Heavy Metals in the Bed and Suspended Sediments of Anyang River, Korea: Implications for Water Quality

The objective of this study is to compare Anyang River bed sediments with water chemical composition and to assess the anthropogenic chemical inputs into the river system. Eight sampling locations were chosen along the river channel. Bed and suspended river sediments and water samples were collected, and analyzed for their chemical and physical composition. Data revealed that trace element concentrations in the river water were generally below world average, except for As, Mn, Ni and Cr. Among the three phases: water, bed and suspended sediment, more than 99% of the trace elements was associated with the bed sediment. Concentrations of trace elements in the sediment were a function a particle size distribution and organic content. The calculated degrees of enrichment based on the least influenced sample (ASD 1) indicated the river sediments were enriched with respect to background. The enrichment factors for Pb, Zn and As were relatively lower than for Cr, Co, Ni and Zn. The difference in the enrichment seems to reflect the human activities influence in the basin, and specially for Cd. Speciation of the elements in the five different chemical forms in the sediment by sequential extraction indicated that the reducible fraction was predominant for Fe, Zinc and Cu showed an irregular variation among the different fractions; whereas, Cd and Pb were more regular. Zinc and Cu highly existed mostly in exchangeable forms. Acid soluble and reducible forms were also important for most metals. The speciation implies that the metals associated with the sediment are subject to release into water bodies as goechemical variables (pH and Eh) change. Currently, the introduced metals are deposited near the source area and are mostly associated with the sediment, implying that the river bed sediment acts mainly as a sink, rather than a pool. The accumulated and enriched toxic trace elements can pose a potential pollution of river water.     

Lysosomal,genetic and chromosomal damage in haemocytes of the freshwater bivalve (Unio pictorum) exposed to polluted sediments from the River Cecina (Italy)

The response to chemical disturbance of an Italian river (Cecina River) characterised by high levels of trace metals was assessed in the sentinel species freshwater painter’s mussel (Unio pictorum). We exposed U. pictorum in the laboratory to metal, metalloid and other trace element polluted river sediments in order to evaluate genetic and cellular biomarkers. Bivalves exposed to sediments taken from all the impacted sites of the river basin exhibited a significant impairment at the DNA, chromosomal and lysosomal levels. The lysosomal membrane stability of circulating haemocytes, assessed by the Neutral Red Retention Time, was found to be higher in specimens from Lake Maggiore and Berignone, while exhibited a significant decrease in specimens exposed to Ponteginori sediments. An increase of DNA migration in specimens exposed to the two contaminated sites in comparison with controls was found. Moreover, higher micronucleated haemocytes frequencies were observed in bivalves exposed to sediments collected at Possera 1 site. This study suggested that biomarkers evaluating cellular impairment, genetic and chromosomal damages, are highly sensitive and suitably applied to laboratory experiments. The painter’s mussel was confirmed to be an appropriate sentinel species for quality assessment in metal-contaminated freshwater environments.     

长江南京段近岸沉积物中重金属富集特征与形态分析

在对长江南京段八卦洲和杨中两个冲积洲近岸沉积物及其优势野生植物中A1、Cu、zn、Cr、Pb、Nj和Cd元素含量分析的基础上,分别考查了这些重金属的富集系数(EF)和生物富集因子(BCF),并采用BCR连续提取法对Cd的赋存形态进行了研究.结果表明,本区域长江近岸沉积物和野生植物中重金属存在不同程度的富集现象,两洲沉积物中Cu、Cr、Pb、Ni、Cd均有富集趋势,各元素EF>1的样品占总样品比例分别为Cu 50%、Cr40%、Pb40%、Ni 40%、Cd20%.而在野生桐蒿和芦蒿两种优势植物中Cd富集显著,其中桐蒿的BCF平均值高达2.57.采用BCR连续提取法对沉积物中Cd进行形态分析,结果显示,沉积物中Cd主要以酸溶/交换态(B1)和可还原态(B2)为主,二者分别为31.7%和45.5%,占到总量的70%以上,B1态远高于一般土壤和沉积物中重金属的分布,表现出很强的迁移性和生物可利用性.新生成沉积物较老沉积物中的B1态有显著增加,反映出沉积物越新,Cd的迁移性越强的趋势.研究结果说明长江城市段近岸沉积物中Cd受近期人为因素影响明显,具有一定的生态风险.     

