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.     

Blood levels of PCDDs,PCDFs, and coplanar PCBs in Yusho mothers and their descendants: Association with fetal Yusho disease

Maternal exposure to polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), and polychlorinated biphenyls (PCBs) may result in adverse health effects in their children. In Japan in 1968, an accidental human exposure to rice oil contaminated with PCDDs, PCDFs, and PCBs, led to the development of Yusho disease. Yusho mothers delivered descendants with low birth weights and hyperpigmented skin and mucosa, which are characteristic of fetal Yusho disease (FYD). The Yusho cohort was used to evaluate the effect of maternal exposure to PCDDs, PCDFs, and PCBs on the development of FYD. Blood samples, obtained from 64 Yusho mothers (117 descendants: 10 with FYD and 107 without FYD), were analyzed for congeners of seven PCDDs, 10 PCDFs, and four coplanar PCBs. We investigated the association between the maternal estimated blood levels of dioxins at delivery and the risk of fetal Yusho disease. We also studied the differences in dioxin blood levels in 24 mother–descendant pairs (5 with FYD and 19 without FYD). The estimated levels of total PCDD TEQ, total PCDF TEQ, total coplanar PCB TEQ, and total TEQ in the maternal blood at delivery were associated with significantly increased risk of FYD. The odds ratios, which present the risk of FYD for a 10-fold increase in blood dioxin, were largest for 1,2,3,6,7,8-HexaCDD (odds ratio = 28.6, 95% confidence interval = 1.67–489.9, p = 0.02). The levels of 1,2,3,6,7,8-HexaCDD in both the Yusho mothers and their descendants with FYD were higher than the levels in those without FYD. These findings suggest that 1,2,3,6,7,8-HexaCDD is the most important causative congener for the development of FYD.     

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.     

Polychlorinated biphenyls and dibenzofurans retained in the tissues of a deceased patient with Yucheng in Taiwan

Various tissues from a deceased Yucheng (oil disease) patient were analyzed for individual polychlorinated biphenyl (PCB) and dibenzofuran (PCDF) congeners. With a few exceptions, PCBs with 5 or less chlorine atoms were almost completely excreted from the patient's tissues about two years after the ingestion of the toxic oil. In contrast, most PCB congeners with 6 or more chlorine atoms were retained in the tissues. The intestinal fat contains the highest level of PCBs while the liver contains the highest concentration of PCDFs. The major PCDF congeners retained in the tissues were 1,2,3,4,7,8-hexaCDF, 2,3,4,7,8-pentaCDF, and 1,2,4,7,8-pentaCDF. The former two congeners, especially 2,3,4,7,8-pentaCDF, are very toxic PCDFs; they may play important roles in the etiology of Yucheng.     

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).     

Comparative toxicities of the polychlorinated dibenzofuran (PCDF) and biphenyl (PCB) mixtures which persist in Yusho victims

The toxic Yusho oil contained a mixture of polychlorinated biphenyls (PCBs) which were contaminated by other halogenated aromatics including the highly toxic polychlorinated dibenzofurans (PCDFs). It has been reported that the PCBs and PCDFs which persist in the liver of victims still suffering from Yusho poisoning include the following compounds; 2,3′,4,4′,5-penta-,2,2′,4,4′,5,5′-,2,2′,3′,4,4′,5- and 2,3,3′,4,4′,5-hexa, 2,2′,3,4,4′,5,5′- and 2,2′,3,3′,4,4′,5-heptachlorobiphenyls and the 2,3,7,8-tetra-, 1,2,4,7,8-, 1,2,3,7,8- and 2,3,4,7,8-penta- and 1,2,3,4,7,8-hexachlorodibenzofurans. All of these PCBs and PCDFs have been synthesized and reconstituted to approximate their composition in human liver. A comparison of the dose-response effects of the reconstituted PCB and PCDF mixtures in causing weight loss, thymic atrophy and the induction of cytochrome P-448-dependent monooxygenases indicated that the PCDF mixture was at least 700 times more active than the PCBs. Since the ratio of PCBs/PCDFs persisting in Yusho patients' blood and liver was less than 600:1 and 5:1 respectively, the results suggest that the PCDFs are the major etiologic agent in Yusho poisoning.     

