Evaluation of dioxin-like chemicals in pooled human milk samples collected in Australia

DESIGN: Human milk samples were collected and analysed for the levels of polychlorinated dibenzodioxins (PCDDs), polychlorinated dibenzofurans (PCDFs) and selected dioxin-like polychlorinated biphenyls (PCBs). In total, 157 individual samples collected during 2002 and 2003 as well as 24 samples collected in 1993 were analysed as 20 pools. RESULTS: PCDDs, PCDFs and dioxin-like PCBs were detected in all pooled samples. For samples collected during 2002/2003, the TEQ(DFP) ranged from 6.0 to 15.2 pg TEQ g(-1) lipid with an average of 9.0 pg TEQ g(-1) lipid. The average lipid content was 3.7+/-0.5%. No systematic differences were observed in the levels of PCDDs, PCDFs and PCBs in human milk samples collected from different regions of Australia during 2002/2003. For samples collected in 1993 and analysed as pools, the mean level, expressed as TEQ(DFP) was 16+/-1.4 pg TEQ g(-1) lipid. The average lipid content was 3.9+/-0.7%. CONCLUSION: The levels of PCDDs, PCDFs and dioxin-like PCBs in the human milk of Australian women are both low compared to international levels and similar across all regions of Australia. Consistent with world-wide trends, the levels of PCDDs, PCDFs and dioxin-like PCBs have decreased over a 10 year period from 1993 to 2003 by approximately 40%.     

PCDDs, PCDFs and dioxin-like PCBs in food of animal origin (Slovakia)

The levels of 17 toxic polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs) and 12 non-ortho and mono-ortho polychlorinated biphenyls (PCBs) in 73 foodstuff samples of animal origin collected from shops and small farms in selected districts of Slovak Republic are presented in this paper. The concentrations expressed as WHO-TEQ in analysed samples ranged for PCDDs/PCDFs from 0.25 pg/g fat in pork to 75 pg/g fat in cod liver. The TEQ concentrations of non-ortho PCBs were between 0.007 and 181 pg/g fat and mono-ortho PCBs between 0.0083 and 66.5 pg/g fat. The mean concentrations in freshwater fish and imported species of marine fish were 0.089 pg TEQ/g fresh weight for PCDDs/PCDFs, 0.17 pg TEQ/g fresh weight for non-ortho PCBs and 0.034 pg TEQ/g fresh weight for mono-ortho PCBs. The mean total concentration of PCDDs/PCDFs and dioxin-like PCBs in samples of infant milk formula imported from EU countries was 0.98 pg TEQ/g fat.     

Distribution of dioxins, furans, and dioxin-like PCBs in solid products generated by pyrolysis and melting of automobile shredder residues

Polychlorinated dibenzo-p-dioxins, polychlorinated dibenzofurans, and dioxin-like polychlorinated biphenyls (PCBs) in char and slag produced from automobile shredder residue by pyrolysis and melting process were analyzed to measure changes in the characteristics and distribution of their congeners caused by thermal treatment. In particular, a large quantity of dioxin-like PCBs occurred in low-chlorinated congeners. The concentration of PCDDs/PCDFs in char was 0.542 microg/kg, with mostly PCDFs dominant and its toxicity equivalent concentration (TEQ) was about 70ngTEQ/kg. The concentration and toxicity equivalent concentration of dioxin-like PCBs in char were 0.869 microg/kg and 1.60ngTEQ/kg, respectively. Melted char slag was produced using various cooling methods: water quenching, air cooling, and slow cooling. The concentrations of PCDDs/PCDFs in slag produced by the methods were 1.51, 1.38, and 2.43ngTEQ/kg, respectively; those of dioxin-like PCBs were close to 0.01ngTEQ/kg. The congener distributions varied only slightly among the cooling methods. Applying melting procedure to char reduced PCDD/PCDF concentration by 95.3%, and the corresponding TEQ concentration was reduced by 97.9%. We thus conclude that melting process is an efficient way to reduce the concentrations of PCDDs/PCDFs in solids produced by pyrolysis.     

