Altered menstrual cycles in women with a high dietary intake of persistent organochlorine compounds

Dietary exposure to persistent organochlorine compounds (POCs) has been found to affect the menstrual cycle in both animals and humans. In Sweden, the major exposure route for POCs is the consumption of fatty fish from the Baltic Sea. Thus, women who eat relatively large amounts of this fish constitute a suitable study group when investigating a possible association between dietary exposure to POC and menstrual cycle disruption. Questionnaires were sent to the exposed women, as well as to a socioeconomically similar cohort of controls, and information was collected on their menstrual cycles. Since the exposed women tended to smoke more than the controls, all results were adjusted for smoking habits. A cohort comparison found that the exposed women on average had 0.46 (95% confidence interval: 0.03, 0.89) days shorter menstrual cycles than controls. However, within the exposed cohort no effects were found of the proxy variables early life exposure and high consumption of Baltic Sea fatty fish. The results give some support to previous results from studies on women with similar exposure, but are not conclusive with respect to whether there is a causal association between POC exposure and menstrual cycle disruption.     

Comparison of residue levels of persistent organochlorine compounds in butter from Spain and from other European countries

Abstract

Commercially available butter from Spain (n=36) and from other European countries (n=20) has been analyzed by high resolution gas chromatography with an electron capture detector for organochlorine contaminants. The results showed that both groups of samples have a similar pattern of these pollutants, but in all cases where significant differences in concentrations were found, Spanish samples presented higher values. This was especially notable for lindane (median values 11.6 vs. 3.0 ng/g wet weight), hexachlorobenzene (6.4 vs. 0.5) and ß‐hexachlorocyclohexane (3.1 vs. 1.2). Total PCBs showed no differences (5.4 vs. 6.6), but detailed analysis of congener composition indicated a higher presence in Spanish samples of the most persistent chlorinated PCBs. No sample presented levels of concern for any single organochlorine compound. It is interesting to note that consumption of butter in Spain is low so, although levels of organochlorines are higher than those found in other countries, consumers are less exposed through this foodstuff than in other European countries. These results also confirm the fact that environmental pollution by organochlorines is more important in Spain than in the rest of Europe.     

Comparison of residue levels of persistent organochlorine compounds in butter from Spain and from other European countries

Commercially available butter from Spain (n = 36) and from other European countries (n = 20) has been analyzed by high resolution gas chromatography with an electron capture detector for organochlorine contaminants. The results showed that both groups of samples have a similar pattern of these pollutants, but in all cases where significant differences in concentrations were found, Spanish samples presented higher values. This was especially notable for lindane (median values 11.6 vs. 3.0 ng/g wet weight), hexachlorobenzene (6.4 vs. 0.5) and beta-hexachlorocyclohexane (3.1 vs. 1.2). Total PCBs showed no differences (5.4 vs. 6.6), but detailed analysis of congener composition indicated a higher presence in Spanish samples of the most persistent chlorinated PCBs. No sample presented levels of concern for any single organochlorine compound. It is interesting to note that consumption of butter in Spain is low so, although levels of organochlorines are higher than those found in other countries, consumers are less exposed through this foodstuff than in other European countries. These results also confirm the fact that environmental pollution by organochlorines is more important in Spain than in the rest of Europe.     

Occurrence and levels of organochlorine compounds in human breast milk in Bangladesh

