Publications by authors named "Päivi Ruokojärvi"

20 Publications

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Persistent organic pollutants and the size of ovarian reserve in reproductive-aged women.

Environ Int 2021 May 1;155:106589. Epub 2021 May 1.

Division of Obstetrics and Gynecology, Department of Clinical Science, Intervention and Technology, Karolinska Institutet and Karolinska University Hospital Huddinge, 141 86 Stockholm, Sweden. Electronic address:

Industrial chemicals such as persistent organic pollutants (POPs) have been associated with reduced fertility in women, including longer time-to-pregnancy (TTP), higher odds for infertility, and earlier reproductive senescence. Fertility is highly dependent on the ovarian reserve, which is composed of a prenatally determined stock of non-growing follicles. The quantity and quality of the follicles decline with age, thereby eventually leading to menopause. In the clinical setting, assessing ovarian reserve directly through the histological analysis of follicular density in ovaries is not practical. Therefore, surrogate markers of ovarian reserve, such as serum anti-Müllerian hormone (AMH) are typically used. Here, we studied associations between chemical exposure and ovarian reserve in a cohort of pregnant women undergoing elective caesarean section (n = 145) in Stockholm, Sweden. Full data (histological, clinical, serum) were available for 50 women. We estimated the size of the reserve both directly by determining the density of follicles in ovarian cortical tissue samples, and indirectly by measuring AMH in associated serum samples. Concentrations of 9 organochlorine pesticides (OCPs), 10 polychlorinated biphenyls (PCBs), 3 polybrominated diphenylethers (PBDEs) and 9 perfluoroalkyl substances (PFAS) were determined in serum, and clinical data were retrieved from electronic medical records. Healthy follicle densities (median 0, range 0-193 follicles/mm) and AMH levels (median 2.33 ng/mL, range 0.1-14.8 ng/mL) varied substantially. AMH correlated with the density of growing follicles. Twenty-three chemicals detected in more than half of the samples were included in the analyses. None of the chemicals, alone or as a mixture, correlated with AMH, growing or atretic follicles. However, HCB, transnonachlor, PCBs 74 and 99 were associated with decreased non-growing follicle densities. HCB and transnonachlor were also negatively associated with healthy follicle density. Further, mixture of lipophilic POPs (PBDE 99, p,p'-DDE, and PCB 187) was associated with lower non-growing follicle densities. In addition, exposure to HCB, p,p'-DDE, and mixture of OCPs were significantly associated with higher odds of infertility. The results suggest that exposure to chemicals may reduce the size of ovarian reserve in humans, and strongly encourage to study mechanisms behind POP-associated infertility in women in more detail.
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http://dx.doi.org/10.1016/j.envint.2021.106589DOI Listing
May 2021

Persistent organic pollutants, pre-pregnancy use of combined oral contraceptives, age, and time-to-pregnancy in the SELMA cohort.

Environ Health 2020 06 15;19(1):67. Epub 2020 Jun 15.

Department of Environmental Medicine and Public Health, Icahn School of Medicine at Mount Sinai, New York, USA.

Background: We are exposed to several chemicals such as persistent organic pollutants (POPs) in our everyday lives. Prior evidence has suggested that POPs may have adverse effects on reproductive function by disrupting hormone synthesis and metabolism. While there is age-related decline of fertility, the use of hormonal combined oral contraceptives (COCs) and its association to return of fertility remains controversial. The goal of this study is to investigate the association between exposure to POPs, both individually and as a mixture, and fecundability measured as time-to-pregnancy (TTP) according to pre-pregnancy use of COCs and age.

Methods: Using the SELMA (Swedish Environmental Longitudinal Mother and Child, Allergy and Asthma) study, we have identified 818 pregnant women aged 18-43 years (mean 29 years) with data on how long they tried to get pregnant and what was their most recently used contraceptive method. These data were collected at enrollment to the study (median week 10 of pregnancy). Concentrations of 22 POPs and cotinine were analyzed in the blood samples collected at the same time as the questions on TTP and pre-pregnancy use of contraceptive. Analyses were done on the association between POPs exposure and TTP measured as continuous (months) and binary (infertile for those with TTP > 12 months). To study the chemicals individually, Cox regression and logistic regression were used to estimate fecundability ratios (FRs) and odds ratios (ORs), respectively. Weighted quantile sum (WQS) regression was used to investigate the chemicals as a mixture where chemicals of concern were identified above the 7.6% threshold of equal weights. To perform the subgroup analysis, we stratified the sample according to use of COCs as the most recent pre-pregnancy contraception method and age (< 29 years, and ≥ 29 years). The models were adjusted for parity, regularity of menses, maternal body mass index (BMI) and smoking status, and stratified as described above.

Results: Prior to stratification, none of the POPs were associated with fecundability while increased exposure to HCB, PCB 74 and 118 had higher odds of infertility. Upon stratification, POP exposure was significantly associated with longer TTP in women aged ≥29 years who did not use COC. Specifically, PCBs 156, 180, 183, and 187 were associated with reduced fecundability while PCBs 99, 153, 156, 180, 183, and 187 had higher odds of infertility. As a mixture, we identified the chemicals of concern for a longer TTP include PCBs 118, 156, 183, and 187. Moreover, chemicals of concern identified with increased odds of infertility were PCB 74, 156, 183, 187, and transnonachlor.