Concentrations of polychlorinated dibenzo-p-dioxins, polychlorinated dibenzofurans, and dioxin-like polychlorinated biphenyls in blood collected from 195 pregnant women in Sapporo City, Japan

We measured the concentrations of polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), non-ortho coplanar polychlorinated biphenyls (non-ortho PCBs), and mono-ortho coplanar polychlorinated biphenyls (mono-ortho PCBs) in blood collected between 2002 and 2004 from 195 pregnant women living in Sapporo City of Hokkaido Prefecture, Japan. The present study is one of the few studies in which PCDDs, PCDFs, and dioxin-like PCBs have been measured in the blood of pregnant women. Of the 195 pregnant women, 101 were primipara (mean: 28.8 years) and 94 were multipara (mean: 32.4 years). The arithmetic mean total TEQ concentrations of PCDDs, PCDFs, non-ortho PCBs, and mono-ortho PCBs of primiparous and multiparous mothers in Sapporo City were 17.4 (median: 15.7) and 14.0 (median: 13.9)pgTEQ/glipid, respectively, and the concentrations were in the range of 6.6-43.4 and 3.4-28.2pgTEQ/glipid, respectively. In regard to the relationship between the total TEQ concentrations of PCDDs, PCDFs, non-ortho PCBs, and mono-ortho PCBs in maternal blood and the number of deliveries or age of primiparous and multiparius mothers, the levels of these dioxin-like compounds tended to decrease with increases in the number of deliveries and significantly increased with increasing maternal age in both groups. Furthermore, significant correlations were observed between the total TEQ concentrations of these dioxin-like compounds and the age of primiparae and multiparae. The total TEQ concentration of PCDDs, PCDFs, non-ortho PCBs, and mono-ortho PCBs measured in 195 pregnant women has decreased compared to past levels in Japan for the last several decades. The results of the present study have indicated that dioxin contamination in the blood of young women in Japan is continuing to decrease.     

Concentration changes of PCDDs, PCDFs, and dioxin-like PCBs in human breast milk samples as shown by a follow-up survey

Breast milk is known to discharge dioxins from the human body. However, to date, no direct comparison has been made of the concentrations of dioxin analogues in breast milk obtained from identical population after successive deliveries. We present here follow-up survey results of PCDDs, PCDFs, and dioxin-like PCBs concentrations in human breast milk samples from 35 women living in Tokyo from whom samples had been obtained and analyzed to determine the corresponding concentrations in the past. The average concentrations of total PCDDs, PCDFs, dioxin-like PCBs were 8.5, 5.5, 11 TEQ pg/g fat for the first samples and 5.4, 4.0, 6.6 TEQ pg/g fat for the second samples, respectively. The degrees of reduction of total PCDDs and total dioxin-like PCBs were higher than that of total PCDFs because 1,2,3,7,8-PeCDD, 2,3,4,7,8-PeCDF and 3,3',4,4',5-PeCB (#126), which were the predominant congeners among PCDDs, PCDFs, and dioxin-like PCBs, respectively, had different degrees of reduction. Moreover we observed a significant increase of the concentrations of PCDDs, PCDFs, and dioxin-like PCBs in samples from three women in this follow-up survey, and the patterns of increased isomers differed among the three samples. It was conjectured that the increase of the concentrations was due mainly to dietary intake between deliveries. It is important for pregnant women to have a balanced diet to mitigate the exposure of infants to these chemicals.     

Concentrations of polychlorinated dibenzo-p-dioxins, polychlorinated dibenzofurans, and dioxin-like polychlorinated biphenyls in blood and breast milk collected from 60 mothers in Sapporo City, Japan

