Contrasting retinoid and thyroid hormone status in differentially-contaminated northern fulmar colonies from the Canadian Arctic,Svalbard and the Faroe Islands

The northern fulmar (Fulmarus glacialis) has previously been shown to accumulate a wide range, and occasionally high concentrations of organochlorines (OCs) (e.g., PCBs, chlorobenzenes, DDT- and chlordane-related compounds, dioxins and furans). The present study aimed to investigate, using a meta-analysis approach, the variations in cytochrome P450 (CYP) 1A-like enzyme induction based on ethoxyresorufin O-deethylase activity (EROD) and selected physiological variables (retinoids and thyroid hormones) in northern fulmar breeding in three differentially OC-exposed populations: Nunavut (Canadian Arctic), Svalbard (Norwegian Arctic) and the Faroe Islands. Substantially higher (roughly two-fold) OC levels were uncovered in the liver of this long-lived fulmarine petrel breeding in the Faroe Islands relative to Svalbard and Nunavut. Liver levels of PCDDs, PCDFs and non-ortho PCBs in Faroe Islands fulmars were amongst the highest reported thus far in any seabirds from the northern regions. Positive correlations were depicted in combined fulmars (all three populations) between hepatic EROD activity and concentrations of OCs, in which strongest associations were found for dioxin-like compound (PCDFs and PCDDs) and TEQ concentrations. Moreover, moderate to strong positive correlations were found between liver OC concentrations and plasma total thyroxin (TT₄) levels and TT₄/total triiodothyronine (TT₃) level ratios, as well as strong negative correlations between the same suite of OCs and plasma TT₃ levels. Hepatic OC concentrations (PCBs, PCDDs, PCDFs, HCB, p,p'-DDE and oxychlordane) also were positively correlated with hepatic retinyl palmitate levels which, in turn, were associated with a significant decrease in plasma retinol levels and somewhat unchanged liver retinol levels. The present meta-analysis investigation on northern fulmar breeding in three geographically-distant sites illustrated that OC exposure (mainly PCBs and dioxins/furans) may be associated with modulation of the thyroid and retinoid homeostasis. However, the impact of confounding environmental factors (e.g., temperature and nutritional status) on current physiological variable variations could not be ruled out, and thus any cause-effect linkages between thyroid and retinoid system perturbation and OC exposure cannot be ascertained.     

The effect of in utero exposure to dioxins and polychlorinated biphenyls on reproductive development in eight year-old children

We have previously reported on the effects of in utero exposure to polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) and polychlorinated biphenyls (PCBs) on thyroid function and growth hormone concentrations at birth and in two and five year-old children. Herein, we present our most recent follow-up examination findings for the same cohort of children at eight-years of age. A total of 56 children (23 boys, 33 girls) were examined. Bone age (BA), hormone concentrations, and indicators of reproductive development including Tanner, breast, genital, and armpit stages were assessed. Estradiol concentrations were significantly lower in children exposed to higher levels than median of PCDD/Fs + PCBs TEQ compared to the children exposed to levels lesser than median (P = 0.003). Girls exposed to higher levels than median of indicator PCBs had a significantly greater proportion in genital stage 1 and shorter fundi and uteri lengths, as compared to those exposed to low levels (P = 0.025 and P < 0.05, respectively). There was a significant negative relationship between estradiol concentrations and PCDD/Fs + PCB exposure level (P = 0.005). After adjusting for BA, there was a significant association between fundus length and indicator PCB exposure level (P = 0.034). Exposure to both high levels of ΣPCDD/Fs + PCBs TEQ and high levels of total PCBs was associated with decreased fundus length (P = 0.016) and uterus length (P = 0.016). In utero exposure to high levels of PCDD/Fs and PCBs may result in lower estradiol concentrations in eight year-old children and impaired reproductive development in girls.     

Yusho and its latest findings—A review in studies conducted by the Yusho Group

The Yusho incident is an unprecedented mass food poisoning that occurred in Japan in 1968. It was caused by the ingestion of rice bran oil contaminated with polychlorinated biphenyls (PCBs) and various dioxins and dioxin-like compounds, such as polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs). The victims of Yusho have suffered from characteristic skin manifestations associated with systemic, ophthalmological, and mucosal symptoms for a long period of time. The Study Group of Yusho (the Yusho Group) has been conducting annual medical check-ups on Yusho victims for more than 45 years. Since 2002, when concentrations of dioxins in the blood of Yusho patients started to be measured, the pharmacokinetics of dioxins, relationship between blood levels of dioxins and symptoms/signs in patients directly exposed to dioxins, and the adverse effects on the next generation have become dramatically clear. Herein we review recent findings of studies conducted by the Yusho Group to evaluate chronic dioxin-induced toxicity to the next generation as well as Yusho patients in comparison with a similar food mass poisoning, the Yucheng incident. Additionally, we summarized basic studies carried out by the Yusho Group to re-evaluate the mechanisms of dioxin toxicities in experimental models and various functions of the aryl hydrocarbon receptor (AhR), known as the dioxin receptor, pathway.     