Inorganic and organic contaminants in sediments from an urban playa and associated toxicity among Hyalella azteca

Playa wetlands are important components of the Southern High Plains (USA) landscape as they are the major aquatic surface feature. Chemical contaminants associated with playas have been documented, particularly for grassland and agricultural watersheds, but not for playas in urban settings. The objectives of this study were to determine concentrations of inorganic and organic contaminants in sediments from an urban playa within the I-20 Wildlife Preserve and Jenna Welch Nature Study Center in Midland, TX, and evaluate toxicity of these sediments to Hyalella azteca. Concentrations of most trace elements were below sediment quality guidelines with exceptions of lead, cadmium, and arsenic. Concentrations of organic contaminants, particularly PAHs, DDT, DDE, and malathion, were above sediment quality guidelines at various locations within the playa. Decreased survival was observed among H. azteca exposed to sediment from a single location when compared those exposed to reference sediments. This location also produced maximum observed concentrations for five of seven trace elements, potentially due to its location at the lowest elevation within the playa. This study documented concentrations of contaminants in sediments of an urban playa associated with past and present land uses in its urban setting, including those from automotive emissions and historical pesticide use.     

Use of the digestive gland of the oyster Crassostrea rhizophorae (Guilding, 1828) as a bioindicator of Zn,Cd and Cu contamination in estuarine sediments (south-east Brazil)

This study demonstrates the accumulation of Zn, Cd and Cu in the digestive gland of the oyster Crassostrea rhizophorae in response to the contamination of sediments and discusses the potential use of this specific organ in monitoring metal contamination in tropical areas. Sediment and oyster samples were collected from coastal Rio de Janeiro sites with different levels of human impact: Sepetiba Bay, Guanabara Bay and the Paraty coast. Metal concentrations were measured using inductively coupled plasma optical emission spectrometry (ICP OES). Significant statistical differences (p<0.001; p<0.05) were observed for Zn and Cd concentrations in the digestive gland; the highest Zn concentrations were found at Sepetiba, followed by Guanabara and Paraty. The highest digestive gland Cd concentrations were found at Paraty, followed by Sepetiba and Guanabara. These concentrations were proportional to those found in the sediments. There was no significant difference (p>0.05) in Cu among the sampling sites. The highest digestive-gland Cu concentration was also found at Sepetiba, followed by Guanabara. The biosediment accumulation factor indicated a gradient of sediment contamination for Zn and Cd. The digestive gland of C. rhizophorae can be a potential indicator of trace metal contamination in sediments from tropical estuarine environments.     

Historical trends of trace metals in a sediment core from a contaminated tidal salt marsh in San Francisco Bay

Sedimentation of metals preserves historical records of contaminant input from local and regional sources, and measurement of metals in sediment cores can provide information for reconstruction of historical changes in regional water and sediment quality. Sediment core was collected from Stege Marsh located in central San Francisco Bay (California, USA) to investigate the historical input of trace metals. Aluminum-normalized enrichment factors indicate that inputs from anthropogenic sources were predominant over natural input for Ag, Cu, Pb, and Zn. Among these, lead was the most anthropogenically impacted metal with enrichment factors ranging from 32 to 108. Depth profiles and coefficients of variation show that As, Cd, and Se were also influenced by anthropogenic input. The levels of these anthropogenically impacted metals decline gradually towards the surface due to regulation of the use of leaded gasoline, municipal and industrial wastewater discharge control, and closure of point sources on the upland of Stege Marsh. Although trace metal contamination is expected to be continuously declining, the rates of decline have slowed down. For lead, it is estimated to take 44, 82, and 153 years to decrease to probable effects level (112 μg/g), the San Francisco Bay ambient surface sediment level (43.2 μg/g), and the local baseline levels (5 μg/g), respectively. Some metals in surface sediments (0–6 cm) are still higher than sediment quality guidelines such as the probable effects level. To further facilitate the recovery of sediment quality, more efficient management plans need to be developed and implemented to control trace metals from non-point sources such as stormwater runoff.     