We measured the concentrations of polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), non-ortho polychlorinated biphenyls (non-ortho PCBs), and mono-ortho polychlorinated biphenyls (mono-ortho PCBs) in paired samples of blood and breast milk collected from 60 mothers in Sapporo City, Hokkaido Prefecture, Japan. The present study is one of the few studies in which PCDDs, PCDFs, and dioxin-like PCBs have been measured in blood and breast milk collected from 60 same mothers. Of these 60 mothers, 30 were primipara (mean: 30.1 years, median: 28.0 years) and 30 were multipara (mean: 32.2 years, median: 32.5 years). The arithmetic mean TEQ concentrations of PCDDs, PCDFs, non-ortho PCBs, and mono-ortho PCBs in blood and breast milk of the primiparous mothers were 9.0, 3.3, 5.7, and 0.4 pg TEQ g(-1) lipid, respectively, and 5.2, 2.2, 4.5, and 0.4 pg TEQ g(-1) lipid, respectively, with the total TEQ concentrations of these dioxin-like compounds being 9.3-42.9 (mean: 18.4, median: 17.3) and 7.0-41.1 (mean: 12.3, median: 11.4) pg TEQ g(-1) lipid, respectively. In the case of multiparous mothers, the arithmetic mean TEQ concentrations of these dioxin-like compounds in blood and breast milk were 7.1, 2.7, 5.3, and 0.4 pg TEQ g(-1) lipid, respectively, and 3.9, 1.7, 3.8, and 0.4 pg TEQ g(-1) lipid, respectively, with the total TEQ concentrations being 3.4-28.1 (mean: 15.5, median: 13.9) and 2.7-20.0 (mean: 9.8, median: 9.2)pg TEQ g(-1) lipid, respectively. The total TEQ concentrations of PCDDs, PCDFs, non-ortho PCBs, and mono-ortho PCBs in blood and breast milk of primiparous mothers in Sapporo City appeared to be generally lower than those recently surveyed throughout the greater area of Japan. Significant correlations were observed between age and the total TEQ concentrations of PCDDs, PCDFs, non-ortho PCBs, and mono-ortho PCBs in the blood of primiparae and multiparae, and significant correlations were also observed between age and the total TEQ concentrations of these dioxin-like compounds in the breast milk of primiparae and multiparae. The total TEQ concentrations of PCDDs, PCDFs, and dioxin-like PCBs in the blood of primiparous mothers showed a close correlation to those in their breast milk and also showed good correlations between the total TEQ concentrations of these dioxin-like compounds in the blood of multiparous mothers and those in their breast milk. The result of a comparison of the arithmetic mean concentrations of each congener of PCDDs, PCDFs, non-ortho PCBs, and mono-ortho PCBs in blood and breast milk indicated that the transfer of octachlorodibenzo-p-dioxin (OCDD) from the blood to the breast milk was lower than those of other congeners. In contrast, among mono-ortho PCBs congeners, the arithmetic mean concentrations of 2,3',4,4',5-pentachlorobiphenyl (PentaCB) (#118) and 2,3,3',4,4'-PentaCB (#105) in the breast milk were slightly higher than those in the blood, which suggested that breast-fed infants may be at higher risk from mono-ortho PCBs.     

Estimation of 1999-2004 dietary daily intake of PCDDs, PCDFs and dioxin-like PCBs by a total diet study in metropolitan Tokyo, Japan

A study of the dietary intake of dioxins, consisting of polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs) and dioxin-like polychlorinated biphenyls (dioxin-like PCBs) through foods retailed in the metropolitan Tokyo area from 1999 to 2004 was carried out by the total diet-market basket method on the basis of food classification (14 groups) and the data on food consumption in the Tokyo region obtained from the Japan Nutrition Survey. The daily intake of dioxins per kg of body weight for a 50 kg average adult body was 2.18 pg TEQ/kg/day in 1999, 1.87 pg TEQ/kg/day in 2000, 1.25 pg TEQ/kg/day in 2001, 1.60 pg TEQ/kg/day in 2002 and 2003 and 1.55 pg TEQ/kg/day in 2004, respectively. These amounts were less than the tolerable daily intake (TDI) of 4 pg TEQ/kg/day for dioxins established in Japan. The dioxins taken daily through fish and shellfish (group 10) accounted for more than 50% of sum WHO-TEQs. In addition, more than 90% of the daily intake of dioxins was taken through fish and shellfish (group 10), meat and eggs (group 11), milk and dairy products (group 12). Also, this study clearly showed that the ratio of dioxin-like PCBs in the daily intake of dioxins was increasing yearly because the reduction rate of dioxin-like PCBs was lower than that of PCDDs and PCDFs in foods.     

