Dietary intake of polychlorinated dioxins, furans and dioxin-like polychlorinated biphenyls from foods of animal origin in China

Four food groups of animal origin from the Chinese Total Diet Study (TDS) in 2000 were analysed for 17 polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) and 12 dioxin-like polychlorinated biphenyls (PCBs). The samples were from four regions, covering 12 provinces of China. PCDD/Fs, expressed as WHO toxic equivalents (TEQ), ranged from 0.02 to 0.28 pg TEQ g^-1 and dioxin-like PCBs ranged from 0.01 to 0.24 pg TEQ g^-1 (wet weight, ND = LOD), in all samples. Using food consumption data from a 3-day household dietary survey, daily dietary intake of dioxin-like compounds from foods of animal origin in China was estimated. Daily intake among regions ranged 0.09-0.59 pg TEQ kg^-1 body eight day^-1.     

The use of the DR CALUX bioassay and indicator polychlorinated biphenyls for screening of elevated levels of dioxins and dioxin-like polychlorinated biphenyls in eel

The DR CALUX bioassay is a very suitable screening method for dioxins and dioxin-like-PCBs in feed and food. This was, e. g. demonstrated in a survey in the Netherlands to control the dioxin levels in eel. The DR CALUX assay, but also indicator polychlorinated biphenyls (PCB) were evaluated as a screening method. Based on the limit for polychlorinated dibenzo-p-dioxins/dibenzofurans (PCDD/F) [at that time 8 pg toxic equivalents (TEQ)/g eel], and the relation between PCDD/F and dioxin-like-PCB, a decision limit of 30 pg TEQ/g eel was used for screening of 153 field samples. Suspected samples (21) and part of the higher contaminated negative samples (35) were analyzed by GC/MS for dioxins, non-ortho, mono-ortho and indicator PCB, revealing 13 samples exceeding the action limit of 30 pg TEQ/g eel. Only one sample slightly exceeded the dioxin level of 8 pg TEQ/g eel. The relatively low sensitivity for mono-ortho PCB was overcome by the use of reference samples, as shown by the correlation of 0.93 between GC/MS and CALUX determined total TEQ levels. The present data show that the DR CALUX assay can be used for screening of total TEQ levels in eel. The use for dioxins only requires a safe, and therefore relatively low, decision limit. The indicator PCB also showed a good correlation with total TEQ levels, mainly due to the large contribution of the mono-ortho PCB at higher concentrations. The relation with dioxins was very poor and as such indicator PCB seem less suitable than the DR CALUX assay for screening for dioxins only. The present study clearly shows that part of the wild eel samples contains high total TEQ levels and will exceed the future European Union limit of 12 pg TEQ/g eel for dioxins and dioxin-like PCB. Especially at high TEQ levels, dioxin-like PCB contribute most to the total TEQ. In practice, wild eel presents only a minor part of the eel consumed.     

Risk assessments of polychlorinated dibenzo- p-dioxins, polychlorinated dibenzofurans, and dioxin-like polychlorinated biphenyls in food

The polychlorinated dibenzo-p-dioxins (PCDD), polychlorinated dibenzofurans (PCDF), and dioxin-like polychlorinated biphenyls (dioxin-like PCB) are ubiquitous in food of animal origin and accumulate in fatty tissues of animals and humans. The most toxic congener is 2,3,7,8-tetrachlorodibenzo-p-dioxin (TCDD). The toxic responses include dermal toxicity, immunotoxicity, carcinogenicity, and reproductive and developmental toxicity. Toxic equivalency factors have been established for the other PCDD, PCDF and dioxin-like PCB relative to TCDD, and the combined toxicity of a sample can be expressed as toxic equivalent (WHO-TEQ). The EC Scientific Committee for Food evaluated these compounds in 2001. The assessment used the most sensitive adverse toxicological end-points of TCDD in experimental animals. These were developmental and reproductive effects in the male offspring of rats administered TCDD during pregnancy. Because of the large difference between rats and humans in the biological half-life of TCDD, the assessment used a body burden approach to compare across species and derived a tolerable weekly intake of 14 pg TCDD/kg of body weight (bw), which was extended to include all the 2,3,7,8-substituted PCDD and PCDF, and the dioxin-like PCB, and expressed as a group tolerable weekly intake of 14 pg WHO-TEQ/kg bw. The FAO/WHO Joint Expert Committee on Food Additives (JECFA) performed a similar assessment whereas the US Environmental Protection Agency (US EPA) has paid more attention to human data on carcinogenicity.     