Conclusion: Serum concentrations of selected POPs, both as individual chemicals and as a mixture, were significantly associated with lower fecundability and increased odds of infertility in women aged 29 years and above not using COC as their most recent pre-pregnancy contraceptive. Our findings suggest that pre-pregnancy use of oral contraceptive and age may modify the link between POPs and fecundability. The differences of specific chemicals in the individual analysis and as a mixture support the need to study combination effects of chemicals when evaluating reproductive outcomes.
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http://dx.doi.org/10.1186/s12940-020-00608-8DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7294652PMC
June 2020

Pre-diagnostic blood immune markers, incidence and progression of B-cell lymphoma and multiple myeloma: Univariate and functionally informed multivariate analyses.

Int J Cancer 2018 09 26;143(6):1335-1347. Epub 2018 Apr 26.

Department of Radiation Sciences, Oncology, Umeå University, Umeå, Sweden.

Recent prospective studies have shown that dysregulation of the immune system may precede the development of B-cell lymphomas (BCL) in immunocompetent individuals. However, to date, the studies were restricted to a few immune markers, which were considered separately. Using a nested case-control study within two European prospective cohorts, we measured plasma levels of 28 immune markers in samples collected a median of 6 years before diagnosis (range 2.01-15.97) in 268 incident cases of BCL (including multiple myeloma [MM]) and matched controls. Linear mixed models and partial least square analyses were used to analyze the association between levels of immune marker and the incidence of BCL and its main histological subtypes and to investigate potential biomarkers predictive of the time to diagnosis. Linear mixed model analyses identified associations linking lower levels of fibroblast growth factor-2 (FGF-2 p = 7.2 × 10 ) and transforming growth factor alpha (TGF-α, p = 6.5 × 10 ) and BCL incidence. Analyses stratified by histological subtypes identified inverse associations for MM subtype including FGF-2 (p = 7.8 × 10 ), TGF-α (p = 4.08 × 10 ), fractalkine (p = 1.12 × 10 ), monocyte chemotactic protein-3 (p = 1.36 × 10 ), macrophage inflammatory protein 1-alpha (p = 4.6 × 10 ) and vascular endothelial growth factor (p = 4.23 × 10 ). Our results also provided marginal support for already reported associations between chemokines and diffuse large BCL (DLBCL) and cytokines and chronic lymphocytic leukemia (CLL). Case-only analyses showed that Granulocyte-macrophage colony stimulating factor levels were consistently higher closer to diagnosis, which provides further evidence of its role in tumor progression. In conclusion, our study suggests a role of growth-factors in the incidence of MM and of chemokine and cytokine regulation in DLBCL and CLL.
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http://dx.doi.org/10.1002/ijc.31536DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6100111PMC
September 2018

Human exposure to PCDDs and their precursors from heron and tern eggs in the Yangtze River Delta indicate PCP origin.

Environ Pollut 2017 Jun 31;225:184-192. Epub 2017 Mar 31.

State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China; Department of Environmental Science and Analytical Chemistry, Stockholm University, SE-10691 Stockholm, Sweden; Swetox, Karolinska Institute, Unit of Toxicology Sciences, Forskargatan 20, SE-15136 Södertälje, Sweden.

Polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) are highly toxic to humans and wildlife. In the present study, PCDD/Fs were analyzed in the eggs of whiskered terns (Chlidonias hybrida), and genetically identified eggs from black-crowned night herons (Nycticorax nycticorax) sampled from two lakes in the Yangtze River Delta area, China. The median toxic equivalent (TEQ) of PCDD/Fs were 280 (range: 95-1500) and 400 (range: 220-1100) pg TEQ g lw (WHO, 1998 for birds) in the eggs of black-crowned night heron and whiskered tern, respectively. Compared to known sources, concentrations of PCDDs relative to the sum of PCDD/Fs in bird eggs, demonstrated high abundance of octachlorodibenzo-p-dioxin (OCDD), 1,2,3,4,6,7,8-heptaCDD and 1,2,3,6,7,8-hexaCDD indicating pentachlorophenol (PCP), and/or sodium pentachlorophenolate (Na-PCP) as significant sources of the PCDD/Fs. The presence of polychlorinated diphenyl ethers (PCDEs), hydroxylated and methoxylated polychlorinated diphenyl ethers (OH- and MeO-PCDEs, known impurities in PCP products), corroborates this hypothesis. Further, significant correlations were found between the predominant congener CDE-206, 3'-OH-CDE-207, 2'-MeO-CDE-206 and OCDD, indicating a common origin. Eggs from the two lakes are sometimes used for human consumption. The WHO health-based tolerable intake of PCDD/Fs is exceeded if eggs from the two lakes are consumed regularly on a weekly basis, particularly for children. The TEQs extensively exceed maximum levels for PCDD/Fs in hen eggs and egg products according to EU legislation (2.5 pg TEQ glw). The results suggest immediate action should be taken to manage the contamination, and further studies evaluating the impacts of egg consumption from wild birds in China. Likewise, studies on dioxins and other POPs in common eggs need to be initiated around China.
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http://dx.doi.org/10.1016/j.envpol.2017.03.052DOI Listing
June 2017

Temporal trends in the levels of polychlorinated dioxins, -furans, -biphenyls and polybrominated diethyl ethers in bank voles in Northern Finland.