A worldwide survey of polychlorinated dibenzo-p-dioxins, dibenzofurans, and related contaminants in butter

The main source of human exposure to persistent organic pollutants (POPs) is, in general, food. In this study, 64 butter samples from 37 countries were analyzed to assess the global contamination of polychlorinated dibenzo-p-dioxins (PCDDs), dibenzofurans (PCDFs), biphenyls (PCBs), hexachlorobenzene (HCB), and 2,2-bis (4-chlorophenyl)-1,1,1-trichloroethane (DDT) together with its major metabolites. The objectives of the study were to assess the presence of major organohalogen contaminants in butter, to trace geographical differences, and to determine toxic equivalents (TEQs) of PCDDs/Fs and dioxin-like PCBs in butter. The highest PCDD/F concentrations were found in butter from Korea with an average of 1.4 pg TEQ g(-1) lipid weight (l.w.). from PCDD/F and an additional contribution from the non- and mono-ortho-PCBs of 0.55 pg TEQ g(-1) l.w. Belgian butter showed average levels of 0.53 and 1.2 pg TEQ g(-1) l.w. for PCDDs/Fs and PCBs, respectively, but one sample of Belgium butter had a total TEQ level as high as 4.0 pg TEQ g(-1) l.w. Three out of five butter samples from Portugal showed similarly high PCDD/F TEQ levels. The sigmaPCB levels in European butter appeared to be somewhat higher than in the samples from the rest of the world. The average contribution of CB-153 to the total PCB concentration was 22% (SD 6.4, coefficient of variation 29%). Generally, the PCBs contributed around 60% of the total TEQ value, with CB-126 contributing approximately half of this value. This shows the important TEQ contribution from dioxinlike PCBs to the total TEQs. The highest HCB levels were found in butter samples from Russia, Ukraine, Belgium, and Slovenia. Low levels of HCB in butter were generally found in the Southern Hemisphere. Butter samples from countries from Eastern Europe had elevated sigmaDDT concentrations, with a particularly high concentration in Ukraine butter, followed by some Russian samples, Brazil, and the U.S.     

Embryonic abnormalities and organochlorine contamination in double-crested cormorants (Phalacrocorax auritus) and Caspian terns (Hydroprogne caspia) from the upper Great Lakes in 1988

Persistent organochlorine contaminants including polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs) and polychlorinated biphenyls (PCBs) were determined in eggs with normal and deformed embryos collected in 1988 from different colonies during an epizootiological survey of double-crested cormorants (Phalacrocorax auritus) and Caspian terns (Hydroprogne caspia) from the upper Great Lakes. PCBs and p,p'-DDE were found in the highest concentrations in eggs of both species. The residue pattern of PCB isomers and chlordane compounds suggested that double-crested cormorants have greater metabolic capacity to degrade contaminants than Caspian terns. According to the toxicity evaluation using the 2,3,7,8-TCDD equivalents (TEQs) approach, non-ortho coplanar PCBs contributed much more toxicity than PCDDs and PCDFs. Total TEQ of dioxin-like compounds was likely associated with occurrence of live-deformed embryos in double-crested cormorants eggs. The toxic effects of these contaminants were also estimated in Caspian tern eggs, where elevated levels of coplanar PCBs, PCDDs and PCDFs were observed in concordance with increased rate of anomalies in eggs during a breeding season in the Great Lakes.     