Dietary intakes of polychlorinated dibenzo-p-dioxins, dibenzofurans and dioxin-like polychlorinated biphenyls in Spain.

Congener-specific analyses of seventeen 2,3,7,8-substituted PCDD/Fs, three non-ortho and 8 mono-ortho dioxin-like polychlorinated biphenyls (PCBs) were performed on 258 Spanish foodstuff samples, mainly of animal origin, for 2000--03. Daily dietary intakes of PCDD/Fs and PCBs, expressed as toxic equivalents (WHO-TEQs), were estimated by combining food consumption data from the Spanish National Institute Statistics survey and concentration levels measured in individual samples, using upper bound determination values (not detectable = limit of detection). The calculated dietary intake of PCDD/Fs for a person weighing 70 kg was 1.35+/-0.11pg WHO-TEQs kg(-1) bw day(-1), and 3.22+/-0.75 pg WHO-TEQs kg(-1) bw day(-1) if dioxin-like PCBs (non- and mono-ortho PCBs) were included, showing the importance of their inclusion in monitoring studies. Both values were within the range of tolerable daily intake (TDI) proposed by the WHO (1-4pg WHO-TEQs kg(-1) bw day(-1)). The current levels are lower than earlier intakes estimates conducted in Spain. Meat and meat products accounted for more than 35% of the intake, followed by milk and milk products (29%), vegetables oils (19%), fish and seafood (11%) and eggs (4%). Dioxin-like PCBs are an important component in the total WHO-TEQs in foodstuffs. This is particularly true for the fish food group, where the total WHO-TEQs is dominated by dioxin-like PCBs (up to 80% of WHO-TEQs in some cases).     

Occurrence of polychlorinated dibenzo-p-dioxins (PCDDs), dibenzofurans (PCDFs) and polychlorinated biphenyls (PCBs) in eggs from free-range hens in Campania (southern Italy) and risk evaluation

ABSTRACT

Hens’ eggs collected in home-producing farms located in different areas of the Campania region of southern Italy were analysed for six NDL-polychlorobiphenyls (PCB indicators), 17 polychlorodibenzo-p-dioxins (PCDDs) and polychlorodibenzofurans (PCDFs), and 12 congeners of dioxin-like PCBs (DL-PCBs). In the investigated area, waste from civil, industrial and hospital activities was illegally dumped and in many cases burned, so the area is called the ‘Land of fire’. This illicit practice has been considered the main source of pollution in this territory and the cause of the persistent organic pollutants’ (POPs) contamination in the neighbouring lands intended for agricultural use and livestock. The results, which were obtained from the analysis of 56 samples of eggs, showed levels of contamination by dioxins and PCBs that have often exceeded the action levels set by European Union Recommendation 711/2013 and sometimes even exceeded the maximum levels set by Commission Regulation (EU) 1259/2011. The median PCDD/Fs was 0.41 pg TEQ g^?1 fat (range = 0.01–6.18 pg TEQ g^?1 fat) and the median concentration of DL-PCBs was 0.70 pg TEQ g^?1 fat (range = 0.01–14.60 pg TEQ g^?1 fat), whereas NDL-PCBs median was 7.35 ng g^?1 fat (range = 0.48–67.55 ng g^?1 fat). Nevertheless, the estimated weekly intake (EWI) calculated for consumers of eggs home produced in Campania is lower than the tolerable weekly intake (TWI) established by the European Union Scientific Committee on Food (SCF).     

Contamination of human fat from Rostock residents with DDT and polychlorinated biphenyls in 1979)

70 fat samples collected from Rostock men and women, aged between 20 and 90 years, were analysed by gas chromatography for total DDT and polychlorinated biphenyls (PCB). It was found that the mean value for DDT and also that for PCB increased with the increase in age, the mean values for all the subjects being 4.0 +/- 0.5 mg/kg (PCB). There were no statistically significant differences among the residue values found in men and women.     