In low-income countries, the use of some organochlorine pesticides is still common in order to increase food production. Monitoring the chemical exposure is an important step in risk-reducing strategies. This is the first study to report concentrations of organochlorines in breast milk of women from Bangladesh where farming is the main income source.Organochlorines such as p,p′-DDT, o,p′-DDT, p,p′-DDE, p,p′-DDD (i.e., ∑DDT), HCB, α-, β- and γ-HCH, trans-chlordane, cis-chlordane, oxy-chlordane, trans-nonachlor, cis-nonachlor, mirex and polychlorinated biphenyls (CB 28, 52, 99, 101, 105, 114, 118, 123, 128, 138, 141, 149, 153, 156, 157, 163, 167, 170, 180, 183, 187, 189, 194) were analyzed in breast milk collected in 2002 from 72 first-time mothers (median age 20 years) living in the rural area Matlab, Bangladesh.While the concentrations of PCBs and many of the pesticides were low, the concentrations of p,p′-DDT and its metabolite p,p′-DDE were high (median 349 and 1645 ng g⁻¹ lipid, respectively) in comparison to other countries. The median value of ∑DDT was 2123 ng g⁻¹ lipid. The estimated daily exposure to p,p′-DDT, p,p′-DDE and ∑DDTs was 10, 30 and 42 μg kg⁻¹ body weight, respectively, in 3 months old infants. The p,p′-DDE/p,p′-DDT ratio ranged from 1 to 23, where 58% of the mothers had a ratio below 5 indicating recent or ongoing DDT exposure.This study reports infant exposure and maternal body burden of organochlorines through breast milk. Although the findings give no reason to limit breast-feeding, it is essential to identify the main exposure sources and find means to decrease the exposure.     

Environmental and lifestyle factors for organochlorine exposure among women living in Southern Spain

Southern Spain has the largest area of intensive greenhouse agriculture in Europe, and may constitute a special case of occupational and female exposure, because this type of farming requires considerable pesticide use and employs many women. We measured adipose tissue levels of 14 organochlorine pesticides in 458 women living in this area and analyzed the relationship between pesticide level/presence and sociodemographic characteristics, reproductive history or life-style factors that may influence this exposure. Pesticide presence was determined by gas chromatography with electron-capture detector. All fat samples were positive for 1 residue. DDT or metabolites were found in 98.25%, with mean value of 660 ng g⁻¹ of lipid. p,p′-DDE level was higher in women who were older, with lower educational level or obese. Almost 70% had measurable levels of endosulfan and/or metabolites, with a mean total value of 38.8 ng g⁻¹ of lipid. Endosulfan-I exposure was higher in women with shorter residence in rural settings and more frequent in women with 3 children. 52.62% were exposed to 1 of aldrin–dieldrin–endrin group. Endrin was more frequent in women who were younger, with higher educational level or no agricultural working experience; dieldrin was more frequent in women who were older, with lower educational level or more children. Finally, lindane residues were found in 39.30%. Lindane levels were higher in women who breastfed longer or had more children. Research is required on women occupationally exposed to a selected group of organochlorine pesticides, especially those of reproductive age, as a basis for preventive action.     

Serum levels of organochlorine pesticides in healthy adults from five regions of Spain

The aim of this study was to measure of serum levels of p,p′-dichlorodiphenyl trichloroethane (p,p′-DDT), p,p′-dichlorodiphenyl dichlorethylene (p,p′-DDE), β-hexachlorocyclohexane (β-HCH), and hexachlorobenzene (HCB) in healthy adults in Spain. Furthermore, we also analyzed these levels according to dietary, other lifestyle factors and anthropometric characteristics. We measured the concentrations of such organochlorine pesticides (OCPs) in serum samples collected during 1992–1996 from 953 subjects aged 35–64 years, they were residents of five Spanish regions, they were randomly selected from the European Prospective Investigation into Cancer and Nutrition (EPIC) cohort. OCPs were determined by means of gas chromatography with electron-capture detection (GC-ECD). The most frequent compound found in serum was p,p′-DDE, present in 98% of the samples, followed by HCB and β-HCH, found in 89% and 77% of samples, respectively, while p,p′-DDT could be measured only in 26% of subjects. The geometric means of serum concentrations (ng/g lipid) were 822 for p,p′-DDE, 167 for β-HCH, and 379 for HCB. The concentrations of all OCPs were positively associated with age and body mass index, and decreased along the period of blood collection. No association was found between OCPs levels and dietary factors. The concentrations of p,p′-DDE and β-HCB were higher in Murcia, one of southern regions, most likely associated with intensive past use of pesticides related to agricultural practices, while higher levels of HCB were found in Navarra, located in the north, maybe due to industrial use rather than agricultural application.     