Mercury in surface sediments and benthic organisms from Guaymas Bay,east coast of the Gulf of California

In order to know the concentration of mercury in surface sediments, macroalgae and clams from Guaymas Bay, Mexico, 20 surface sediment samples and several individuals of Codium amplivesciculatum (3), Enteromorpha clathrata (4), Gracilaria subsecundata (2), Ulva lactuca (2), Chione subrugosa (80) and Crassostrea gigas (40) were collected and their Hg concentration was measured by a cold vapor Hg analyzer, after acid digestion. In addition, granulometric analysis and quantification of total organic carbon, aluminum, iron and manganese contents in sediments were performed. A Pearsons correlation matrix was determined and, the enrichment factor, the geoaccumulation index and the biota-sediment accumulation factor were calculated. Mercury concentrations in sediments ranged from 0.3 to 2.3 μg g⁻¹, with the central and northern portions showing the highest values. Macroalgae had a content of Hg that oscillated from 0.058 to 0.134 μg g⁻¹, while the average concentrations of this metal for clams and oysters were 0.063 and 0.230 μg g⁻¹, respectively. A clear effect of Guaymas City and the anthropogenic activities carried out around the Guaymas Bay has been observed and the enrichment factor and the geochemical index suggest that sediments from this coastal ecosystem are moderately to strongly contaminated with Hg. However, according to the figure of the maximum human consumption of Hg per week recommended by the World Health Organization, people can ingest clams without risk to their health.     

Assessment of potentially harmful elements pollution in the Calore River basin (Southern Italy)

The geographical distribution of concentration values for harmful elements was determined in the Campania region, Italy. The study area consists of the drainage basin of the River Calore, a tributary of the river Volturno, the largest Southern Italian river. The results provide reliable analytical data allowing a quantitative assessment of the trace element pollution threat to the ecosystem and human health. Altogether 562 stream sediment samples were collected at a sampling density of 1 site per 5 km². All samples were air-dried, sieved to <100 mesh fraction and analyzed for 37 elements after an aqua regia extraction by a combination of ICP-AES and ICP-MS. In addition to elemental analysis, gamma-ray spectrometry data were collected (a total of 562 measurements) using a hand-held Scintrex GRS-500 spectrometer. Statistical analyses were performed to show the single-element distribution and the distribution of elemental association factor scores resulting from R-mode factor analyses. Maps showing element distributions were made using GeoDAS and ArcGIS software. Our study showed that, despite evidence from concentrations of many elements for enrichment over natural background values, the spatial distribution of major and trace elements in Calore River basin is determined mostly by geogenic factors. The southwestern area of the basin highlighted an enrichment of many elements potentially harmful for human health and other living organisms (Al, Fe, K, Na, As, Cd, La, Pb, Th, Tl, U); however, these anomalies are due to the presence of pyroclastic and alkaline volcanic lithologies. Even where sedimentary lithologies occur, many harmful elements (Co, Cr, Mn, Ni) showed high concentration levels due to natural origins. Conversely, a strong heavy metal contamination (Pb, Zn, Cu, Sb, Ag, Au, Hg), due to an anthropogenic contribution, is highlighted in many areas characterized by the presence of road junctions, urban settlements and industrial areas. The enrichment factor of these elements is 3–4 times higher than the background values. The southwestern area of the basin is characterized by a moderate/high degree of contamination, just where the two busiest roads of the area run and the highest concentration of industries occurs.     

Elemental composition of bottom-sediments from Pangani river basin,Tanzania: lithogenic and anthropogenic sources

River-bed sediments from the Pangani basin, Tanzania, were characterized for elemental compositions, following contamination risks from rapid expansions of human activities in the area. Samples were collected during two individual seasons and analyzed by high-polarizing beam energy dispersive X-ray fluorescence (EDXRF) for eight major and 14 trace elements. Evaluation of enrichment factors (EFs) was used to investigate the elemental flux and assess the contributions of natural and anthropogenic influences. The abundances of the major elements followed the order Si?>?Al?>?Fe?>?Ca?>?K?>?Ti?>?Mn?>?P, similar to that of the upper earth's crust, and were generally from the weathering of the bed-rock. The high concentrations of typical anthropogenic trace-elements (Cr??1, V??1, Ni??1, Cu??1, La??1) coupled with high EFs (>2) in some locations indicated contamination associated with agricultural and industrial activities. Factor analysis extracted five principal components that contributed to 96.0% of the total observed variance. The results indicated that river-bed sediments of the Pangani basin were influenced to a larger extent by lithogenic sources than anthropogenic impacts.     