Blood levels of dioxins,furans, dioxin-like PCBs,and TEQs in general populations: A review, 1989–2010

A comprehensive worldwide literature review of blood levels of dioxins and dioxin-like compounds in non-exposed adult general populations was performed. The studies published in 1989–2010 reporting information on polychlorinated dibenzo-para-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), non-ortho-PCBs (nPCBs), mono-ortho-PCBs (mPCBs) levels and Toxic Equivalencies (TEQs, a summary weighted measure of their combined toxicity) were reviewed. TEQs were calculated using as standard the most recent WHO 2005 reevaluation of Toxic Equivalency Factors (TEFs). Weighted multiple regression analyses adjusted for year, subject's age, type of sample analyzed, method used for values below detection limit, and central tendency measure used were performed for each congener and standardized TEQs (log-transformed). We identified 187 studies regarding 29,687 subjects of 26 countries. Year of blood collection ranged from 1985 to 2008. The studies reporting congener levels 161. In adjusted analyses, European countries showed higher levels of most dioxin-like congeners and TEQs. A strong positive association of subjects' age with most congeners and with TEQ values was found, confirming previous findings. Significant decreases over time (1985–2008) were documented for PCCDs, PCDFs, and TEQs including their contributions. No significant decrease was found for non-ortho-PCBs, notably PCB 126. Only some mono-ortho-PCBs showed clear significant declines. Accordingly, TEQs including only PCB contribution did not decrease over time. In interpreting these findings, it should be considered that for dioxin-like PCBs the analysis period was shorter (17 years), since these compounds were first measured in 1992.     

Temporal trends of polychlorinated dibenzo-p-dioxins and dibenzofurans and dioxin-like polychlorinated biphenyls in mothers' milk from Sweden, 1972–2011

Temporal trends of polychlorinated dibenzo-p-dioxins (PCDDs), dibenzofurans (PCDFs) and dioxin-like polychlorinated biphenyls (DL-PCBs) in mothers' milk are still quite rare. Data are particularly scarce when it comes to concentrations from the last decade, 2000 and onwards. The aims of the present study were to assess temporal trends of PCDD, PCDF and DL-PCB in mothers' milk from Stockholm, 1972–2011 and to compare the results with previous analysis of some of the older samples.The samples were analyzed by high resolution GC/MS and results were statistically evaluated for the periods, 1972–2011 and 2002–2011. The rate of which ∑PCDDs, ∑DL-PCBs and the ∑TEQ are decreasing (on pg/g fat WHO-TEQ2005) is higher in the last decade compared to the 40 year period, 1972–2011. A similar trend is indicated, but not confirmed, for ∑TEQ of PCDFs, probably due to too many PCDF congeners below LOQ in the period 2002–2011. Concentrations of ∑PCDDs, ∑PCDFs, ∑DLPCBs and ∑TEQ, all expressed as pg/g fat on TEQ-WHO2005-basis, show a statistically significant decline over time, 5.8–6.8% per year, 1972–2011. The last ten years the annual declines for ∑PCDDs, ∑DL-PCBs and ∑TEQ are 9.2–11% and for ∑PCDF, 5.4%. Congener specific trend analysis, 2002–2001, of PCDDs and DL-PCBs showed the same pattern, while the PCDF congeners showed no such general trend. The results from the re-analysis showed good agreement with slightly lower ∑TEQ1998 pg/g fat concentrations in six out of seven samples and mean difference of 13% in ∑TEQ1998. The study shows that time series can be elongated from previous studies, as long as the sample population remains the same.     