PCDDs, PCDFs, and PCBs concentrations in breast milk from two areas in Korea: body burden of mothers and implications for feeding infants

We determined breast milk concentration of polychlorinated dibenzo-p-dioxins (PCDDs)/polychlorinated dibenzofurans (PCDFs) and polychlorinated biphenyls (PCBs) in 24 mothers living in Korea, and assessed the maternal body burden based on PCDDs/PCDFs and PCBs concentrations in breast milk and an infant intake rate through breast-feeding based on their concentration in breast milk. PCDDs/PCDFs and PCBs levels in breast milk from primipara mothers were found to be higher than those from multipara mothers. For total PCDDs/PCDFs TEQ level, 2,3,4,7,8-PeCDD was the predominant congener, and the proportion of 2,3,7,8-TCDD was less than 3% of total PCDDs/PCDFs TEQ level. For PCBs TEQ level, PCB-126 was the predominant congener. Maternal body burden levels of PCDDs/PCDFs and PCBs based on their concentrations in breast milk were 268-622 TEQ ng. The daily dioxin intakes of mothers were predicted to be 0.78-2.18 TEQ pg/kg/day for PCDDs/PCDFs and 0.34-0.66 TEQ pg/kg/ day for PCBs. For the first year, the body burden of an infant was predicted to be 212 TEQ ng and the daily intake of an infant was predicted to be 85 TEQ pg/kg/day, assuming the mean dioxin-related compounds concentration (27.54 TEQ pg/g fat).     

Concentrations of polychlorinated dibenzo-p-dioxins, polychlorinated dibenzofurans, and non-ortho and mono-ortho polychlorinated biphenyls in blood of Yusho patients

We measured the concentrations of polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), non-ortho polychlorinated biphenyls (non-ortho PCBs) and mono-ortho polychlorinated biphenyls (mono-ortho PCBs) in blood collected from 279 Yusho patients living in Japan, 92 Yusho-suspected persons living in Japan and 127 normal controls living in Fukuoka Prefecture, and compared among the groups in terms the concentrations of these compounds. The total toxic equivalents (TEQ) concentrations of PCDDs, PCDFs, non-ortho PCBs, and mono-ortho PCBs in the bloods of Yusho patients and Yusho-suspected persons were 161.4 and 51.2 pg TEQ/g lipid, respectively and were about 3.5 and 1.1 times higher than those of normal controls, respectively. Although the TEQ concentrations of PCDDs, non-ortho PCBs, and mono-ortho PCBs among Yusho patients, Yusho-suspected persons and normal controls were nearly the same, the PCDFs levels of Yusho patients were significantly higher than those of Yusho-suspected persons and about 10.3 times higher than those of normal controls. In Yusho patients, PCDFs contributed about 65% to the total TEQ concentration. Among the PCDFs congeners for Yusho patients, the concentration of 2,3,4,7,8-pentachlorodibenzofuran (PeCDF) was about 11.3 times higher than that of normal controls. These findings indicated that Yusho patients even now, more than 34 years after the outbreak of Yusho, have much higher blood levels of 2,3,4,7,8-PeCDF in general than do unaffected persons.     

Levels of PCDDs, PCDFs, and PCBs in the blood of the non-occupationally exposed residents living in the vicinity of a chemical plant in the Czech Republic

In 2003, concentrations of altogether 17 PCDD/Fs congeners and 12 non-ortho and mono-ortho dioxin-like PCBs were measured in the blood of 60 randomly selected adults who lived in three settlements surrounding a chemical plant that had been producing chlorinated herbicides (mainly HCHs, HCB, pentachlorophenole, 2,4,5-T) in the 1960's; subjects consuming home-produced animal foods were chosen. Twenty blood donors with similar characteristics from the locality with about 80 km distance were used as control subjects. The factors that influenced the dioxin levels were investigated on the basis of a questionnaire. The aim of our study was to find out whether the residents living in the surroundings of the chemical plant are at a greater exposure risk than the controls. To calculate TEQ values, WHO-TEFs were used. The concentrations of four PCDD and six PCDF congeners were below the LOD in more than 50% of samples. Significantly higher WHO-TEQ levels (p<0.05) were found for PCDDs, PCDFs, or PCBs in all three followed up groups compared with controls. The geometric means of the total TEQ values for PCDD/F/PCBs were 43.8, 50.2, and 40.0 pg/g fat compared to 23.2 pg/g fat in the control. The percentages of TEQ due to the measured congeners in exposed groups were 9-10.3% for PCDDs, 20.5-26.9% for PCDFs, 19.2-23.1% for coplanar and 43.6-47.2% for mono-ortho PCBs. In control, the percentage of TEQ was 11.6, 26.7, 24.1, and 37.5%. PCBs, predominantly PCB156, followed by PCB126 contributed 60 to 70% of the total TEQ value. Positive correlation of the PCDD/PCDF/PCB blood levels with age and with consumption of locally produced eggs was found.     