Cumulative risk assessment of dietary exposure to phthalates in pregnant women in Beijing,China

Diet is an important exposure route for phthalates, such as di-iso-butyl phthalate (DiBP), dibutyl phthalate (DBP), bis(2-ethylhexyl) phthalate (DEHP), and benzyl butyl phthalate (BBP). In this study, we aimed to estimate phthalate exposure in the diet of pregnant women and assess the health risk. A total of 517 pregnant women in the first trimester were recruited, and food frequency questionnaires were collected. A simple distribution assessment method was used to estimate daily exposure, and the hazard index (HI) method was used to assess cumulative risk. The maximum daily dietary exposure to DEHP, DBP, DiBP, and BBP was 5.25, 3.17, 2.59, and 0.58 μg/kg bw/day, respectively, and did not exceed the safety limit values. Cereals and vegetables were the main sources of the estimated daily intake (EDI) of phthalates in the diet. The cumulative risk assessment, based on the European Food Safety Authority tolerable daily intake (TDI) and the US Environmental Protection Agency reference dose (RfD), did not exceed the threshold of 1. DiBP, DBP, and DEHP had higher hazard quotient (HQ) values for cumulative health risk than BBP. In conclusion, a low health risk was posed by the cumulative dietary exposure to phthalates for pregnant women in Beijing.

Graphical abstract

     

Age trends and reproductive transfer of organochlorine compounds in long-finned pilot whales from the Faroe Islands

Total DDT and PCB concentrations were determined in blubber of 130 long-finned pilot whales, Globicephala melas (100 females and 30 males) from the Faroe Islands (northern north-east Atlantic). In males and immature females no relation was observed between age and organochlorine concentrations or the ratio of tDDT (total DDT)/PCB; in contrast, concentrations and ratios in mature females declined with age, which is attributed to reproductive transfer to their offspring during gestation and lactation. Relative abundance of DDE respective to tDDT increased in males and young females and decreased in mature females. Organochlorine transfer to offspring during lactation was found to represent about 60-100% of the mother's body load, while that occurring during gestation was estimated to be much lower, in the range 4-10% of mother's body load. Transfer rates tended to decrease with mother's age and were, consequently, much higher in primiparous females than in those that had already given birth. Transplacental rates were found to be consistent with the ratio between mother's body weight and neonatal body weight.     

Trends of organochlorine compounds in Finnish inland waters

Caged common lake mussels (Anodonta piscinalis) have been used in the monitoring of organochlorine compounds in pulp and paper mill recipient watercourses of Finland annually from 1984 to 1998. Statistically significant decreasing trends of chlorophenols and chloroguaiacols originating from chlorobleaching were observed in all recipients in parallel with the decreasing discharges from the mills. Metabolites of chlorophenols, chloroanisoles and chloroveratroles had no or slightly increasing trends. Elevated PCB concentrations were measured in four watercourses. In two areas, PCBs were found to be significantly increasing, in two other cases they showed no trend. A mill producing recycled paper was apparently responsible for an increase of PCBs and DDE in recipient watercourses. Overall decreases were observed for other chlorohydrocarbons except for DDT. Material flows of chlorohydrocarbons were positively correlated with waterflows (Q) in some cases.     

A method to determine residue levels of persistent organochlorine pesticides in human milk from Indonesian women

A method has been developed for the analysis of organochlorine pesticides in human milk using solvent extraction, Florisil solid phase extraction clean-up and analysis by gas chromatography with an electron capture detector. The recovery of analytes from spiked milk samples was in the range 53 +/- 1% to 109 +/- 7% (n = 9). A small number of samples were obtained from women in a rural and an urban area of Indonesia and analysed using the developed method. The results are reported on a milk fat basis. All samples contained detectable residues of p,p'-DDT (urban mean 0.11 +/- 0.18 mgkg(-1) (n = 5), rural mean 0.07 +/- 0.03 mg kg(-1) (n = 5)) and p,p'-DDE (urban mean 0.05 +/- 0.04 m kg(-1) (n = 5), rural mean 0.76 +/- 1.46 mg kg(-1) (n = 5)). Residues of HCB, betaHCH, alpha-endosulfan and dieldrin were also detected in some samples. There was no significant difference (at the 95% confidence level) in levels of pesticides between urban and rural areas. The levels of organochlorine pesticides in milk from Indonesian women were lower than those reported from Indonesian women exposed to DDT through malaria eradication schemes and were similar to levels reported from UK and Japan.     