Emission factors for PCDD/PCDF and dl-PCB from open burning of biomass

The Stockholm Convention on Persistent Organic Pollutants includes in its aims the minimisation of unintentional releases of polychlorinated dibenzo-dioxins and dibenzofurans (PCDD/PCDF) and dioxin like PCB (dl-PCB) to the environment. Development and implementation of policies to achieve this aim require accurate national inventories of releases of PCDD/PCDF/dl-PCB. To support this objective, the Conference of Parties established a process to review and update the UNEP Standardized Toolkit for Identification and Quantification of Dioxin and Furan Releases. An assessment of all emission inventories was that for many countries open burning of biomass and waste was identified as the major source of PCDD/PCDF releases. However, the experimental data underpinning the release estimates used were limited in number and, consequently, confidence in the accuracy of the emissions predictions was low. There has been significant progress in measurement technology since the last edition of the Toolkit in 2005. In this paper we reassess published emission factors for release of PCDD/PCDF and dl-PCB to land and air.In total, four types of biomass and 111 emission factors were assessed. It was found that there are no systematic differences in emission factors apparent between biomass types or fire classes. The data set is best described by a lognormal distribution. The geometric mean emission factors (EFs) for releases of PCDD/PCDF to air for the four biomass classes used in the Toolkit (sugarcane, cereal crops, forest and savannah/grass) are 1.6 μg TEQ (t fuel)⁻¹, 0.49 μg TEQ (t fuel)⁻¹, 1.0 μg TEQ (t fuel)⁻¹ and 0.4 μg TEQ (t fuel)⁻¹, respectively. Corresponding EFs for release of PCDD/PCDF to land are 3.0 ng TEQ (kg ash)⁻¹, 1.1 ng TEQ (kg ash)⁻¹, 1.1 ng TEQ (kg ash)⁻¹ and 0.67 ng TEQ (kg ash)⁻¹. There are now also sufficient published data available to evaluate EFs for dl-PCB release to air for sugarcane, forest and grass/savannah; these are 0.03 μg TEQ (t fuel)⁻¹, 0.09 μg TEQ (t fuel)⁻¹ and 0.01 μg TEQ (t fuel)⁻¹, respectively. The average EF for dl-PCB release to land is 0.19 ng TEQ (kg ash)⁻¹. Application of these EFs to national emissions of PCDD/PCDF for global estimates from open burning will lower previous estimates of PCDD/PCDF releases to air and to land by 85% and 90%, respectively. For some countries, the ranking of their major sources will be changed and open burning of biomass will become less significant than previously concluded.     

Development and validation of prediction models for blood concentrations of dioxins and PCBs using dietary intakes

BackgroundDioxins and PCBs accumulate in the food chain and might exert toxic effects in animals and humans. In large epidemiologic studies, exposure estimates of these compounds based on analyses of biological material might not be available or affordable.ObjectivesTo develop and then validate models for predicting concentrations of dioxins and PCBs in blood using a comprehensive food frequency questionnaire and blood concentrations.MethodsPrediction models were built on data from one study (n = 195), and validated in an independent study group (n = 66). We used linear regression to develop predictive models for dioxins and PCBs, both sums of congeners and 33 single congeners (7 and 10 polychlorinated dibenzo-p-dioxins and furans (PCDDs/PCDFs), 12 dioxin-like polychlorinated biphenyls (PCBs: 4 non-ortho and 8 mono-ortho), sum of all the 29 dioxin-like compounds (total TEQ) and sum of 4 non dioxin-like PCBs (∑ CB-101, 138, 153, 183 = PCB₄). We used the blood concentration and dietary intake of each of the above as dependent and independent variables, while sex, parity, age, place of living, smoking status, energy intake and education were covariates. We validated the models in a new study population comparing the predicted blood concentrations with the measured blood concentrations using correlation coefficients and Weighted Kappa (К_W) as measures of agreement, considering К_W > 0.40 as successful prediction.ResultsThe models explained 78% (sum dioxin-like compounds), 76% (PCDDs), 76% (PCDFs), 74% (no-PCBs), 69% (mo-PCBs), 68% (PCB₄) and 63% (CB-153) of the variance. In addition to dietary intake, age and sex were the most important covariates.The predicted blood concentrations were highly correlated with the measured values, with r = 0.75 for dl-compounds 0.70 for PCB₄, (p < 0.001) and 0.66 (p < 0.001) for CB-153. К_W was 0.68 for sum dl-compounds 0.65 for both PCB₄ and CB-153. Out of 33 congeners 16 (13 dl-compounds and 3 ndl PCBs) had К_W > 0.40.ConclusionsThe models developed had high power to predict blood levels of dioxins and PCBs and to correctly rank subjects according to high or low exposure based on dietary intake and demographic information. These models underline the value of dietary intake data for use in investigations of associations between dioxin and PCB exposure and health outcomes in large epidemiological studies with limited biomaterial for chemical analysis.     

Global DNA hypermethylation is associated with high serum levels of persistent organic pollutants in an elderly population

Dioxin exposure has experimentally been associated with changes in DNA methylation, an epigenetic change that is associated with disease. The present study aims to investigate if serum levels of dioxin and other persistent environmental pollutants are related to global DNA methylation in a human sample. In the population-based Prospective Investigation of the Vasculature in Uppsala Seniors (PIVUS) study (all aged 70), global DNA methylation was measured by the Luminometric Methylation Assay in 524 subjects. Twenty-three different POPs, including 16 PCBs, five pesticides, one dioxin (OCDD) and one brominated flame retardant (BDE47) were analysed by HRGC/HRMS. Ten single nucleotide polymorphisms (SNPs) in the Aryl hydrocarbon (Ah)-receptor were analysed by mini-sequencing. High levels of toxic equivalency (TEQ) for PCBs and dioxin were associated with DNA hypermethylation (p = 0.030). This was mainly attributed to coplanar non-ortho PCBs. While no significant associations were found between DNA methylation and SNPs in the Ah-receptor, an interaction was found between the SNP rs2237297 and TEQ so that TEQ was associated with hypermethylation (p = 0.009) only in subjects with one G-allele (n = 103). Also high levels of the PCB126 congener, the OCDD, and the pesticide metabolite p,p′-DDE were related to DNA hypermethylation (p = 0.01, 0.03 and 0.003, respectively). In conclusion, in a sample of elderly subjects, high TEQ including PCBs and the dioxin OCDD and high serum levels of PCB126, OCDD, and p,p′-DDE were related to global DNA hypermethylation in a cross-sectional analysis.     