Trace element contents in fine particulate matter (PM<Subscript>2.5</Subscript>) in urban school microenvironments near a contaminated beach with mine tailings,Chañaral,Chile

Air quality in schools is an important public health issue because children spend a considerable part of their daily life in classrooms. Particulate size and chemical composition has been associated with negative health effects. We studied levels of trace element concentrations in fine particulate matter (PM_2.5) in indoor versus outdoor school settings from six schools in Chañaral, a coastal city with a beach severely polluted with mine tailings. Concentrations of trace elements were measured on two consecutive days during the summer and winter of 2012 and 2013 and determined using X-ray fluorescence. Source apportionment and element enrichment were measured using principal components analysis and enrichment factors. Trace elements were higher in indoor school spaces, especially in classrooms compared with outdoor environments. The most abundant elements were Na, Cl, S, Ca, Fe, K, Mn, Ti, and Si, associated with earth’s crust. Conversely, an extremely high enrichment factor was determined for Cu, Zn, Ni and Cr; heavy metals associated with systemic and carcinogenic risk effects, whose probably origin sources are industrial and mining activities. These results suggest that the main source of trace elements in PM_2.5 from these school microenvironments is a mixture of dust contaminated with mine tailings and marine aerosols. Policymakers should prioritize environmental management changes to minimize further environmental damage and its direct impact on the health of children exposed.     

Trace Metal Distribution and Enrichment in Benthic, Estuarine Sediments: Southport Broadwater, Australia

The distribution and enrichment of selected trace metals (Cd, Cr, Cu, Ni, Pb, Sn, Zn) in benthic sediments of the Southport Broadwater, a semi-enclosed coastal body of water adjacent to the Gold Coast city, south-eastern Queensland, Australia, was studied with the objective of assessing the extent and degree of sediment contamination. Sediment samples from the 0–10 cm and 10–20 cm depth intervals of 32 sites within the Southport Broadwater and surrounding residential canals were analysed for particle size distribution, pH, organic C and ‘near-total’ major (Al, Ca, Fe, Mn) and trace (Cd, Cr, Cu, Ni, Pb, Sn, Zn) metal contents. Sediment contamination for each trace metal was assessed by (1) comparison with Australian sediment quality guidelines, (2) calculation of the index of geoaccumulation based on regional background values, and (3) geochemical normalisation against Al (i.e. the abundance of alumino-silicate clay minerals). Based on this approach, the results indicate that submerged sediments in the study area are not presently enriched with Cd, Cr or Ni, with the spatial distribution of these metals being very well explained by the abundance of alumino-silicate clay minerals. However, several sites were strongly enriched with Cu, Pb, Sn and Zn, arising from sources related to either urban runoff or vessel maintenance activities. The study indicates that several varying approaches are needed for a satisfactory assessment of contaminant enrichment in estuarine sediments.     

Trace elements distributions at Datoko-Shega artisanal mining site,northern Ghana

Environmental geochemistry classifies elements into essential, non-essential and toxic elements in relationship to human health. To assess the environmental impact of mining at Datoko-Shega area, the distributions and concentrations of trace elements in stream sediments and soil samples were carried out. X-ray fluorescence analytical technique was used to measure the major and trace element concentrations in sediments and modified fire assay absorption spectrometry in soils. The results showed general depletion of major elements except titanium oxide (TiO₂) compared to the average crustal concentrations. The retention of TiO₂ at the near surface environment probably was due to the intense tropical weathering accompanied by the removal of fine sediments and soil fractions during the harmattan season by the dry north-east trade winds and sheet wash deposits formed after flash floods. The results also showed extreme contamination of selenium (Se), cadmium (Cd) and mercury (Hg), plus strong contaminations of arsenic (As) and chromium (Cr) in addition to moderate contamination of lead (Pb) in the trace element samples relative to crustal averages in the upper continental crust. However Hg, Pb and Cd concentrations tend to be high around the artisanal workings. It was recognised from the analysis of the results that the artisanal mining activity harnessed and introduces some potentially toxic elements such as Hg, Cd and Pb mostly in the artisan mine sites. But the interpretation of the trace element data thus invalidates the elevation of As concentrations to be from the mine operations. It consequently noticed As values in the mine-impacted areas to be similar or sometimes lower than As values in areas outside the mine sites from the stream sediment results.