Polychlorobiphenyls and other organochlorine compounds in human follicular fluid

Based on observations in animals, there is an increasing evidence that a number of persistent organochlorine pollutants can alter the endocrine homeostasis, this resulting in toxic effects in particular in the developing organism. However, the role of these chemicals in determining endocrine-related diseases in humans, and possibly a decrease of fertility, is still controversial. Exposure data concerning the human reproductive system are essential for risk assessment. Based on this, the occurrence in follicular fluid of polychlorobiphenyls (PCBs), 2,3,7,8-chlorosubstituted polychlorinated dibenzo-p-dioxins (PCDDs) and dibenzofurans (PCDFs), 1,1,1-trichloro-2,2-bis(4-chlorophenyl)-ethane (p,p'-DDT) and its metabolites, and hexachlorobenzene (HCB) was investigated. With respect to PCBs, the sum of the three most abundant congeners (PCBs 138, 153 and 180) was 1230 ng/g, lipid basis (0.37 ng/g, wet weight). Congener distribution profile overlapped what is usually observed in other human tissues, as blood and milk. PCDDs, PCDFs, p,p'-DDT and 1,1-dichloro-2,2-bis(4-chlorophenyl)-ethane (p,p'-DDD) were below their determination limits. 1,1-dichloro-2,2-bis(4-chlorophenyl)-ethene (p,p'-DDE) and HCB were detected in concentrations respectively in the order of 700 and 70 ng/g, lipid basis (approximately 0.2 and approximately 0.02 ng/g, wet weight).     

Anthropometric, socioeconomic, and maternal health determinants of placental transfer of organochlorine compounds

The aim of this study was to relate placental transfer, quantified by the cord to maternal serum concentration ratio (C/M), of five organochlorine pesticides (OCP) hexachlorobenzene (HCB), β-hexachlorocyclohexane (β-HCH), γ-hexachlorocyclohexane (γ-HCH) , p,p'-DDT, p,p'-DDE and 15 polychlorinated biphenyl (PCB) congeners (28, 52, 101, 105, 114, 118, 123⁺¹⁴⁹, 138⁺¹⁶³, 153, 156⁺¹⁷¹, 157, 167, 170, 180, and 189) to anthropometric, socioeconomic, and maternal health characteristics. We included into the study 1,134 births during the period 2002–2004 from two districts in eastern Slovakia with high organochlorine concentrations relative to other areas of the world. Only concentrations >LOD were taken into account. Variables as age, weight and height of mothers, parity, ethnicity, alcohol consumption, illness during pregnancy, smoking during pregnancy, hypertension, respiratory diseases, rheumatoid arthritis and diabetes mellitus, and birth weight were related to C/M. Results of regression analyses showed that C/M was predicted by several factors studied. Positive associations were observed for gestational alcohol consumption, fewer illnesses during pregnancy, maternal age, and maternal weight. Caucasians had a greater C/M compared to Romani for wet weight data of congeners 170 and 180 and in contrast C/M for HCB was greater in Romani. Our results show that drinking mothers compared to abstaining expose their fetuses not only to alcohol but to an increased level of several PCB congeners. A straightforward explanation of associations between C/M shifts and factors studied is very difficult, however, with regard to the high lipophilicity of OCPs and PCBs, changes in their kinetics probably reflect lipid kinetics.     

Trends in organochlorine and mercury levels in Gannet eggs

Levels of DDE, HEOD, PCBs and mercury were measured in Gannet eggs from several colonies around Britain during 1971-1987. At two colonies (Ailsa Craig and Bass Rock) sampled throughout this period, organochlorine levels declined between the early 1970s and 1983, and then increased again. The trends at other colonies, sampled over shorter periods, were generally consistent with those at Ailsa Craig and Bass Rock. Trends in mercury levels were more variable, and increases were observed at four colonies and declines at two. Some shell-thinning occurred in association with DDE contamination. However, levels of this chemical were too low to affect breeding success in the years concerned. The same was probably true of the other chemicals.     