Environmental and lifestyle factors affect benzene uptake biomonitoring of residents near a petrochemical plant

Background

We monitored urinary benzene excretion to examine factors affecting benzene uptake in a sample of the general population living near a petrochemical plant.

Methods

Our study population included 143 subjects: 33 petrochemical plant workers (W) with low level occupational benzene exposure; 30 residents in a small town 2 km from the plant (2kmR); 26 residents in a second small town located 2 to 4 km from the plant (4kmR); and 54 urban residents 25 km from the plant (25kmR). Exposure to benzene was evaluated by personal air sampling during one work-shift for the W group, and from 8.00 to 20:00 for general population subgroups, and by urinary benzene (BEN-U).

Results

Median airborne benzene exposure was 25, 9, 7 and 6 μg/m³ benzene among the W, 2kmR, 4kmR, and 25kmR subgroups, respectively; the highest level was found among the workers, while there was no significant difference among the other groups. Median BEN-U was 2 to 14-fold higher in smokers compared to non-smokers; among non-smokers BEN-U was the highest in W (median 236 ng/L), and lower in the 2kmR (48 ng/L) and 4kmR (63 ng/L) subgroups than in the 25kmR (120 ng/L) subgroup. A multiple linear regression analysis, explaining up to 73% of BEN-U variability, confirmed that active smoking and airborne benzene most strongly affected BEN-U. Among the non-smoking, non-occupationally exposed study subjects, a positive association was found between BEN-U and the distance of residence from the plant. This association was explained by increased exposure to urban traffic emissions in the study group residing at a greater distance from the plant. Environmental tobacco smoke had a marginally positive role.

Conclusion

Among factors affecting benzene uptake in non-occupationally exposed individuals, urban residence contributes to benzene exposure more than residing in close proximity to a petrochemical plant.     

Relative effect potency estimates of dioxin-like activity for dioxins,furans, and dioxin-like PCBs in adults based on cytochrome P450 1A1 and 1B1 gene expression in blood

BackgroundIn the risk assessment of PCDDs, PCDFs, and dioxin-like (DL) PCBs, regulatory authorities support the use of the toxic equivalency factor (TEF)-scheme derived from a heterogeneous data set of the relative effect potency (REPs) estimates.ObjectivesWe sought to determine REPs for dioxin-like compounds (DLCs) using expression of cytochrome P450 (CYP) 1A1 and 1B1 mRNA in human peripheral blood mononuclear cells representing two different pathways.MethodsWe used a sex and age adjusted regression-based approach comparing the strength of association between each DLC and the cytochrome P450 (CYP) 1A1 and 1B1 mRNA expression in 320 adults residing in an organochlorine-polluted area of eastern Slovakia.ResultsWe calculated REPs based on CYP1A1 expression for 4 PCDDs, 8 PCDFs, and 1 PCB congener, and based on CYP1B1 expression for 5 PCDFs and 11 PCB congeners. REPs from CYP1A1 correlated with REPs previously derived from thyroid volume (ρ = 0.85; p < 0.001) and serum FT4 (ρ = 0.77; p = 0.009). The 13 log REPs from CYP1A1 correlated with log WHO-TEFs (r = 0.63; p = 0.015) and 11 log PCB REPs with PCB consensus toxicity factors (CTFs) for compounds with WHO-TEFs (r = 0.80; p = 0.003). The complete set of derived 56 log REPs correlated with the log CTFs (r = 0.77; p = 0.001) and log WHO-TEFs (r = 0.81; p < 0.001).ConclusionsREPs calculated from thyroid and cytochrome P450 endpoints realistically reflect human exposure scenarios because they are based on human chronic and low-dose exposures. While the CYP 1A1 seems more suitable for toxicity evaluation of PCDD/Fs, the CYP 1B1 is more apt for PCDFs and PCBs and reflects different pathways.     