Butter as an indicator of regional persistent organic pollutant contamination: further development of the approach using polychlorinated dioxins and furans (PCDD/Fs), and dioxin-like polychlorinated biphenyls (PCBs)

The potential for use of butter as a widely available, relatively uniform lipid-rich matrix for the determination of spatial distributions of persistent organic pollutants has already been demonstrated. The present study determines the contributions to toxicity equivalence (TEQ) from polychlorinated dioxins and furans (PCDD/Fs) and polychlorinated biphenyls (PCBs) using butter samples from 24 countries world wide. Concentrations of PCDD/Fs and dioxin-like PCBs ranged from 0.07 to 5.69 pg ΣWHO-TEQ g -1 lipid. For most samples, PCDD/F TEQ fell within ranges reported for European dairy products over the last decade (0.3-2 pg g -1 lipid I-TEQ), though a single sample from Spain was a notable exception. Other than this sample, the highest values were recorded for samples from the Netherlands and Italy, with those from India, China and Tunisia also being relatively high. The contribution from non- ortho -PCBs was particularly significant in samples from Germany, Austria, Italy, the Czech Republic, Tunisia, India and Argentina. Although overall TEQs were generally highest in European and Mediterranean butters, elevated levels were also apparent in industrializing regions of Asia (India, China) and Latin America (Argentina). More detailed regional studies would be necessary to identify likely dioxin and PCB sources in each case. Nevertheless, this study supports the utility of butter as a monitoring matrix that may be especially applicable in regions for which monitoring programmes are currently lacking.     

Dietary exposure and risk assessment of polychlorinated dibenzo-p-dioxins,polychlorinated dibenzofurans and dioxin-like polychlorinated biphenyls of the population in the Region of Valencia (Spain)

Dietary exposure of the Valencia Region population to polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs) and PCBs was assessed in the Region of Valencia in 2010–2011. A total of 7700 food samples were collected. Occurrence data were combined with consumption data to estimate dietary exposure in adults (>15 years of age) and young people (6–15 years of age). The estimated intake was calculated by a probabilistic approach. Average intake levels (upper-bound scenario) were 1.58 and 2.76 pg toxic equivalent (TEQ) kg^?1 body weight (bw) day^?1 for adults and young people, respectively. These average intakes are within range of the tolerable daily intake of 1–4 pg WHO-TEQ kg^?1 bw day^?1 recommended by WHO, and slightly above the tolerable weekly intake (TWI) of 14 pg TEQ kg^?1 bw week^?1 and the Provisional tolerable monthly intake of 70 pg TEQ kg^?1 bw month^?1 set by the Scientific Committee on Food and the Joint FAO/WHO Expert Committee on Food, respectively. These results show that the contamination levels in food and therefore the exposure of the general population to PCDD/Fs and PCBs have declined in this region and therefore show the efficiency of the European risk-management measures. In terms of risk characterisation, the results showed that, under the upper-bound scenario, 22% of the adult and 58% of the young people population could exceed the TWI.     

Development of a screening analytical method for the determination of non-dioxin-like polychlorinated biphenyls in chicken eggs by gaschromatography and electron capture detection

ABSTRACT

A sensitive and reproducible screening analytical method is here proposed for the determination of six non dioxin-like polychlorinated biphenyls (NDL-PCBs, congener 28, 52, 101, 138, 153, 180) in chicken eggs based on accelerated solvent extraction (ASE) procedure for the fat extraction and determination, a solid phase extraction (SPE) sample clean-up process, and a gas chromatography – electron capture detection (GC-ECD) analysis. The optimized chromatographic separation, in less than 25 min, returned good responses for the six NDL-PCBs in the range of 2.5–60.0 µg L^?1, with correlation coefficients always higher than 0.9995. Instrumental limits of detection were between 0.08–0.35 µg L^?1, corresponding to 0.05 and 0.23 ng g^?1 fat in the matrix, while method detection limits, calculated on spiked egg samples, ranged from 1.6 to 3.5 ng g^?1 fat. The method has been extensively validated in terms of selectivity, sensitivity, recovery, precision, ruggedness and measurement uncertainty, following the European Directives.     

A preliminary comparison of polybrominated diphenyl ether concentrations relative to lipid content and to levels of dioxins and dioxin-like polychlorinated biphenyls in Norwegian farmed Atlantic salmon (Salmo salar)

Polybrominated diphenyl ethers (PBDEs) are environmental contaminants structurally similar to polychlorinated biphenyls (PCBs), and correlations between PBDE concentrations and concentrations of lipid, PCBs, dioxins and furans in feed and farmed Atlantic salmon filet indicate PBDEs may be derived from similar sources. PBDE concentrations (3.9 ± 0.6 ng g^?1 wet wt) in farmed Atlantic salmon correlated well with lipid content and these other halogenated contaminants, however, lower concentrations of PBDEs (1.6 ± 0.3 ng g^?1 wet wt) showed no correlation. Possible explanations for the non‐linear behaviour of PBDE concentrations in Atlantic salmon are discussed.     