Polychlorobiphenyls and organochlorine pesticides in conventional and organic brands of milk: occurrence and dietary intake in the population of the Canary Islands (Spain)

The population of the Spanish archipelago of the Canary Islands has been studied in depth regarding its levels of contamination by organochlorine pesticides (OCs) and polychlorinated biphenyls (PCBs). Foodstuffs of animal origin, such as milk, are prominent contributors to the body burden of these contaminants. As this population presents one of the highest milk-intake in Spain and Europe, we evaluated the level of OCs and PCBs in 26 commercially available brands of milk (16 conventional and 10 organic brands) present in the market of these Islands, in order to estimate the relevance of milk as a source of these chemicals for the Canary population. Our findings showed that hexachlorobenzene, trans-chlordane, and PCB153 were present in almost all the samples with independence of the type of milk. For both types of milks, the concentration of OCs was very low, showing organic milks lower levels than conventional ones. As a consequence, the estimated daily intake for OCs was lower than the tolerable daily intake (TDI) established by International Agencies. The levels of PCBs in milk were also found to be very low, but, in this case, the situation was the opposite: there were higher levels of PCBs in organic than in conventional brands of milk. Unexpectedly, levels of dioxin-like PCBs (DL-PCBs) reached values higher than 25 pg WHO-TEQ g⁻¹ fat in percentile 75 for both types of milk indicating the existence of a number of brands of milk highly contaminated by these toxicants. Consequently, the population who consume the most contaminated milk brands could have estimated daily intakes well above the recommended TDI (2 pg WHO-TEQ kg⁻¹ b.w. d⁻¹) established by European Union Authorities. These results are of concern if we consider the well known adverse health effects exerted by dioxin-like compounds.     

Levels of organochlorine compounds in spotted dolphins from the Coiba archipelago, Panama

Blubber and skin samples from 63 spotted dolphins (Stenella attenuata) (18 males, 40 females and 5 of unknown sex) were collected by biopsy techniques in the waters of the Coiba archipelago. Blubber was analyzed for organochlorine compounds and skin for gender determination. Mean levels of HCB (hexachlorobenzene), tPCB (polychlorinated biphenyls) and tDDT (dichlorodiphenyltrichloroethane) were 0.064, 2.30 and 6.4 mgkg(-1), respectively. These levels are low and are not considered to represent a threat to the S. attenuata population. No significant differences either in concentrations of HCB, tPCB and tDDT or in PCB profiles were observed between males and females. The ratio tDDT/tPCB was 2.69, indicating predominantly agrarian versus industrial activities in the area. The ratio ppDDE/tDDT was 0.83, a high figure that suggests both a local reduction of DDT inputs and a high rate of DDT degradation. Significant quantitative and qualitative differences were observed between two schools, suggesting intra-population heterogeneity in organochlorine exposure possibly due to demographic segregation.     

Formation of organochlorine compounds in kraft pulp bleaching processes

The most abundant volatile organochlorine compounds (VOCCs), trichloroacetic and dichloroacetic acids and AOX, were determined in bleaching effluent and waste water from three kraft pulp mills during ClO₂ bleaching. 0.6–7.7 g of VOCCs per ton bleached pulp were formed, the most abundant being chloroform and dichloroacetic acid methyl ester. Most of the VOCCs were removed during treatment, and it was estimated that 2–30 t of VOCCs would be removed annually from activated sludge treatment plants in Finnish kraft pulp mills using elemental chlorine free bleaching, most likely by volatilization. Dichloroacetic acid was formed in considerably higher amounts than trichloroacetic acid, and both compounds were removed effectively during treatment. The formation of all organochlorine compounds decreased considerably when non-chlorinated bleaching was employed.     