The predictive power of the elimination of dioxin-like pollutants from pigs: an in vivo study

Pigs accidentally given feed contaminated by dioxin-like pollutants are a serious public health issue. We have examined whether pigs with limited exposure during early periods of fattening would be categorized as non-compliant with the EU limit at slaughtering when growth-dilution, excretion and metabolism effects are considered. Sixteen female and sixteen castrated male weaned pigs were divided into four groups (e.g. DG0, DG1, DG2 and DG3) in week 2 after birth. From weeks 3 to 13, groups DG1, DG2, and DG3 pigs were fed with a polychlorinated dibenzo-p-dioxin/dibenzofuran (PCDD/F) and polychlorinated biphenyl (PCB) mixture at dosages of 1, 10 and 100 ng-toxic equivalent (TEQ) per kg dry mass feed in capsules, respectively. From weeks 13 to 23, the animals were nourished with clear feed. Control group DG0 was always fed with clear feed. Subcutaneous fat samples were collected at weeks 13, 18 and 23 by biopsies. The pollutant residues were analyzed by high resolution gas chromatography-high resolution mass spectrometry and quantified by a ¹³C-isotope dilution method. The results showed the following: (1) when slaughtered at week 23, the TEQ for DG1 pigs (0.66 ± 0.21 pg/g fat) was under the EU limit of 1 pg PCDD/F-TEQ/g fat; (2) PCDD/F congener-specific first-order elimination rates were linearly correlated with their toxicity equivalency factors (TEFs), and the rates were significantly dose-dependent for the more toxic congeners (TEF ≥ 0.1). Therefore, the pigs' exposure above the EU limit during the early fattening stage did not necessarily lead to their categorization as non-compliant pork; and the residual TEQ for pork can be predicted from early exposure concentrations based on the models established here.     

Transfer parameter values in temperate forest ecosystems: a review

Compared to agricultural lands, forests are complex ecosystems as they can involve diverse plant species associations, several vegetative strata (overstorey, shrubs, herbaceous and other annual plant layer) and multi-layered soil profiles (forest floor, hemi-organic and mineral layers). A high degree of variability is thus generally observed in radionuclide transfers and redistribution patterns in contaminated forests. In the long term, the soil compartment represents the major reservoir of radionuclides which can give rise to long-term plant and hence food contamination. For practical reasons, the contamination of various specific forest products has commonly been quantified using the aggregated transfer factor (T_ag in m² kg⁻¹) which integrates various environmental parameters including soil and plant type, root distribution as well as nature and vertical distribution of the deposits. Long lasting availability of some radionuclides was shown to be the source of much higher transfer in forest ecosystems than in agricultural lands. This study aimed at reviewing the most relevant quantitative information on radionuclide transfers to forest biota including trees, understorey vegetation, mushrooms, berries and game animals. For both radiocaesium and radiostrontium in trees, the order of magnitude of mean T_ag values was 10⁻³ m² kg⁻¹ (dry weight). Tree foliage was usually 2–12 times more contaminated than trunk wood. Maximum contamination of tree components with radiocaesium was associated with (semi-)hydromorphic areas with thick humus layers. The transfer of radionuclides to mushrooms and berries is high, in comparison with foodstuffs grown in agricultural systems. Concerning caesium uptake by mushrooms, the transfer is characterized by a very large variability of T_ag, from 10⁻³ to 10¹ m² kg⁻¹ (dry weight). For berries, typical values are around 0.01–0.1 m² kg⁻¹ (dry weight). Transfer of radioactive caesium to game animals and reindeer and the rate of activity reduction, quantified as an ecological half-life, reflect the soil and pasture conditions at individual locations. Forests in temperate and boreal regions differ with respect to soil type and vegetation, and a faster decline of muscle activity concentrations in deer occurs in the temperate zone. However, in wild boar the caesium activity concentration shows no decline because of its special feeding habits. In the late phase, i.e. at least a few months since the external radionuclide contamination on feed plants has been removed, a T_ag value of 0.01 m² kg⁻¹ (fresh weight) is common for ¹³⁷Cs in the muscles of adult moose and terrestrial birds living in boreal forests, and 0.03 m² kg⁻¹ (fresh weight) for arctic hare. Radiocaesium concentrations in reindeer muscle in winter may exceed the summer content by a factor of more than two, the mean T_ag values for winter ranging from 0.02 to 0.8 m² kg⁻¹ (fresh weight), and in summer from 0.04 to 0.4 m² kg⁻¹. The highest values are found in the year of initial contamination, followed by a gradual reduction. In waterfowl a relatively fast decline in uptake of ¹³⁷Cs has been found, with T_ag values changing from 0.01 to 0.002 m² kg⁻¹ (fresh weight) in the three years after the contaminating event, the rate being determined by the dynamics of ¹³⁷Cs in aquatic ecosystems.     