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

We measured the concentrations of polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), dioxin-like polychlorinated biphenyls (PCBs), and non-dioxin-like PCBs in paired samples of blood and breast milk collected from 67 secundiparas in Sapporo City, Japan, and combined this data with those of the 30 secundiparas previously measured. The arithmetic mean total toxic equivalents (TEQ-WHO) concentrations of PCDDs, PCDFs, non-ortho PCBs, and mono-ortho PCBs in blood and breast milk of the 97 secundiparous subjects were 3.0-23 (mean: 13, median: 14) and 2.7-20 (mean: 8.6, median: 8.5) pg TEQ g⁻¹ lipid, respectively. The sums of the concentrations of 56 non-dioxin-like PCB congeners that were measured in the subjects’ blood and breast milk were 16-326 (mean: 107, median: 100) and 12-252 (mean: 73, median: 67) ng g⁻¹ lipid, respectively. The partitioning ratios of individual congeners of PCDDs, PCDFs, dioxin-like PCBs, and non-dioxin-like PCBs from blood to breast milk in secundiparas were almost the same as those of primiparas that have been recently reported, suggesting that the partitioning ratios of these compounds from maternal blood to breast milk in women is little affected by delivery. Furthermore, the partition of PCB congeners with chlorine at the 2-, 3-, 4′-, and 5-positions or the 2-, 4-, 4′-, and 5-positions of the biphenyl ring from the blood to the breast milk tended to occur at a higher level than that of other congeners. In particular, the levels of tetraCB-74 and hexaCB-146 in the breast milk for both primiparous and secundiparous mothers were slightly higher than those in the blood.     

Congener profiles of PCDDs, PCDFs, and dioxin-like PCBs in the breast milk samples in Tokyo, Japan

Exposure to dioxins has raised much public concern recently. We determined the congeners' distribution of polychlorinated-dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs) and dioxin-like polychlorinated biphenyls (dl-PCBs) in the breast milk samples collected in Tokyo, Japan. Breast milk was taken from 240 mothers, 30 days after delivery in 1999 and 2000 in Tokyo, Japan. The actual concentration and TEQ concentration of PCDDs (14 congeners), PCDFs (15 congeners), and dl-PCBs (12 congeners), and each congener's contribution to the total TEQ level were calculated. Among all the samples, PCDDs accounted for 34.8%, PCDFs accounted for 23.5%, dl-PCBs accounted for 41.7%, which was also similar in the breast milk from the primiparae and secundiparae. The main contributors to the total TEQ with increasing percentages were 2,3,4,7,8-PeCDF, 1,2,3,7,8-PeCDD and 3,3',4,4',5-PCB (#126), and they accounted for more than 65% of the total TEQ. Detailed congener analysis in breast milk samples is effective to understand dioxin sources.     

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.     

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

We measured the concentrations of polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), dioxin-like polychlorinated biphenyls (PCBs), and non-dioxin-like PCBs in paired samples of blood and breast milk collected from 67 secundiparas in Sapporo City, Japan, and combined this data with those of the 30 secundiparas previously measured. The arithmetic mean total toxic equivalents (TEQ-WHO) concentrations of PCDDs, PCDFs, non-ortho PCBs, and mono-ortho PCBs in blood and breast milk of the 97 secundiparous subjects were 3.0–23 (mean: 13, median: 14) and 2.7–20 (mean: 8.6, median: 8.5) pg TEQ g⁻¹ lipid, respectively. The sums of the concentrations of 56 non-dioxin-like PCB congeners that were measured in the subjects’ blood and breast milk were 16–326 (mean: 107, median: 100) and 12–252 (mean: 73, median: 67) ng g⁻¹ lipid, respectively. The partitioning ratios of individual congeners of PCDDs, PCDFs, dioxin-like PCBs, and non-dioxin-like PCBs from blood to breast milk in secundiparas were almost the same as those of primiparas that have been recently reported, suggesting that the partitioning ratios of these compounds from maternal blood to breast milk in women is little affected by delivery. Furthermore, the partition of PCB congeners with chlorine at the 2-, 3-, 4′-, and 5-positions or the 2-, 4-, 4′-, and 5-positions of the biphenyl ring from the blood to the breast milk tended to occur at a higher level than that of other congeners. In particular, the levels of tetraCB-74 and hexaCB-146 in the breast milk for both primiparous and secundiparous mothers were slightly higher than those in the blood.     

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.     

Polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs) and polychlorinated biphenyls (PCBs) in breast milk of first-time Irish mothers: impact of the 2008 dioxin incident in Ireland

The 2008 dioxin incident in Ireland resulted in elevated concentrations of polychlorinated dibenzo-p-dioxins (PCDDs), dibenzofurans (PCDFs) and polychlorinated biphenyls (PCBs) in Irish pork and pork products, due to the consumption of contaminated animal feed by pigs. In order to investigate any resulting impact on the Irish population, these contaminants were measured in pooled breast milk samples from 109 first-time mothers, collected in 2010. A comparison of the results with similar data from 2002 revealed generally lower concentrations of PCDD/Fs and dioxin-like PCBs in the 2010 samples, confirming the declining trend reported by many authors. Contaminant concentration levels for both 2002 and 2010 were generally slightly lower than those reported internationally, with a mean combined PCDD/F and PCB WHO-TEQ of 9.66 pg g⁻¹ fat, for an overall pooled sample of milk from 2010. An apparent slight increase in PCDFs was observed between 2002 and 2010 (from 2.73 pg WHO-TEQ g⁻¹ fat to 3.21 pg WHO-TEQ g⁻¹ fat), with the main contributory congener being 2,3,4,7,8-PentaCDF. While it cannot be totally discounted that the slight increase in 2,3,4,7,8-PentaCDF and in the overall PCDF WHO-TEQ in breast milk could be attributable to consumption of Irish pork during the 2008 incident, we consider that it is more likely that this was due to other factors, including the predominantly urban/industrial sampling locations for the 2010 samples, compared to 2002.     

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.     

Trend studies of polychlorinated biphenyls, dibenzo-p-dioxins and dibenzofurans in human milk

Human milk has been used in studies of long-term changes in the concentrations of organochlorine contaminants in mothers from the Stockholm region. The previously observed decline (1972 to 1985) in the levels of polychlorinated biphenyls (PCBs), dibenzo-p-dioxins (PCDDs) and dibenzofurans (PCDFs) seems to have ceased for certain compounds since the levels were about the same in samples collected in 1985 and 1989. Calculating with the proposed toxicity equivalency factors for the different congeners of PCDDs, PCDFs and PCBs it is seen that the congeners of PCBs contribute more to the possible toxicity than those of PCDDs and PCDFs. The mono-ortho substituted congener 2,3′,4,4′,5-pentachlorobiphenyl (IUPAC No. 118) contributes with the largest part.     

Persistent organochlorines in the serum of the non-occupationally exposed New Zealand population

Concentrations of polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), polychlorinated biphenyls (PCBs), and organochlorine pesticides were measured in the serum of a sample of the New Zealand population aged 15 years and older. This was the first study to obtain representative measures of PCDDs, PCDFs and PCBs in the adult population of an entire country. Serum samples were obtained in 1996-1997. Potentially occupationally exposed individuals were excluded. Serum samples were pooled according to stratification criteria for area of residence, ethnicity, age, and sex. Of the 80 possible strata, sufficient serum for chemical analysis was available for 60, to which 1,834 individual samples contributed. For the PCDDs and PCDFs, most 2,3,7,8-chlorinated congeners were measured in all strata, with a mean toxic equivalents concentration across all strata of 12.8 ng TEQ kg(-1) lipid. Seven PCB congeners were frequently measured, including the coplanar congeners #126 and #169, quantified in all strata. Of the pesticides and their metabolites, only beta-HCH, dieldrin and pp'-DDE were consistently detected across strata. There was a general trend of increasing concentration with age. There were no consistent differences between the sexes, or between people of Maori (the indigenous people of New Zealand) and non-Maori ethnicity. Concentrations of PCDDs and PCDFs tended to increase in a North-South direction, possibly reflecting greater levels of industrialization and population concentration, and concentrations of the pesticide products were highest in the South, possibly reflecting historical use patterns. Results were consistent with a recent study of concentrations of these compounds in the milk of first-time mothers.     

Concentrations of dioxins and related compounds in the blood of Fukuoka residents

Blood samples of 152 residents (male 75 and female 77) aged 20-60 years in Fukuoka, Japan, were analyzed for dioxin toxic compounds of polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), non-ortho polychlorinated biphenyls (non-ortho PCBs) and mono-ortho polychlorinated biphenyls (mono-ortho PCBs) as well as 35 PCB congeners and 12 chlorinated pesticides by high-resolution gas chromatography/high-resolution mass spectrometry. Average concentrations of dioxin toxic equivalents (TEQ) from PCDDs, PCDFs, non-ortho PCBs, mono-ortho PCBs and their total in the blood of 152 residents were 10.28, 5.56, 7.75, 4.57 and 28.15 ppt in lipid, respectively. These total TEQ levels were comparable to the blood TEQ levels of normal Japanese (n=735). Lipid basis total TEQ levels progressively increased in the males from 17.1 ppt at age 20s to 47.5 ppt at age 50s and in the females from 19.5 ppt at age 20s to 54.5 ppt at age 50s. Dioxin toxic contribution of PCBs to total TEQ was increased from 31% at age 20s to 55% at age 50s. Average concentrations of total 35 PCBs and total 12 pesticides in the blood of 151 residents were 386 and 1079 ppb in lipid, respectively. Average concentrations (ppb in lipid) of total PCBs and total pesticides also progressively increased in the males from 213 and 444 at age 20s to 868 and 2140 at age 50s, respectively, and in the females from 199 and 588 at age 20s to 550 and 1977 at age 50s, respectively. The levels of TEQ, PCBs, hexachlorobenzene, beta-hexachlorocyclohexane, dieldrin, p,p'-dichlorodiphenyldichloroethylene, p,p'-dichlorodiphenyltrichloroethane, trans-nonachlor and cis-nonachlor were positively correlated with each other in most of the combinations, and the highest correlations (r>0.8) were observed between total TEQ and PCBs in both sexes.     