Sci Total Environ 2015 Sep 25;526:70-6. Epub 2015 Apr 25.

The Centre for Arctic Medicine, Thule Institute, PO BOX 7300, FI-90014, University of Oulu, Finland. Electronic address:

Dioxin-like chemicals and brominated flame retardants are ubiquitous in the environment, despite the introduction of international prohibitions and restrictions. These chemicals do not remain in the vicinity of their source, instead they can be transported over long distances, in fact even to pristine areas in the northern latitudes. However, there have been rather few time series experiments monitoring the trends in the levels of chlorinated and brominated forms of these chemicals in the environment. In this study, the concentrations of polychlorinated dibenzo-p-dioxins and -furans (PCDDs/Fs), polychlorinated biphenyls (PCBs) and polybrominated diethyl ethers (PBDEs) were measured in the liver and muscle of bank voles (Myodes glareolus) caught in a remote area in Finnish Lapland during 1986-2007. Five time points were selected: years 1986, 1992, 1998, 2003 and 2007. The levels of PCDDs/Fs and PCBs declined from 1986 until 2003 in both females and males, but tended to increase again in 2007. The peak levels of the most abundant PBDE congeners (PBDEs 47, 99, 100 and 153) were measured in 1998 and 2003. These results reveal that the levels of dioxin-like chemicals remain high also in rural areas in Lapland, whereas the concentrations of brominated flame retardants decreased and follow the current restriction prohibitions.
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http://dx.doi.org/10.1016/j.scitotenv.2015.04.067DOI Listing
September 2015

Levels and congener profiles of PBDEs in edible Baltic, freshwater, and farmed fish in Finland.

Environ Sci Technol 2015 Mar 4;49(6):3851-9. Epub 2015 Mar 4.

†Department of Environmental Health, National Institute for Health and Welfare, P.O. Box 95, FI-70701 Kuopio, Finland.

Fish is the major source of polybrominated diphenyl ethers (PBDEs) for Finnish consumers. To estimate the PBDE contamination in fish that Finns regularly consume as food, a large-scale sampling was undertaken in 2009-2010. Altogether 207 samples of 17 edible fish species were collected from commercially and recreationally important fishing areas in the Baltic Sea, freshwater lakes, and farming facilities. The analysis of 15 PBDE congeners was performed in an accredited testing laboratory with high-resolution gas chromatography mass spectrometry. In all of the samples, the Σ15PBDE varied between 0.029 and 73 ng/g fw. The most abundant congeners were BDE-47 (average proportion 42%), -99 (8.4%), -100 (11%), -154 (5.6%), and -209 (27%). High levels of BDE-209 were observed in the Baltic Sea, off the coast of Pori, in Baltic herring, perch, pike, and pike-perch. Overall, the PBDE levels in Baltic and freshwater fish were low. The levels in farmed whitefish were slightly higher than in wild whitefish. The reasons for the high BDE-209 levels in Baltic herring in Pori and the elevated levels of PBDEs in farmed whitefish should be investigated more thoroughly.
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http://dx.doi.org/10.1021/es505266pDOI Listing
March 2015

PCDD/Fs, PCBs and PBDEs in zooplankton in the Baltic Sea - spatial and temporal shifts in the congener-specific concentrations.

Chemosphere 2014 Nov 14;114:172-80. Epub 2014 May 14.

Finnish Environment Institute (SYKE), P.O. Box 140, Helsinki, Finland. Electronic address:

In the marine food-webs, zooplankton is a key element in the transfer of persistent organic pollutants to higher trophic levels. We determined the congener-specific concentrations of polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), polychlorinated biphenyls (PCBs) and polybrominated diphenyl ethers (PBDEs) in offshore zooplankton (size from 0.2 to 20mm) collected in 2001, 2002 and 2010 in the northern and central Baltic Sea. Of the PCDD/Fs, the concentrations of 2378-TCDF were from 18 to 47 and of 23478-PeCDF from 7.9 to 29 pg g(-1)fat and showed little temporal differences. However, 1234678-HpCDF and OCDF were abundant in 2001-2002 especially in the eastern Gulf of Finland (average concentrations 50 and 89 pg g(-1)fat, respectively). In 2010 the concentrations of these two congeners were lower, 29 and 30 pg g(-1)fat, respectively, but still substantially higher than in the other surveyed areas. The principal components analysis (PCA) supported that area-specific patterns in pollution strongly contributed to the congener profiles particularly in surface sediment and in sediment trap material, but even in zooplankton. The concentrations of the PCBs were highest in the Gulf of Finland and in the Bothnian Bay. The concentrations of most PCBs were somewhat lower in 2010 than in 2001-2002. Of the dioxin-like PCBs, the concentrations of PCB-77 were highest (271-572 pg g(-1)fat) but PCB-126 (32-113 pg g(-1)fat) contributed from 85% to 91% of the total toxicity of PCBs due to its higher toxic potency. Of the PBDEs, the BDE47 and BDE99 were the most abundant (concentrations from 1.2 to 4.6 and from 0.4 to 3.3 ng g(-1) fat, respectively). The concentrations of most PBDEs were lower in 2010 than in 2001/2002 except in the eastern Gulf of Finland.
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http://dx.doi.org/10.1016/j.chemosphere.2014.04.026DOI Listing
November 2014

Sedimentation of PCDD/Fs and PCBs in the Gulf of Finland and the Gulf of Bothnia, the Baltic Sea.