Short-term seasonal variability in Be wet deposition in a semiarid ecosystem of central Argentina

The ⁷Be wet deposition has been intensively investigated in a semiarid region at San Luis Province, Argentina. From November 2006 to May 2008, the ⁷Be content in rainwater was determined in 58 individual rain events, randomly comprising more than 50% of all individual precipitations at the sampling period. ⁷Be activity concentration in rainwater ranged from 0.7 ± 0.3 Bq l⁻¹ to 3.2 ± 0.7 Bq l⁻¹, with a mean value of 1.7 Bq l⁻¹ (sd = 0.53 Bq l⁻¹). No relationship was found between ⁷Be content in rainwater and (a) rainfall amount, (b) precipitation intensity and (c) elapsed time between events. ⁷Be ground deposition was found to be well correlated with rainfall amount (R = 0.92). For the precipitation events considered, the ⁷Be depositional fluxes ranged from 1.1 to 120 Bq m⁻², with a mean value of 32.7 Bq m⁻² (sd = 29.9 Bq m⁻²). The annual depositional flux was estimated at 1140 ± 120 Bq m⁻² y⁻¹. Assuming the same monthly deposition pattern and that the ⁷Be content in soil decreases only through radioactive decay, the seasonal variation of ⁷Be areal activity density in soil was estimated. Results of this investigation may contribute to a valuable characterization of ⁷Be input in the explored semiarid ecosystem and its potential use as tracer of environmental processes.     

Dioxins and PCBs in game animals: Interspecies comparison and related consumer exposure

Polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), dioxin-like polychlorinated biphenyls (DL-PCB) and non-dioxin-like polychlorinated biphenyls (NDL-PCB) are ubiquitous, persistent toxic compounds that are highly bioaccumulative in nature. Wild-living animals are vulnerable to the negative impacts of human activity. Dioxins and PCBs enter the animal organisms through foraging. Due to the toxicological threat, much attention is paid to these compounds worldwide. The aim of this study was to determine the dioxin contamination status of three game animal species (red deer, roe deer, and wild boar) and compare the PCDD/F and PCB congener bioaccumulation in the muscles, abdominal fat and liver. The chemical analysis was performed by the isotope dilution technique (IDMS) with high-resolution gas chromatography coupled with high-resolution mass spectrometry (HRGC/HRMS). Dioxins and PCBs were found in specimens collected from all studied species, suggesting the presence of the test compounds in the environment of the animals. The highest concentrations were found in the livers of all animals. The toxic equivalent (TEQ) levels in the muscles, adipose tissue and liver were in the order red deer > roe deer > wild boar. PCDD/Fs were the dominant congeners in TEQ value. For all tested species, the dominant contributors to the total WHO-TEQ were PCB-126, 2,3,4,7,8-PeCDF and 1,2,3,7,8-PeCDD. Among the PCDD/F congeners in the deer tissues, OCDD, OCDF and 2,3,4,7,8-PeCDF were dominant, while in wild boar, OCDD, 1,2,3,4,6,7,8-HpCDD and 1,2,3,4,6,7,8-HpCF occurred in the highest amounts. Among PCBs, PCB-105, 118, 156, 138, 153 and 180 were dominant in all species, but with different levels. The regular consumption of muscle meat from game animals should not cause unacceptable dioxin intake above the Tolerable Weekly Intake (TWI) value for children and adults. However, liver consumption should be avoided, especially by children and pregnant or lactating women. High consumption of contaminated liver may cause dioxin intake at levels up to 300% of TWI for adults and up to 700% TWI for children.     

High background radiation investigated by gamma spectrometry of the soil in the southwestern region of Cameroon

The aim of this work is to determine the radioactivity concentration of ²²⁶Ra, ²³²Th and ⁴⁰K in sub-surface (0-5 cm) soil samples collected from Awanda, Bikoué, Ngombas in the southwestern region of Cameroon, to assess their contribution to the external dose exposure relative to the United Nation Scientific Committee on Effects of Atomic Radiation (UNSCEAR) data. An HPGe p-type detector coupled to a multichannel analyzer was used to perform measurements and data processing. The activity concentrations of ²²⁶Ra varied from 0.06 ± 0.01 to 0.27 ± 0.02 kBq kg⁻¹ with a mean value of 0.13 ± 0.01 kBq kg⁻¹ wet weight. The activity concentrations of ²³²Th varied from 0.10 ± 0.01 to 0.70 ± 0.05 kBq kg⁻¹ with a mean value of 0.39 ± 0.03 kBq kg⁻¹ wet weight, and ⁴⁰K concentrations varied from 0.37 ± 0.02 to 1.53 ± 0.11 kBq kg⁻¹ with a mean value of 0.85 ± 0.07 kBq kg⁻¹ wet weight, respectively. The mean value of outdoor annual effective doses were estimated to be 0.48 mSv y⁻¹, 0.39 mSv y⁻¹ and 0.38 mSv y⁻¹ from Ngombas, Awanda and Bikoué, respectively. The studied areas can be said to have a high background radiation level.     