Concentration of polychlorinated dibenzo-p-dioxins, polychlorinated dibenzofurans and dioxin-like PCBs in human adipose tissue from Turkish men

There is no previous report from Turkey on chemically determined polychlorinated dibenzo-para-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), and dioxin-like polychlorinated biphenyls (PCBs) in human tissues expressed as World Health Organization (WHO) toxic equivalents (TEQs). The objective of this study was to determine the occurrence of PCDDs/Fs, and dioxin-like PCBs in the general adult Turkish population. For this reason we measured adipose tissue concentrations of PCDDs/Fs and dioxin-like PCBs in 23 Turkish men living in Ankara,Turkey in 2004. PCDD/F concentrations ranged between 3.2 and 19.7 pg WHO-TEQ/g fat (5.34 and 42.7 WHO-TEQ/g fat, respectively, including dioxin-like PCBs). The mean concentrations of WHO(PCDD/F)-TEQ and WHO(PCB)-TEQ were 9.2 and 6.67 pg/g on a lipid basis , respectively. Samples were analyzed for PCDD/F and twelve dioxin-like PCB congeners using high resolution gas chromatography/high resolution mass spectrometry (HRGC/HRMS). This study is very important since it is the first report on PCDDs/Fs and dioxin-like PCB contamination in human adipose tissue from Turkey.     

Leaching characteristics of PCDDs/DFs and dioxin-like PCBs from landfills containing municipal solid waste and incineration residues

To investigate the leaching characteristic of persistent organic pollutants (POPs), such as non-ortho and mono-ortho substituted chlorobiphebyls (dioxin-like PCBs), polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDDs/DFs), in leachate from municipal solid waste (MSW) landfill sites containing incineration residues, raw leachate samples were collected twice from 12 selected MSW landfill sites. The samples were divided into their liquid and solid phases using GF/B (pore size 1.0 microm), and the concentrations of POPs then determined. The concentrations of PCDDs/DFs ranged from 0.65 to 5.88 pg-TEQ/l (average 2.86 pg-TEQ/l), and those of dioxin-like PCBs from 0.05 to 0.32 pg-TEQ/l (average 0.18 pg-TEQ/l). The major congeners of leached PCDDs/DFs and dioxin-like PCBs in liquid and solid phases were OCDD (about 60%), 2,3',4,4',5-PeCBs (about 30%), and 2,3,4,4',5-PeCBs (about 54%). The relationship between landfill age and the leaching concentration of PCDDs/DFs, and effects of dissolved organic carbon (DOC) on the leaching of PCDDs/DFs are also discussed. Finally, a leaching prediction model of PCDDs/DFs from MSW landfills has been suggested using parameters, such as hydrophobic neutral organic carbons, total dissolved solid, and the ratio of non-biodegradable wastes in landfill sites.     