Chemosphere 2013 Nov 21;93(8):1541-7. Epub 2013 Sep 21.

Finnish Environment Institute (SYKE), P.O. Box 140, Helsinki, Finland. Electronic address:

Sediment trap material was collected during May-December in the period 1996-2008 in three coastal areas and four open sea stations in the Finnish territory of the Baltic Sea. The highest sedimentation of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) with a typical source-related congener profile from chlorophenol production dominated by highly chlorinated dibenzofurans was found close to a historical source in the Kymijoki estuary. This was an order of magnitude higher than in other river estuaries and two orders of magnitude higher than in the open sea stations. The sedimentation of polychlorinated biphenyls (PCBs) was also higher in river estuaries than in other areas. No significant decrease over a 12 year period of monitoring was found in concentration or in sedimentation in the Kymijoki estuary. In the western Gulf of Finland, the Archipelago Sea and the Gulf of Bothnia, the dominating congeners, calculated as toxic equivalent (TEQ) in sedimentation were 1, 2, 3, 7, 8-PeCDD and 2, 3, 4, 7, 8-PeCDF, often reported as the main congeners in deposition.
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http://dx.doi.org/10.1016/j.chemosphere.2013.07.072DOI Listing
November 2013

Levels of PCDD/Fs, PCBs and PBDEs in breast milk of women living in the vicinity of a hazardous waste incinerator: assessment of the temporal trend.

Chemosphere 2013 Nov 23;93(8):1533-40. Epub 2013 Aug 23.

Laboratory of Toxicology and Environmental Health, School of Medicine, IISPV, Universitat Rovira i Virgili, Sant Llorenç 21, 43201 Reus, Catalonia, Spain; Environmental Engineering Laboratory, Departament d'Enginyeria Quimica, Universitat Rovira i Virgili, Av. Països Catalans 26, 43007 Tarragona, Catalonia, Spain.

The concentrations of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), polychlorinated biphenyls (PCBs) and polybrominated diphenyl ethers (PBDEs) were determined in breast milk from women living in the vicinity of a hazardous waste incinerator (HWI) in Catalonia, Spain. The results were compared with the levels obtained in previous surveys carried out in the same area in 1998 (baseline study), 2002 and 2007. The current total concentrations of 2,3,7,8-chlorinated PCDD/Fs in breast milk ranged from 18 to 126 pg g(-1)fat (1.1-12. 3 pg WHO2005-TEQPCDD/F), while the total levels of PCBs ranged from 27 to 405 pg g(-1)fat(0.7-5.3 pg WHO2005-TEQPCB). In turn, PBDE concentrations (sum of 15 congeners) ranged 0.3-5.1 g g(-1)fat, with a mean value of 1.3 ng g(-1)fat. A general decrease in the concentrations for PCDD/Fs, both planar and total PCBs, and PBDEs in breast milk was observed. The levels of PCDD/Fs, PCBs, and PBDEs in milk of women living in urban zones were higher than those corresponding to industrial zones (41%, 26%, and 8%, respectively). For PCDD/Fs and PCBs, the current decreases are in accordance with the reduction in the dietary intake of these pollutants that we have also observed in recent studies carried out in the same area of study.
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http://dx.doi.org/10.1016/j.chemosphere.2013.07.071DOI Listing
November 2013

Polychlorinated dibenzo-p-dioxins (PCDDs), dibenzofurans (PCDFs), polychlorinated biphenyls (PCBs), and polybrominated diphenyl ethers (PBDEs) in Finnish semi-domesticated reindeer (Rangifer tarandus tarandus L.).

Environ Int 2011 Feb 30;37(2):335-41. Epub 2010 Oct 30.

University of Oulu, Department of Biology, P.O. Box 3000, 90014 Oulu, Finland.

To explore the concentrations and dynamics of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), polychlorinated biphenyls (PCBs) and polybrominated diphenyl ethers (PBDEs) in Finnish semi-domesticated reindeer (Rangifer tarandus tarandus L.) the reindeer milk and tissue samples were collected from the sub-arctic northern Finland. Reindeer milk's PCB sum (1.20 ng g(-1) wet weight) and PCDD/F sum (0.70 pg g(-1) ww) in autumn were higher than in summer (PCBs 0.50 ng g(-1) ww and PCDD/Fs 0.20 pg g(-1) ww). The mean fat content in autumn milk (26%) was significantly higher than in summer (10%). Concentrations in reindeer milk were generally far below 50% of that in adult reindeer body burden. However, the bioaccumulation factors were multiple in milk/reindeer calf ratio and that aroused the question of other important exposure routes than lactation. The muscle and liver of reindeer calves had higher PCDD/F and PCB concentrations than adult animals that possibly indicate the significance of transfer of these compounds from dam to calf through lactation and placenta. However, PBDE concentrations were higher in adult reindeer, especially in liver. In addition, reindeer liver seems to have a special feature to collect highly toxic PCDD/Fs, although the PCB sum concentrations (range from 0.33 to 1.69 ng g(-1) wet weight) were clearly higher than the sums of PCDD/Fs (range from 3.78 to 39.2 pg g(-1) ww). Stillborn reindeer calves represented individuals who had got their PCDD/F, PCB and PBDE load only via the placenta. Concentrations in muscle and brown adipose tissue samples did not indicate dependency on fat content. Obviously effective placental transfer of PCBs and PBDEs from reindeer dam to foetus was seen in this study.
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http://dx.doi.org/10.1016/j.envint.2010.10.003DOI Listing
February 2011

