 16 For Peer Review Only 17 58 2007). Headspace solid-phase microextraction (HS-SPME) in combination with HPLC 18 19 59 was proposed for determination of benzene in fruit juices (Clasadonte et al. 1997). The 20 21 22 60 recent finding of benzene in drinks has raised concerns over analytical methodology, 23 24 61 especially heating during the purge-and-trap step that might lead to artefactual formation 25 26 62 of benzene (Hileman 2006). 27 28 29 63 30 31 64 There are only a few surveys that are currently available about benzene in food. Page et 32 33 -1 34 65 al. (1992) determined benzene levels ranging from 0.018 to 3.83 µg kg in 97 Canadian 35 36 66 samples of various fruits, juices and drinks. McNeal et al. (1993) showed that food 37 38 39 67 without added benzoates contained lower levels than some foods and beverages 40 41 68 containing both ascorbic acid and sodium benzoate. In a study of 60 soft drinks from 42 43 69 Italy (Fabietti et al. 2001), none of the samples were found to have benzene levels above 44 45 -1 46 70 the World Health Organization (WHO) guideline value of 10 µg l for benzene in 47 48 71 drinking water (WHO 2006). Out of 150 soft drinks sampled in the United Kingdom, 49 50 51 72 107 did not contain detectable levels of benzene but four contained average levels above 52 53 73 10 µg kg -1 (Food Standards Agency 2006). In a sample of 68 Australian flavoured 54 55 -1 56 74 beverages, 38 contained trace levels of benzene ranging from 1 to 40 µg kg (Anon 57 58 75 2006). From 84 Chinese lager beers, six contained detectable benzene concentrations up 59 60 76 to 7.1 µg l-1 (Wu et al. 2006). The U.S. Food and Drug Administration (FDA) tested 4 http://mc.manuscriptcentral.com/tfac Email: [email protected] Page 5 of 21 Food Additives and Contaminants 1 2 3 4 5 77 more than 100 soft drinks and other beverages from the United States. Almost all of 6 7 78 which contained either no benzene or levels below 5 µg kg -1 (Meadows 2006). Cao et al. 8 9 79 (2007) assessed benzene levels in 124 Canadian beverages, and found that 40% of the 10 11 12 80 samples contained detectable benzene levels and two products had benzene levels above 13 14 81 10 µg l-1.