     

Terrigenous Inputs and Accumulation of Trace Metals in the Southeastern Taiwan Strait

Abstract

Terrigenous inputs and sedimentary fluxes of trace metals were studied to understand the metal sources, transport and sinks in the southeastern Taiwan Strait. the major terrigenous metals come from seven major rivers in the southwestern Taiwan, even though significant fractions of most metals were retained in estuaries. the net fluxes of river borne metals contributed from 65% (Pb) to 92% (Fe, Zn) of total inputs. the remainder was attributed to marine sewage discharges (0.6–6.9%) and atmospheric inputs (5.3–31.5%). Sedimentary fluxes of trace metals were spatially variable as a result of derivation from site-specific sedimentation rates and metal distributions in sediments. in spite of imbalance between sources and sinks of trace metals, an accumulation of metals in the sediment of southeastern Taiwan Strait was found for sites close to Taiwan Island. Surface enrichment of metals in near-shore sediments beginning around 1976 was coincident with a time of industrial boom in Taiwan. the metal enrichment hierarchy was found as (Cd, Pb < Cu < Zn < Mn, Fe).     

Effect of long-term irrigation with sewage effluent on the metal content of soils, Berlin, Germany

This study aimed to determine whether >110 years of sewage application has led to recognizable changes in the metal chemistry of soils from former sewage farms, Berlin, Germany. Background concentrations of soils and element enrichment factors were used for the evaluation of possible perturbations of natural element abundances in sewage farm soils. Calculations verify that precious metals (Ag, Au) as well as P, C_org, and heavy metals (Cd, Cu, Ni, Pb, Sn, and Zn) are invariably enriched in sewage farm topsoils (0–0.1 m depth) compared to local and regional background soils. Long-term irrigation of soils with municipal wastewater has caused significant heavy metal contamination as well as a pronounced enrichment in precious metals. Leaching of metals including Ag into underlying aquifers may impact on the quality of drinking water supplies.     

Assessment of Trace Metals in the Sediments From the Coastal Zone of Alexandria, Egypt

Freshly deposited surface sediments from the Alexandria coastal zone were collected and analysed in 1995 for their trace metal concentrations. Metal concentrations in the sediments vary between sites within a wide range for copper, zinc, iron, lead, chromium and cadmium. the statistical analysis between the metal concentrations and the different constituents (organic carbon, total nitrogen, silt, clay and total iron) showed significant correlations. the enrichment factors for the sediments ranged between 3 and 4-fold for copper, chromium and zinc and reached up to 9-fold for lead and 113-fold for cadmium. the highest index for cadmium and lead may be attributed to the anthropogenic inputs from the surrounding area, where they are highest in lower discharge areas.     

Assessment of Trace Metals in the Sediments From the Coastal Zone of Alexandria,Egypt

Freshly deposited surface sediments from the Alexandria coastal zone were collected and analysed in 1995 for their trace metal concentrations. Metal concentrations in the sediments vary between sites within a wide range for copper, zinc, iron, lead, chromium and cadmium. the statistical analysis between the metal concentrations and the different constituents (organic carbon, total nitrogen, silt, clay and total iron) showed significant correlations. the enrichment factors for the sediments ranged between 3 and 4-fold for copper, chromium and zinc and reached up to 9-fold for lead and 113-fold for cadmium. the highest index for cadmium and lead may be attributed to the anthropogenic inputs from the surrounding area, where they are highest in lower discharge areas.     

Geochemical index of trace metals in the surficial sediments from the western continental shelf of India, Arabian Sea