Persistent organic pollutants in two Finnish watercourses: levels, congener profiles and source estimation by mussel incubation.

Chemosphere 2010 Jul 1;80(6):625-33. Epub 2010 Jun 1.

National Institute for Health and Welfare, Department of Environmental Health, P.O. Box 95, FI-70701 Kuopio, Finland.

Mussel incubation was used to compare two Finnish watercourses, which have been contaminated by effluents from pulp mills and are known to be polluted with polychlorinated biphenyls (PCBs). Lake mussels (Anodonta Piscinalis) incubated in 1998 and 2004 in the rivers Kymijoki and Vuoksi were analysed for PCBs and polychlorinated dibenzo-p-dioxins (PCDDs), dibenzofurans (PCDFs), naphthalenes (PCNs), diphenyl ethers (PCDEs), hydroxy diphenyl ethers (HO-PCDEs), methoxy diphenyl ethers (MeO-PCDEs), and polybrominated diphenyl ethers (PBDEs). The contamination of the River Kymijoki, which descends to the Baltic Sea, proved significantly greater than that of the River Vuoksi, with no decreasing apparent trend, except for the PBDEs. The River Vuoksi represented more a background area compared to the River Kymijoki, excluding the PCBs. The concentration of the PCDD/PCDFs in the Kymijoki mussels exceeded the EU's maximum permissible level for PCDD/PCDFs in foodstuffs (4 pg g(-1) fresh weight). Analyses of perfluorooctanesulphonate and perfluorooctanoate in the mussels incubated in 2005 and 2006 in the River Kymijoki revealed no significant contamination of the river with these compounds. Comparison of the data of the mussels with that of sediments and commercial formulations showed that the past manufacture of a chlorophenol-based wood preservative has remained a significant source of the PCDD/PCDFs, HO-PCDEs and PCDEs in the River Kymijoki. PCB formulations are believed to represent the major sources of the PCBs and PCNs in both watercourses, though situation in the River Kymijoki had been influenced by a chlor-alkali plant. Municipal wastewaters are believed to represent the major source of the PBDEs.
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http://dx.doi.org/10.1016/j.chemosphere.2010.04.058DOI Listing
July 2010

Polychlorinated dibenzo-p-dioxins, dibenzofurans, and polychlorinated biphenyls in semi-domesticated reindeer (Rangifer tarandus tarandus) and wild moose (Alces alces) meat in Finland.

Chemosphere 2009 May 12;75(5):617-622. Epub 2009 Feb 12.

Finnish Food Safety Authority Evira, Fish and Wildlife Health Research Unit, P.O. Box 517, FI-90101 Oulu, Finland.

Semi-domesticated reindeer and wild moose meat samples were analyzed for polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), and polychlorinated biphenyls (PCBs). Both calves and adults were studied. Individual reindeer and moose meat samples and pooled reindeer calf meat samples were collected from the northern, the middle, and the southern reindeer herding regions in Finland. Samples represented the edible parts of carcasses. In individual samples of reindeer the fat based WHO-PCDD/F-PCB-TEQ concentration was on average 3.2pgg(-1) in calves and 2.3pgg(-1) in adults. In moose calves the fat based WHO-PCDD/F-PCB-TEQ concentration (1.9pgg(-1)) was lower than in reindeer calves. WHO-PCDD/F-PCB-TEQ concentration in the adult moose samples was equal as in the adult reindeer samples. The mean fat based WHO-PCDD/F-PCB-TEQ concentration was highest in reindeer calf samples from the middle region. These samples contained also the highest content of fat. Individual samples of reindeer contained on average more WHO-PCB-TEQ than WHO-PCDD/F-TEQ, while the opposite was true for moose samples, and also samples of adult reindeer from the southern area. The contributions of PCDD/Fs and PCBs to the total TEQ were similar in the reindeer calves' pooled samples which were collected from more western regions than individual samples.
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http://dx.doi.org/10.1016/j.chemosphere.2009.01.013DOI Listing
May 2009

Concentrations of PCDD/Fs, PCBs and PBDEs in breast milk of women from Catalonia, Spain: a follow-up study.

Environ Int 2009 Apr 21;35(3):607-13. Epub 2009 Jan 21.

Laboratory of Toxicology and Environmental Health, School of Medicine, Rovira i Virgili University, San Lorenzo 21, E-43201 Reus, Catalonia, Spain.