Update of daily intake of PCDDs, PCDFs, and dioxin-like PCBs from food in Japan

Total diet study (TDS) samples of 14 food groups from 16 locations in Japan, collected in 1999 and 2000, were analyzed for polychlorinated dibenzo-p-dioxins (PCDDs), dibenzofurans (PCDFs), and dioxin-like polychlorinated biphenyls (dioxin-like PCBs) to estimate the update of daily intake of these contaminants from food. The mean daily intake of toxic equivalency (TEQ) for an adult weighing 50 kg, calculated at non-detected isomer concentrations equal to zero (ND=0), was estimated to be 2.25 pg TEQ/kg b.w./day. When non-detected isomer concentrations are assumed to be equal to half of the limits of detection (ND=1/2 LOD), the mean daily intake was estimated to be 3.22 pg TEQ/kg b.w./day. These values were below the tolerable daily intake (TDI) of 4 pg TEQ/kg b.w. for PCDD/Fs and dioxin-like PCBs set in Japan. In both the estimates, the mean daily intakes were highest from fish and shellfish (76.9% at ND=0 and 53.9% at ND=1/2 LOD of the total TEQs), followed by those from meat and eggs (15.5% at ND=0 and 11.7% at ND=1/2 LOD of the total TEQs). Congener specific data revealed that these total TEQ levels were dominated by 1,2,3,7,8-PeCDD, 2,3,4,7,8-PeCDF and 3,3^′,4,4^′,5-PeCB in each case (71.7% at ND=0 and 63.1% at ND=1/2 LOD of the total TEQs). The dioxin-like PCBs (non-ortho and mono-ortho PCBs) accounted for about 50% of these total TEQs. These data will be very useful in the risk assessment of PCDD/Fs and dioxin-like PCBs from food in Japan.     

Distribution of PCDDs, PCDFs and dioxin-like PCBs in the blood, testis and adipose tissue of suckling beef calves

To determine the distribution of persistent organochlorine compounds in beef cattle, concentrations of 2,3,7,8-substituted PCDDs, PCDFs and dioxin-like PCBs were measured in the blood, testes and adipose tissue of four two-month-old Japanese Black calves. Of 29 congeners analyzed, 19, 20 and 28 were detected in the blood, testes and adipose tissue, respectively, of three or all calves. Total toxic equivalents (TEQs) were similar in the testes and adipose tissue, and approximately two times higher than in the blood on a lipid weight basis (P<0.05). More PCDDs and PCDFs had accumulated in the testes than in adipose tissue (P<0.01), but more dioxin-like PCBs were found in adipose tissue than in the testes (P<0.0001). Accumulation patterns in the testes and adipose tissue varied among the congeners of PCDD and PCDF, whereas the patterns were similar in dioxin-like PCBs. In particular, highly substituted PCDD congeners were detected at high concentrations in the testes but at lower concentrations in adipose tissue compared with other congeners. By contrast, accumulation levels of highly substituted PCDFs were lower in both those tissues than the other congeners. In conclusion, it was demonstrated that PCDDs, PCDFs and dioxin-like PCBs leave the circulation and accumulate in the testes and adipose tissue in bovine calves. It was suggested that congeners of PCDD, especially highly substituted PCDDs, and PCDFs have a tendency to accumulate in the testis and dioxin-like PCB congeners accumulate readily in adipose tissue.     

Relevance of coplanar PCBs for TEQ emission of fluidized bed incineration and impact of emission control devices

Five fluidized bed incinerators combusting municipal solid waste were assessed for the impact of coplanar PCBs on total TEQ emission. In 17 stack measurements, the coplanar PCBs contributed on average less than 3% to total TEQ with a maximum contribution of 7.5% to total TEQ in one measurement. Differences in the design of the flue gas cooling section did not show an effect on the impact of coplanar PCBs on total TEQ. The effect of emission control devices on the impact of coplanar PCBs on the total TEQ was studied in more detail at one incinerator. The relative contribution of PCBs to total TEQ increased along the flue gas line. This was caused by a slightly higher removal efficiency for TEQ relevant PCDDs/PCDFs compared to coplanar PCBs by the bag filters and a higher destruction efficiency for PCDDs/PCDFs compared to PCBs by the SCR catalyst. Additionally, the removal efficiencies of the emission control devices (bag filters and catalyst) for other chlorinated aromatic compounds which have been proposed as TEQ indicator compounds (polychlorinated benzenes and polychlorinated phenols) were compared with those for PCDDs/PCDFs and coplanar PCBs. Removal efficiencies for polychlorinated benzenes or polychlorinated phenols considerably differed from those of PCDD/PCDF and coplanar PCBs. Implications for TEQ assessments using indicator compounds as proposed in the literature are discussed.     