Chemical contamination of free-range eggs from Belgium

The elements manganese, cobalt, nickel, copper, zinc, arsenic, selenium, molybdenum, cadmium, antimony, thallium, lead and mercury, and selected persistent organochlorine compounds (dioxins, marker and dioxin-like polychlorinated biphenyls, dichlorodiphenyltricholroethane (DDT) and metabolites as well as other chlorinated pesticides) were analysed in Belgian free-range eggs obtained from hens of private owners and of commercial farms. It was found that eggs from private owners were more contaminated than eggs from commercial farms. The ratios of levels in eggs from private owners to the levels in eggs from commercial farms ranged from 2 to 8 for the toxic contaminants lead, mercury, thallium, dioxins, polychlorinated biphenyls and the group of DDT. DDT contamination was marked by the substantial presence of p,p'-DDT in eggs from private owners in addition to dichlorodiphenyldichloroethylene (p,p-DDE) and dichlorodiphenyl-dichloroethane (p,p'-DDD). It is postulated that environmental pollution is at the origin of the higher contamination of eggs from private owners. Extensive consumption of eggs from private owners is likely to result in toxic equivalent quantity intake levels exceeding the tolerable weekly intake.     

Levels of polychlorinated bifenilis and organochlorine in pesticides in chicken eggs from different Russian regions

Chicken eggs are recognized as a useful matrix for international comparison of accumulation levels of persistent organic pollutants (POPs) in foodstuffs. The paper contains results of detection of 17 congeners of PCB, hexachlorobenzene, hexachlorocyclohexane, DDT and its metabolites in chicken eggs, collected near the former PCB-containing producing plant (Novomoskovsk), the plant earlier produced organochlorine pesticides and hexachlorobenzene (Chapaevsk) and from several areas of the Saratov region. Comparison of obtained results with data from IPEN international study has shown that PCBs levels in chicken eggs from the town of Novomoskovsk and from Chapaevsk local farms is significantly higher than for the most polluted territories in different countries of the world. Chicken eggs' pollution by DDT and HCCH is less expressed than by PCBs. Analysis of these matters' content in chicken egg samples, collected in five poultry farms in different regions of Russia has not revealed a remarkable level of chlorinated pesticide pollution.     

Dietary intake of dioxins,furans and dioxin-like PCBs in Austria

Human exposure to polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) and dioxin-like PCBs (dl-PCBs) should be assessed regularly. In order to evaluate the contamination levels in various food products on the Austrian market and to assess the dietary exposure of the Austrian population for the first time, a national monitoring programme was conducted from 2005 to 2011. The 235 food products comprised meat, poultry, game and offal, fish and fish products, milk and dairy products, eggs, animal fats and vegetable oils. To estimate the dietary intakes of PCDD/Fs and dl-PCBs, mean concentrations in food were combined with the respective food consumption data from the Austrian food consumption survey. Estimated dietary intakes were expressed as toxic equivalents (WHO-TEQs 1998). The mean intakes for PCDD/Fs and dl-PCBs were estimated as 0.77, 0.75 and 0.61 pg WHO-TEQ kg^?1 bw day^?1 for children, women and men, respectively. The main contributors to total intake were milk and dairy products followed by fish and fish products for children and women, and meat, poultry, game and offal for men (65% and 15% for children, 67% and 14% for women, and 63% and 19% for men, respectively). Comparison of the estimated dietary intakes with the toxicological reference values shows that both children and adults are well below those values.     

Changes in concentrations of dioxins and dioxin-like PCBs during processing of fish

Fish among meat and dairy products mainly contribute to the human exposition with dioxins and dioxin-like PCBs. Contaminant levels of fish are mainly determined in the edible part of the raw material. In Germany fish are not consumed raw but industrially processed to manifold products and cooked, fried or deep-fried in household. To study the influence of processing on the contaminant levels, changes of dioxins and partly of dioxin-like PCBs were followed during canning of herring fillets, hot smoking of mackerel fillets and Greenland halibut cutlets and during sugar salting of beheaded whole herring. The hot smoking process and sugar salting of herring led to an increase of the dioxin content in the edible part of the final product. The increase was related to the loss of water during processing whereas the fat and thus the lipophilic dioxins remained in the muscle meat. For sugar salting also changes of dioxin-like PCB levels were followed and the same effect was observed. Otherwise the production of canned herring fillets in tomato sauce led to a “dilution” of the dioxin content due to the addition of the sauce.     