The concentrations of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), polychlorinated biphenyls (PCBs), and polybrominated diphenyl ethers (PBDEs) were determined in breast milk from women living in the vicinity of a new hazardous waste incinerator (HWI) in Catalonia, Spain. The results were compared with the levels obtained in two previous surveys carried out in 1998 (baseline study) and 2002. The current concentrations of PCDD/Fs in breast milk ranged from 45 to 143 pg/g fat (2.8 to 11.2 pg WHO-TEQ/g fat), while total PCBs ranged from 114 to 617 pg/g fat (2.8 to 17.6 pg WHO-TEQ/g fat). PBDE concentrations (sum 15 congeners) ranged from 0.57 ng/g fat to 5.9 ng/g fat, with a mean value of 2.5 ng/g fat. A general decrease of the concentrations for PCDD/Fs and both planar and total PCBs was observed. Regarding to PBDE concentrations in breast milk, similar levels between the 2002 and the present study were noted. The levels of PCDD/Fs and PCBs in milk of women living in urban areas were higher than those corresponding to the industrial zones (38% and 40%, respectively). However, the current PBDE levels were slightly lower (13%) in the urban than in the industrial zone. For PCDD/Fs and PCBs, the current decreases are in accordance with the reduction in the dietary intake of these pollutants found in recent studies carried out in the same area of study.
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http://dx.doi.org/10.1016/j.envint.2008.12.003DOI Listing
April 2009

A decision framework for possible remediation of contaminated sediments in the River Kymijoki, Finland.

Environ Sci Pollut Res Int 2009 Jan 21;16(1):95-105. Epub 2008 Oct 21.

Finnish Environment Institute (SYKE), P.O. Box 140, 00251, Helsinki, Finland.

Background, Aim, And Scope: The paper describes the spatial contamination of the River Kymijoki, South-Eastern Finland, and the coastal region of the Gulf of Finland with PCDD/Fs and mercury. The findings of ecotoxicologial and human health studies are also reported, including environmental and human risk assessments. Sediments from the River Kymijoki, draining into the Gulf of Finland, have been heavily polluted by the pulp and paper industry and by chemical industries. A wood preservative, known as Ky-5, was manufactured in the upper reaches of the river between 1940 and 1984 causing severe pollution of river sediments with polychlorinated dibenzo-p-dioxins (PCDD) and dibenzofurans (PCDF). Moreover, the sediments have been polluted with mercury (Hg) from chlor-alkali production and the use of Hg as a slimicide in pulp and paper manufacturing.

Materials And Methods: An extensive sediment survey was conducted as well as sediment transport modeling, toxicity screening of sediment invertebrates, and a survey of contaminant bioaccumulation in invertebrates and fish. Studies on human exposure to PCDD/Fs and the possible effects on hypermineralization of teeth as well as an epidemiological study to reveal increased cancer risk were also conducted. An assessment of the ecological and human health risks with a null hypothesis (no remediation) was undertaken.

Results: The sediment survey revealed severe contamination of river and coastal sediments with PCDD/Fs and Hg. The total volume of contaminated sediments was estimated to reach 5x10(6) m3 and hot spots with extremely high concentrations (max 292,000 ng g(-1) or 1,060 ng I-TEQ g(-1) d.w.) were located immediately downstream from the pollution source (approximately 90,000 m3). Sediment contamination was accompanied by changes in benthic assemblages, but direct effects were masked by many factors. The fish showed only slightly elevated PCDD/F levels in muscle, but orders of magnitude higher in the liver compared with reference freshwater sites and the Baltic Sea. The concentrations in human fat did not reveal high human exposure in the Kymijoki area in general and was lower than in sea fishermen. The relative risk for total cancer among farmers was marginally higher (RR=1.13) among those living close to the river, compared with farmers living further away, and the possibility of increased cancer risk cannot be ruled out. A conservative risk assessment revealed that the present probability of exceeding the WHO upper exposure limit of 4 pg WHO-TEQ kg(-1) d(-1) for PCDD/Fs and DL-PCBs was 6%. The probability of exceeding the WHO limit value of 0.23 mug kg(-1) d(-1) for methyl mercury was estimated to be notably higher at 62%. Based on these studies and the estimated risks connected with different remediation techniques a general remediation plan with cost benefit analysis was generated for several sub-regions in the river. Dredging, on-site treatment, and a close disposal of the most contaminated sediments (90,000 m3) was suggested as the first phase of the remediation. The decision regarding the start of remediation will be made during autumn 2008.

Conclusions: The sediments in the River Kymijoki are heavily polluted with PCDD/Fs and mercury from earlier chlorophenol, chlor-alkali, and pulp and paper manufacturing. A continuous transport of contaminants is taking place to the Gulf of Finland in the Baltic Sea. The highly increased PCDD/F and Hg levels in river sediments pose an ecotoxicological risk to benthic fauna, to fish-eating predators and probably to human health. The risks posed by mercury exceed those from PCDD/Fs and need to be evaluated for (former) chlor-alkali sites and other mercury releasing industries as one basis for remediation decision making.