EOX and organochlorine compounds in fish and ringed seal samples from Lake Ladoga, Russia

Information about the pollution of Lake Ladoga, the largest lake in Europe, has been controversial. Various effluents and drainage waters affect the quality of the lake water. Wastewaters have caused eutrophication of parts of Lake Ladoga, but concentrations of persistent organic pollutants in the lake's food webs are poorly understood. In this study, concentrations of some organochlorine compounds, chlorophenols (CPs), and extractable organic halogen (EOX) were determined in smelt (Osmerus eperlanus), vendace (Coregonus albula), pikeperch (Lucioperca lucioperca), whitefish (Coregonus lavaretus), and the Ladoga seal (Phoca hispida ladogensis) from the northern part of the lake. The concentrations of organochlorine compounds in fish were low. Concentrations were between 0.07 and 0.15, 0.65 and 1.0, and 0.29 and 0.48 mg/kg lipids for hexachlorobenzene, total polychlorinated biphenyl (PCB) and p,p'-DDE, respectively. The results indicated biomagnification from smelt and vendace to pikeperch and ringed seal. In ringed seals, concentrations of PCB and DDT were 12 and 29 times higher than in fish used by ringed seals as major food sources.     

Occurrence of organochlorine insecticides, PCBs and PCB congeners in waters and sediments of the Ebro River (Spain)

Complex mixtures extracted from air filters exposed for 24 h in two sessions (27 July and 02 August 1991) and at two locations (Merced, downtown, and Pedregal de San Angel, south-west) in Mexico City were analysed. The organic extracts were from airborne particles equal or smaller than 10 microns (PM10), and from total suspended particles (TSP). These organic extracts were assayed in the somatic mutation and recombination test (SMART) in wings of Drosophila melanogaster using two different crosses as well as in the Salmonella/microsome assay using strain TA98 with and without S9 fraction. The presence of polycyclic aromatic hydrocarbons (PAH) in the extracts was determined by gas chromatography. The genotoxic activities observed in the two test systems were comparable with the indirect mutagens producing greater response than the direct mutagens. The quantities of particulate matter as well as the genotoxic activities were higher on 02 August than on 27 July 1991 for both locations. The amounts of airborne particles and the resulting genotoxic activities were higher at Merced than at Pedregal. In both biological systems, PM10 were more genotoxic than TSP. These results demonstrate the sensitivity of the Drosophila wing SMART-which is an in vivo eukaryotic genotoxicity assay-as a biological monitor of environmental pollution related to airborne particles.     

Inside-sediment partitioning of PAH, PCB and organochlorine compounds and inferences on sampling and normalization methods

Comparability of sediment analyses for semivolatile organic substances is still low. Neither screening of the sediments nor organic-carbon based normalization is sufficient to obtain comparable results. We are showing the interdependency of grain-size effects with inside-sediment organic-matter distribution for PAH, PCB and organochlorine compounds. Surface sediment samples collected by Van-Veen grab were sieved and analyzed for 16 PAH, 6 PCB and 18 organochlorine pesticides (OCP) as well as organic-matter content. Since bulk concentrations are influenced by grain-size effects themselves, we used a novel normalization method based on the sum of concentrations in the separate grain-size fractions of the sediments. By calculating relative normalized concentrations, it was possible to clearly show underlying mechanisms throughout a heterogeneous set of samples. Furthermore, we were able to show that, for comparability, screening at <125 μm is best suited and can be further improved by additional organic-carbon normalization.     

Polychlorinated dibenzo-p-dioxins and related compounds: the blood levels of young Japanese women.

We investigated PCDDs and related compounds in the blood of young Japanese women, approximately 20 years of age, who had not yet had children, and discussed how the TEQ level of PCDDs and related compounds in their blood may affect the next generation. Means of total TEQ levels were 0.063 pg/g for whole blood basis and 21 pg/g for lipid basis. TEQ of PCDDs, PCDFs and coplanar PCBs accounted for about 43, 34 and 23% of the total TEQ in the whole blood basis, respectively. In the lipid basis, their values were about 44, 34 and 22%, respectively. Previously, we investigated PCDDs and related compounds levels in mother's breast milk, lymphocyte subpopulation and thyroid function of their children, and found negative correlations between the TEQ level of PCDDs and related compounds and CD4+/CD8+, and/or the TEQ level of PCDDs and related compounds and the T₄ level in 36 mothers and children. Of these cases, the average age was approximately 28 years. PCDDs and related compounds may be related to immunopathy, such as atopic dermatitis. The effects of PCDDs and related compounds on babies of young Japanese women are important and must be further evaluated.