Pan-arctic river fluxes of polychlorinated biphenyls

Observations of polychlorinated biphenyls (PCB) concentrations in fluvial surface sediments near the mouths of the six Great Arctic Rivers (GARs; Ob, Yenisey, Lena, Indigirka, Kolyma, and Mackenzie) were combined with annual dissolved organic carbon (DOC) and particulate organic carbon (POC) loadings and hydraulic discharge to estimate the pan-Arctic river flux of PCBs. The highest total-phase fluxes of ∑(13)PCB were found for the Ob River, with 184 kg/yr and the smallest for the Indigirka River with 3.9 kg/yr. Consistent with a continent-scale trend among the Eurasian GARs of increasing POC concentrations eastward, which is extending to the North American Mackenzie River, a general shift in the estimated PCB partitioning from dissolved to particle-associated flux was found toward the east. Pentachlorinated and hexachlorinated PCBs constituted the majority (>70%) of the total PCB fluxes in the Eurasian Rivers. In contrast, trichlorinated and tetrachlorinated congeners were the most abundant in the Mackenzie (≈ 75%). The total ∑(13)PCB fluxes from the pan-Arctic rivers are here estimated to be ～0.4 tonne/yr. This is geochemically consistent with the inventory of total PCBs in the Polar Mixed Layer of the entire Arctic Ocean (0.39 tonne) and about a factor 2 less than two new estimates of the PCB settling export to Arctic subsurface waters. Hence, the yearly Great Arctic River PCB fluxes only represent 0.001% of the historical PCB emission into the global environment. To our knowledge, this is the first estimate of circum-Arctic river flux of any organic pollutant based on a comprehensive investigation of the pollutants in several rivers and it contributes toward a more complete understanding of large-scale contaminant cycling in the Arctic.     

Exposure to polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), dioxin-like polychlorinated biphenyls (DL-PCBs) and polybrominated diphenyl ethers (PBDEs) through the consumption of prepared meals in Italy

Diet is a relevant source of exposure to environmental pollutants. Dietary intake of polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), dioxin-like polychlorinated biphenyls (DL-PCBs) and polybrominated diphenyl ethers (PBDEs) by the Italian population was assessed through a duplicate diet study on prepared meals. Baby food composite representative of the diet of toddlers aged 9–12 months and school canteen servings from four towns in Italy representing the diet of children aged 4–9 years were collected on a 5-day basis. Similarly, 5-day lunches from an office canteen, 7-day lunches from a hotel-school, three fast food meals, and eight duplicate 1-day meals of individuals (one vegetarian) were selected to represent the diet of adults aged above 18 years. Servings from each diet were then pooled to form a composite and analysed. Dietary intake was estimated from the resulting contaminant levels in composites combined with age-related food consumption data from national survey. The mean upper bound (UB) intakes for cumulative PCDDs, PCDFs, and DL-PCBs were 0.67, 0.63–0.92, and 0.27–0.63 pg WHO₂₀₀₅-TE kg^?1 body weight (bw) day^?1 for toddlers, children and adults, respectively. BDE-47 (UB) ng kg^?1 bw day^?1 estimates were 2.75 in toddlers, 0.08–0.16 in children and 0.03–0.09 in adults. Similarly, for BDE-99 higher UB intakes (ng kg^?1 bw day^?1) resulted in toddlers (1.26), than those in children (0.06–0.08) and adults (0.03–0.10), respectively. The above estimates fall below the tolerable weekly intake (TWI) (14 WHO₂₀₀₅-TE kg^?1 bw day^?1) established by the European Union Scientific Committee on Food (SCF) for PCDD/Fs and DL-PCBs. The margin of exposure (MOE = 3) of toddlers to BDE-99 clearly indicates this age group as target for a risk-oriented approach. This study is proposed as a first cost-effective screening in PCDD, PCDF, DL-PCB and PBDE intake assessment, with a focus also on time trends.