Recommendations And Perspectives: The studies form the basis of a risk management strategy and a plan for possible remediation of contaminated sediments currently under consideration in the Southeast Finland Regional Environment Centre. It is recommended that a detailed restoration plan for the most seriously contaminated areas should be undertaken. Based on current knowledge, the restoration of the whole river is not feasible, considering the current risk caused by the contaminated sediment in the river and the costs of an extensive restoration project. The experiences gained in the present case should be utilized in the evaluation of PCDD/F- and mercury-contaminated sites in other countries. The case demonstrates that the historic reservoirs are of contemporary relevance and should be addressed, e.g., in the national implementation plans of the Stockholm Convention.
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http://dx.doi.org/10.1007/s11356-008-0061-9DOI Listing
January 2009

Contamination of River Kymijoki sediments with polychlorinated dibenzo-p-dioxins, dibenzofurans and mercury and their transport to the Gulf of Finland in the Baltic Sea.

Chemosphere 2008 Nov 20;73(10):1675-83. Epub 2008 Sep 20.

Finnish Environment Institute, Helsinki, Finland.

Kymijoki, the fourth largest river in Finland, has been heavily polluted by pulp mill effluents as well as the chemical industry. Up to 24,000 ton of wood preservative, chlorophenol known as Ky-5, was manufactured in the upper reaches of the river, an unknown amount of which was discharged into the river between 1940 and 1984. Polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) occurred as impurities in the final Ky-5 product. The PCDD/F concentrations and burden in the river sediments were studied and the transport of PCDD/Fs from contaminated sites downstream and into the Gulf of Finland in the Baltic Sea was estimated. More than 190 sediment cores were sampled to estimate the volume of contaminated sediments and the total PCDD/F burden. The transport of PCDD/Fs was estimated using sediment traps placed at several sites. The survey revealed that sediments in the river were heavily polluted by PCDD/Fs, the main toxic congener being 1,2,3,4,6,7,8-heptachlorodibenzofuran, a major contaminant in the Ky-5 product. The mean total concentration at the most polluted river site downstream from the main source was 42000 microg kg(-1) d.w. (106 microg I-TEQ kg(-1)). The elevated concentrations in the coastal region and the present estimated transport from the River Kymijoki confirm earlier assessments that the river is a major source of PCDD/F for the Gulf of Finland.
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http://dx.doi.org/10.1016/j.chemosphere.2008.07.085DOI Listing
November 2008

Organohalogen pollutants in herring from the northern Baltic Sea: concentrations, congener profiles and explanatory factors.

Environ Pollut 2008 Jul 4;154(2):172-83. Epub 2007 Dec 4.

National Public Health Institute, Department of Environmental Health, P.O. Box 95, FI-70701 Kuopio, Finland.

Organohalogen contaminants were investigated in Baltic herring caught from three catchment areas in the Baltic Sea, off the coasts of Finland. Pools of both small and large herring were analysed for polychlorinated biphenyls (PCB), dibenzo-p-dioxins, dibenzofurans, naphthalenes, camphenes (toxaphene), polybrominated diphenyl ethers and the pesticide DDT and its metabolites. PCB concentrations per fresh weight in small herring were at the same level in all catchment areas, i.e. the Bothnian Bay, the Bothnian Sea and the Gulf of Finland, revealing no hot spots and reflecting most likely long term emissions and atmospheric deposition. Differences in the levels and/or congener profiles of other contaminants between catchment areas may be explained by point sources. Similar concentrations in small and large herring in the Gulf of Finland were possibly due to their common nutrition. In the other areas, differences between small and large herring most likely reflected their different food sources.
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http://dx.doi.org/10.1016/j.envpol.2007.10.019DOI Listing
July 2008

Dioxin exposure in contaminated sawmill area: the use of molar teeth and bone of bank vole (Clethrionomys glareolus) and field vole (Microtus agrestis) as biomarkers.

Chemosphere 2007 Jun 1;68(5):951-7. Epub 2007 Mar 1.

National Public Health Institute, Department of Environmental Health, Kuopio, Finland.

Developmental disorders of teeth are among the most sensitive targets of polychlorinated dibenzo-p-dioxin and -furan (PCDD/F) exposure. In rats, 2,3,7,8-tetrachlorodibenzo-p-dioxin (TCDD) reduces dose-dependently the size of molars, most severely the third lower molars. Dioxins also have effects on developing bone, including altered bone mineral density as well as reduced bending breaking force and stiffness. The aim of this study was to evaluate the use of the third lower molar and long bones as biomarkers of PCDD/F exposure in two wild vole species, the bank vole (Clethrionomys glareolus) and the field vole (Microtus agrestis) collected from a PCDD/F contaminated former sawmill area. Survey of soil and biota of the sawmill area indicated a PCDD/F contamination with a congener profile characteristic for the chlorophenol wood preservative Ky-5. The PCDD/F concentration in the bank vole was notably higher than in the field vole. The third molar of the bank vole was significantly smaller in dioxin-exposed animals compared to control group, while there was no difference between these two groups in the field vole. No significant alterations were observed in bone density and strength in either species except for reduced bending strength of the femur neck in bank vole males exposed to dioxins. Even though the bone changes are among the sensitive endpoints of dioxin-exposure, high variability due to age, size and gender limits their use as biomarkers of wildlife exposure. In conclusion, the size of molar teeth seems to be a sensitive and robust biomarker for PCDD/F exposure in wild bank vole populations and thus worth of further studies.
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http://dx.doi.org/10.1016/j.chemosphere.2007.01.030DOI Listing
June 2007

Dioxin concentrations in sediments of the Baltic Sea--a survey of existing data.