On radiocarbon and plutonium leakage to groundwater in the vicinity of a shallow-land radioactive waste repository

A shallow-land radioactive waste repository operated in boggy forest environment from 1963 to 1989. During the operation period, a considerable amount of technogenic radionuclides, in solidified state, was disposed into the vault established in the geological structure at the depth of up to 3 m. Environmental monitoring activities started after the closure of the repository in 1989. Recent investigations revealed transfer of radiocarbon and plutonium to the groundwater in the prevailing flow direction. Activity concentration of ^239,240Pu in non-filtered fraction of the groundwater from observation well no. 4 determined by alpha-spectrometry was 6.4 × 10⁻⁵ Bq l⁻¹ in 2005, and 3.2 × 10⁻⁴ Bq l⁻¹ in 2006. Further analysis of colloid-facilitated transport of plutonium is planned. Variation of ¹⁴C activity concentration in the same well was monitored in 2006. It varied from 0.2 ± 0.1 Bq l⁻¹ in October to 2.8 ± 0.6 Bq l⁻¹ in June and July. Results imply further research into radiocarbon transfer to atmosphere and selected plant species.     

Factors affecting 210Po and 210Pb activity concentrations in mussels and implications for environmental bio-monitoring programmes

The activity of ²¹⁰Po and ²¹⁰Pb was determined in mussels of the same size (3.5-4.0 cm shell length) sampled monthly over a 17-month period at the Atlantic coast of Portugal. Average radionuclide concentration values in mussels were 759 ± 277 Bq kg⁻¹ for ²¹⁰Po (range 460-1470 Bq kg⁻¹ dry weight), and 45 ± 19 Bq kg⁻¹ for ²¹⁰Pb (range 23-96 Bq kg⁻¹ dry weight). Environmental parameters and mussel biometric parameters were monitored during the same period. Although there was no seasonal variation of radionuclide concentrations in sea water during the study period, the concentration of radionuclide activity in mussels varied seasonally displaying peaks of high concentrations in winter and low concentrations in summer. Analysis of radionuclide data in relation to the physiological Condition Index of mussels revealed that ²¹⁰Po and ²¹⁰Pb activities in the mussel (average activity per individual) remained nearly constant during the investigation period, while mussel body weight fluctuated due to fat storage/expenditure in the soft tissues. Similar variation of radionuclide concentrations was observed in mussels transplanted from the sea coast into the Tejo Estuary. However, under estuarine environmental conditions and with higher food availability throughout the year, transplanted mussel Condition Index was higher than in coastal mussels and average radionuclide concentrations were 210 ± 75 Bq kg⁻¹ (dry weight) for ²¹⁰Po and 10 ± 4 Bq kg⁻¹ (dry weight) for ²¹⁰Pb, therefore lower than in coastal mussels with similar shell length. It is concluded that the apparent seasonal fluctuation and inter-site difference of radionuclide concentrations were mostly caused by mussel body weight fluctuation and not by radionuclide body burden fluctuation. This interpretation can be extended to the apparent seasonal fluctuation in concentrations of lipophilic and lipophobic contaminants in mussels, and provides an explanation for occasional high concentrations of ²¹⁰Po and man-made contaminants measured in mussels far from pollution sources.     

Cesium and strontium sorption by selected tropical and subtropical soils around nuclear facilities

The dynamics of Cs and Sr sorption by soils, especially in the subtropics and tropics, as influenced by soil components are not fully understood. The rates and capacities of Cs and Sr sorption by selected subtropical and tropical soils in Taiwan were investigated to facilitate our understanding of the transformation and dynamics of Cs and Sr in soils developed under highly weathering intensity. The Langmuir isotherms and kinetic rates of Cs and Sr sorption on the Ap1 and Bt1 horizons of the Long-Tan (Lt) and the A and Bt1 horizons of the Kuan-Shan (Kt), Mao-Lin (Tml) and Chi-Lo (Cl) soils were selected for this study. Air-dried soil (<2 mm) samples were reacted with of 7.5 × 10⁻⁵ to 1.88 × 10⁻³ M of CsCl (pH 4.0) or 1.14 × 10⁻⁴ to 2.85 × 10⁻³ M of SrCl₂ (pH 4.0) solutions at 25 °C. The sorption maximum capacity (q_m) of Cs by the Ap1 and Bt1 horizons of the Lt soil (62.24 and 70.70 mmol Cs kg⁻¹ soil) were significantly (p < 0.05) higher than those by the A and Bt1 horizons of the Kt and Cl soils (26.46 and 27.49 mmol Cs kg⁻¹ soil in Kt soil and 34.83 and 29.96 mmol Cs kg⁻¹ soil in Cl soil, respectively), however, the sorption maximum capacity values of the Lt and Tml soils did not show significant differences. The amounts of pyrophosphate extractable Fe (Fe_p) were correlated significantly with the Cs and Sr sorption capacities (for Cs sorption, r² = 0.97, p < 1.0 × 10⁻⁴; for Sr sorption, r² = 0.82, p < 2.0 × 10⁻³). The partition coefficient of radiocesium sorbed on soil showed the following order: Cl soil ? Kt soil > Tml soil > Lt soil. It was due to clay minerals. The second-order kinetic model was applied to the Cs and Sr sorption data. The rate constant of Cs or Sr sorption on the four soils was substantiality increased with increasing temperature. This is attributable to the availability of more energy for bond breaking and bond formation brought about by the higher temperatures. The rate constant of Cs sorption at 308 K was 1.39-2.09 times higher than that at 278 K in the four soils. The activation energy of Cs and Sr sorbed by the four soils ranged from 7.2 to 16.7 kJ mol⁻¹ and from 15.2 to 22.4 kJ mol⁻¹, respectively. Therefore, the limiting step of the Cs⁺ or Sr²⁺ sorption on the soils was diffusion-controlled processes. The reactive components, which are significantly correlated with the Langmuir sorption maxima of Cs and Sr by these soils, substantially influenced their kinetic rates of Cs and Sr sorption. The data indicate that among components of the subtropical and tropical soils studied, short-range ordered sesquioxides especially Al- and Fe-oxides complexed with organics play important roles in influencing their capacity and dynamics of Cs and Sr sorption.     