Detailed study on the levels of polychlorinated dibenzo-p-dioxins,polychlorinated dibenzofurans and polychlorinated biphenyls in Yusho rice oil

One bottle of Yusho rice oil was obtained from a Yusho family in 1998. The levels of polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs) and polychlorinated biphenyls (PCBs) in the causal oil were investigated with two different approaches and the individual concentrations of all the 17 2,3,7,8-substituted PCDD/F and 14 coplanar PCB (Co-PCB) congeners were elucidated for the first time. The concentrations of PCDDs and PCDFs were found to be 0.60 and 8.8 ppm, respectively. For PCBs, more than 130 PCB peaks were observed and a total concentration of 850 ppm including 170 ppm of Co-PCBs was obtained. The toxic equivalents (TEQs) of PCDDs, PCDFs, and Co-PCBs were calculated to be 17, 470, and 120 ppb, respectively. The relative contribution of these classes to the total TEQ in Yusho oil is 3%, 77%, and 20%, respectively, indicating that PCDFs play a major role in the toxicity of Yusho oil. Furthermore, it was confirmed that 2,3,4,7,8-penta-CDF contributes 58% to the total TEQ, supporting the view that this compound is the principal causal agent in Yusho poisoning. It is noteworthy that the most toxic 2,3,7,8-tetra-CDD was newly discovered, although it contributes only 0.1% to the total TEQ. Based on our data, the smallest TEQ intake during the latent period was estimated to be 0.067 mg for Yusho patients. This value is about 60% of that previously reported, suggesting a lower minimum threshold level for the development of the toxic symptoms of Yusho.     

Differential uptake for dioxin-like compounds by zucchini subspecies

The zucchini (Cucurbita pepo) cultivars 'Patty Green', 'Black Beauty', and 'Gold Rush' were cultivated on weathered dioxin-contaminated soil in pots, and concentrations of the 29 dioxin-like compounds that were assigned WHO-TEFs, three non-toxic polychlorinated dibenzo-p-dioxins/dibenzofurans (PCDD/Fs), and two non-dioxin-like polychlorinated biphenyls (PCBs) were analyzed. Toxic equivalent (TEQ) values accumulated in 'Black Beauty' and 'Gold Rush' were about 180 times higher than those in 'Patty Green'. The bioconcentration factor (BCF) based on total mass concentration of the twelve dioxin-like PCBs was higher than those of the seven PCDDs and ten PCDFs in all the cultivars. The BCFs for PCDD and PCDF congeners were negatively correlated with octanol-water partition coefficients in all the plants. No correlations were observed in PCB congeners in the high accumulators, although in 'Patty Green' the BCFs for PCB congeners were significantly correlated with octanol-water partition coefficients. Our findings suggest that the high accumulators had unknown, unique mechanisms for uptake of PCBs, whereas PCDDs and PCDFs were absorbed based on their physicochemical properties.     

Accumulation features and temporal trends of PCDDs, PCDFs and PCBs in Baikal seals (Pusa sibirica)

This study investigated the accumulation features and temporal trends of PCDD/Fs, dioxin-like PCBs (DL-PCBs) and non-dioxin-like PCBs (NDL-PCBs) in the blubber of Baikal seals collected in 1992 and 2005. DL-PCBs (480-3600 ng/g) and NDL-PCBs (980-35,000 ng/g) were dominant contaminants. Concentrations of PCDDs and PCBs in males were significantly higher than in females. In males, age-dependent accumulation was observed for PCDDs, mono-ortho PCBs and NDL-PCBs. PCDFs and non-ortho PCBs showed no such trends, implying that exposure of seals to these contaminants has been decreasing in recent years. No decreasing temporal trend was observed for PCDDs, mono-ortho PCBs and NDL-PCBs, suggesting that Baikal seals are still exposed to PCDDs and PCBs. TEQs of PCDDs and mono-ortho PCBs in seals collected in 2005 accounted for 62-77% of total TEQs. The TEQ levels in 40% of the specimens exceeded the threshold level for immunosuppression observed in harbor seals (209 pg/g).