Chemosphere 2007 Apr 16;67(9):1762-75. Epub 2007 Jan 16.

Finnish Environment Institute (SYKE), P.O. Box 140, FI-00251 Helsinki, Finland.

Recent survey results for polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs, dioxins) in Baltic Sea sediments from Finland, Sweden and Denmark were merged with previously published Baltic Sea data. Regional distribution of concentration levels, differences in congener patterns, and temporal changes in sediment profiles were examined. One of the main objectives was to study if any major point sources for different PCDD/F congeners could be identified on a regional scale, based on sediment records. The survey confirmed the impact of chlorophenol production derived highly chlorinated PCDF-congeners on the total toxicity in sediments in the Gulf of Finland near the Kymijoki river estuary. Signatures of other point sources or combined point sources pertinent to specific industry branches or particular production processes (such as pulp bleaching, vinyl chloride production, thermal processes) may be discerned. However, the findings did not support any of the known point sources significantly influencing those congeners that are most abundant in Baltic herring and salmon. Instead, regional distributions in the Baltic Sea indicate that atmospheric deposition may act as a major source for those congeners and especially for 2,3,4,7,8-PeCDF. There were clear indications of declines in levels in sediment in some areas, but generally the levels of highly chlorinated PCDD/Fs on the northern coast of the Gulf of Finland were still high when compared with other areas of the Baltic Sea. Major areas with data gaps cover the south-eastern and eastern coastal regions of the Baltic Proper and the southern Gulf of Finland.
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http://dx.doi.org/10.1016/j.chemosphere.2006.05.125DOI Listing
April 2007

Chemical inhibition of PCDD/F formation in incineration processes.

Sci Total Environ 2004 Jun;325(1-3):83-94

Department of Environmental Sciences, University of Kuopio, P.O. Box 1627, FIN-70211 Kuopio, Finland.

This review summarises results of our pilot-scale experiments to find suitable inhibitors for preventing the formation of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/F) during waste incineration and to specify the role of the main factors affecting the inhibition process, and is based on doctoral dissertation of Ruokojaärvi (2002). Results of previous experiments reported by other researchers are also presented and compared with ours. The detailed aims of our experiments were (1) to compare the effects of different inhibitors on PCDD/F formation during incineration in a pilot plant, (2) to investigate the role of the particle size distribution of the flue gas on the inhibition of PCDD/Fs, and (3) to find the main parameters affecting PCDD/F inhibition in waste incineration. Prevention of the formation of PCDD/Fs with chemical inhibitors and the effects of different supply points, feed temperatures and process parameters were studied in a pilot scale incinerator (50 kW) using light heating oil and refuse-derived fuel as test fuels. Various concentrations of the gaseous inhibitors (sulfur dioxide, ammonia, dimethylamine and methyl mercaptan) were sprayed into the flue gases after the furnace, in addition to which urea was dissolved in water and injected in at different concentrations. The residence time of the flue gas between the furnace and the PCDD/F sampling point was varied in the tests. In another set of urea tests, urea-water solutions at three concentrations were mixed with the RDF prior to incineration. PCDD/F and chlorophenol concentrations, together with other flue gas parameters (e.g. temperature, O2, CO, CO2 and NO), were analysed in the cooling flue gases. The gaseous and liquid inhibitors both notably reduced PCDD/F concentrations in the flue gas, the reductions achieved with the gaseous inhibitors varying from 50 to 78%, with dimethyl amine the most effective, while that produced with urea was up to 90%. The PCDD/F reductions were greater at increased inhibitor concentrations and with increased residence time of the flue gas between the furnace and the sampling point. PCDD/F concentrations in the particle phase decreased much more markedly than those in the gas phase. The urea inhibitor did not alter the particle size distribution of the PCDD/Fs when the amount of inhibitor was adequate. Chemical inhibitors seem to offer a very promising technique for preventing the formation of PCDD/Fs in waste incineration. The addition of urea to the fuel before combustion proved to be very effective approach and could be a useful technique even in the full-scale incinerators.
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http://dx.doi.org/10.1016/j.scitotenv.2003.11.006DOI Listing
June 2004

Perspectives on the formation of polychlorinated dibenzo-p-dioxins and dibenzofurans during municipal solid waste (MSW) incineration and other combustion processes.

Acc Chem Res 2003 Sep;36(9):652-8

Department of Chemistry, University of Kuopio, P.O. Box 1627, 70211 Kuopio, Finland.

The pathways by which polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) are formed and the interactions between their aromatic precursors, in particular chlorophenols (ClPhs), and transition metal catalysts are discussed. A literature survey and data from pilot-scale combustion experiments allow conclusions to be drawn on the relations between ClPhs and PCDD/Fs in municipal waste incineration and other combustion processes. The results suggest that the ClPh pathway is among the most important for the formation of PCDD/Fs.
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http://dx.doi.org/10.1021/ar020104+DOI Listing
September 2003