Apportionment of TEQs from four major dioxin sources in Japan on the basis of five indicative congeners

The major sources of dioxins (polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), and dioxin-like polychlorinated biphenyls (DL-PCBs)) in the environment in Japan have been considered to be combustion by-products, pentachlorophenol (PCP) formulations, chlornitrofen (CNP, 4-nitrophenyl-2,4,6-trichlorophenyl ether) formulations, and PCB products. Data on PCDDs, PCDFs and DL-PCBs from the four sources were analyzed, and indicative congeners whose concentrations were highly correlated with WHO-2006 toxic equivalencies (TEQs) were identified for each source sample. The indicative congeners for combustion by-products, PCP formulations, and CNP formulations were 2,3,4,7,8-pentachlorodibenzofuran, 1,2,3,4,6,7,8-heptachlorodibenzo-p-dioxin, and 1,2,3,7,8-pentachlorodibenzo-p-dioxin, respectively; for PCB products, the indicative congeners were IUPAC Nos. #126- and #105-pentachlorobiphenyls. Moreover, using the data on PCDDs, PCDFs and DL-PCBs, we developed a set of equations for estimating the apportionment of TEQs from the four sources by using only the concentrations of the above-mentioned five indicative congeners. The equations were used along with the analysis results of different types of environmental samples collected from Japan, to determine the TEQ contributions of the four sources. The obtained values of TEQ contributions seemed to be reasonable. The estimation method was developed by using the data on major dioxin sources in Japan, and therefore, it is generally adaptable to environmental samples from any part of Japan. The method may be usable for regions outside Japan if source identification is carried out and the estimation equations are modified appropriately.     

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.     

Relative importance of polychlorinated naphthalenes compared to dioxins, and polychlorinated biphenyls in human serum from Korea: Contribution to TEQs and potential sources

Polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), and polychlorinated biphenyls (PCBs) in human have been studied extensively; however, polychlorinated naphthalenes (PCNs) have been studied less widely. The mean concentrations of PCNs, PCDDs, PCDFs, and PCBs in 61 healthy human volunteers were 2170 pg/g lipid, 452 pg/g lipid, 116 pg/g lipid, and 120 ng/g lipid respectively, and the mean toxic equivalents (TEQs) contributed by PCNs, PCDDs, PCDFs, and PCBs were 5.88, 5.22, 5.48, and 5.33 pg/g lipid, respectively. PCNs contributed to 26.8% of the total TEQs. 1,2,3,7,8-PeCDD, 2,3,4,7,8-PeCDF, PCB126, and hepta-CN-73 accounted for >62% of the total TEQs in the human serum samples. The overall serum PCN homologue profiles of all subjects were dominated by tetra- and penta-CN homologues, and the most predominant individual congener was hepta-CN-73, which contributed 17.5% of the total serum PCN concentration. Enrichment of hepta-CN-73 in the human serum samples might be due to contributors from combustion sources.     

Comparison between "Yusho" patients and healthy Japanese in contamination level of dioxins and related chemicals and frequency of sister chromatid exchanges

Highly toxic organochlorine chemicals such as polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs) and coplanar polychlorinated biphenyls (CoPCBs) were determined in the peripheral blood and sebum from the face of 16 "Yusho" patients of about 27 yr after the outbreak of Yusho accident, and 39 healthy Japanese people. The mean total toxic equivalent (TEQ) levels of PCDDs, PCDFs and CoPCBs in the blood were still about seven times higher in Yusho patients than in healthy Japanese at the age of 45 yr and more. The sebum excretion of these chemicals seemed proportional to their blood levels in Yusho patients. These toxic chemicals, however, did not enhance frequencies of sister chromatid exchanges (SCEs) in the control and 7,8-benzoflavone (ANF) treated cultures in Yusho patients. Hence, no significant difference was observed in the mean SCE rates between the Yusho patients and general Japanese people of more than 45 yr of age. In this study, the number of Yusho patients examined is limited, so further large-scale investigations are needed to get more conclusive results concerning the genotoxic potency such as SCE induction.