Natural radioactivity levels in topsoil from the Pearl River Delta Zone, Guangdong, China

Concentrations of the natural radionuclides ²³⁸U, ²²⁶Ra, ²³²Th and ⁴⁰K have been measured by γ-ray spectrometry in 796 topsoil samples from the Pearl River Delta Zone (PRDZ) of Guangdong, China. The mean concentrations for ²³⁸U, ²²⁶Ra, ²³²Th and ⁴⁰K were found to be 140 ± 37 Bq kg⁻¹, 134 ± 41 Bq kg⁻¹, 187 ± 80 Bq kg⁻¹ and 680 ± 203 Bq kg⁻¹ dry mass, respectively. These values were all higher than the mean values in soil for China and the world. Outdoor air-absorbed dose rates, calculated from activity concentrations of ²²⁶Ra, ²³²Th and ⁴⁰K, ranged from 86 to 237 nGy h⁻¹, with a mean value of 165 ± 46 nGy h⁻¹. The corresponding annual outdoor effective dose rate per person was estimated to be between 0.11 and 0.29 mSv y⁻¹, with a mean value of 0.20 ± 0.06 mSv y⁻¹, which was also higher than the world mean value of 0.07 mSv y⁻¹. The radium equivalent activity (Ra_eq) and the external hazard index (I_r) resulted from the natural radionuclides in soil, were also calculated and found to vary from 230 to 676 Bq kg⁻¹ and from 0.6 to 1.8, respectively. The Ra_eq and the I_r in all the investigated regions were up to 75% higher than the set limits of 370 Bq kg⁻¹ and 1.0, respectively.     

Cs in a raised bog in central Sweden

The vertical distribution of ¹³⁷Cs activity in peat soil profiles and ¹³⁷Cs activity concentration in plants of various species was studied in samples collected at two sites on a raised bog in central Sweden. One site (open bog) was in an area with no trees and only a few sparsely growing plant species, while the other (low pine) was less than 100 m from the open bog site and had slowly growing Scots pine, a field layer dominated by some ericaceous plants and ground well-covered by plants. The plant samples were collected in 2004–2007 and were compared with samples collected in 1989 from the same open bog and low pine sites. Ground deposition of ¹³⁷Cs in 2005 was similar at both sites, 23?000 Bq m⁻². In the open bog peat profile it seems to be an upward transport of caesium since a clear peak of ¹³⁷Cs activity was found in the uppermost 1–4 cm of Sphagnum layers, whereas at the low pine site ¹³⁷Cs was mainly found in deeper (10–12 cm) layers. The migration rate was 0.57 cm yr⁻¹ at the open bog site and the migration centre of ¹³⁷Cs was at a depth of 10.7, while the rate at the low pine site was 0.78 cm yr⁻¹ and the migration centre was at 14.9 cm. Heather (Calluna vulgaris) was the plant species with the highest ¹³⁷Cs activity concentrations at both sites, 43.5 k Bq⁻¹ DM in 1989 decreasing to 20.4 in 2004–2007 on open bog and 22.3 k Bq kg⁻¹ DM in 1989 decreasing to 11.2 k Bq⁻¹ DM by the period 2004–2007 on the low pine site. ¹³⁷Cs transfer factors in plants varied between 0.88 and 1.35 on the open bog and between 0.48 and 0.69 m² kg⁻¹ DM at the low pine site.