The present study focuses on the determination and abundance of trace metals (viz. Cu, Ni, Zn, Cr, Co, Cd, Mn and Fe) in the surficial sediments of west coast of Arabian Sea along the Indian subcontinent. Sediment samples were collected from three transects along the western continental shelf of Arabian Sea. The enrichment of Fe and Mn in coastal oxic-sediments indicates the precipitation of these redox sensitive elements as Fe- and Mn-hydroxides and oxides, whereas the low Fe and Mn concentrations in the oxygen deficient sediments of deeper stations reflects the dissolution of their hydroxides and oxides. Concentrations of fairly redox insensitive trace metals like Cu, Ni, Zn, Cr and Cd (with the exceptions of Cr) showed higher values at nearshore sediments, then it decreased towards seaward and again showed a slight increase at oxygen minimum stations in all the three transects. This geochemical variability in their distributional characteristics is mainly associated with the extent to which the precipitation or dissolution of Fe- and Mn-oxides/hydroxides occur since the scavenging or releasing effects of Fe- and Mn-oxides/hydroxides act as significant ‘sinks’ or ‘sources’ of heavy metals. The change in wind pattern, coastal upwelling and increased productivity are also the reported factors which influence the biogeochemical cycling of trace metals in the surface sediments of west coast of India. Enrichment factor generally showed a high gradient accumulation from nearshore to shelf.     

Assessment of enrichment,geo-accumulation and ecological risk of heavy metals in surface sediments of the Msimbazi mangrove ecosystem,coast of Dar es Salaam,Tanzania

Results of the assessment of enrichment, accumulation and the ecological risk associated with three heavy metals (Cd, Cu and Pb) and one metalloid (As) in surface sediments of Msimbazi estuary are presented. Surface sediment samples (0–5 cm) were collected from Msimbazi River estuary in September 2016 using handheld PVC short corers. Long-sediment cores from the site were also collected using PVC pipes and their vertical profiles of metals concentrations assessed with the aim of establishing site-specific baseline metals concentrations. The established site-specific baseline values were used for the determination of normalised enrichment factors (EF) and geoaccumulation (Igeo) of metals instead of using average crustal values. Iron-based enrichment factors show that the sediments of Msimbazi have experienced enrichment of metals that originate from anthropogenic sources of pollution (EF > 1). Geo-accumulation results indicate that Msimbazi sediments can be designated as uncontaminated to moderately-contaminated with As, Cd and Pb (class 1–2). Geoaccumulation indices for Cu indicate that sediment can be designated as uncontaminated to moderately contaminated (class 1) and moderately to strongly contaminated (class 3). Results show further that the Ecological Risk associated with the accumulation of these metals in Msimbazi sediments was low based on Hakanson approach.     

Heavy Metals and Arsenic in Sediments, Mussels and Marine Water from Murano (Venice, Italy)

This paper describes a study of the trace element distribution in sediments, marine water and mussel Mytilus galloprovincialis of the Venetian Lagoon around the Island of Murano, an island with a long tradition of glassmaking. Trace elements analysed include Fe, Mn, Zn, Cu, Cr, Pb, Ni, Ag and As. Sediments are contaminated with Zn, Cu, Ag, As and Pb, with levels in the <2m fraction that are likely to cause adverse biological effects to marine organisms. The pelite (<63m) is the main carrier of heavy metals at most sites. However, the fine-grained and coarse sand on the southern coast of Murano accounts for a significant proportion of Fe, Mn, Zn, Cr, Ag, Ni and Pb. Most trace element concentrations found in soft tissue of mussels appear to be within recommended Italian and international guidelines for shellfish for human consumption, the only exception being relatively high As levels. The bioaccumulation of Ag and Cr is more pronounced in the shell of these organisms. In the marine water of the lagoon, trace elements are more enriched than in other areas of the Mediterranean, with particular reference to the dissolved labile species of Zn, Mn, As, Cu, Ni and Cr.     

The potential of spatial information in human biomonitoring by example of two German environmental epidemiology studies

This study aimed at statistically investigating the association between the internal exposure of children and young adults to uranium (U) and epidemiologically relevant external determinants of exposure. The investigation was performed with data from two studies within the framework of the German health-related environmental monitoring program: The German Environmental Survey for Children (GerES IV) conducted by the Federal Environment Agency (Umweltbundesamt) with data on 1,780 children 3–14 years of age and their home environment and the German Environmental Specimen Bank (ESB, section: human specimens) with data on 2,253 students 20–29 years of age. Both studies provided data on the U levels in human urine for all probands. GerES IV furthermore provided an extensive environmental and demographic database on, e.g., U levels in drinking water. The data from GerES IV and ESB were linked by GIS to spatially relevant exposure information, including background values of U in stream sediments and in upper and lower soils, U levels in mosses and particulate matter in the lower atmosphere, precipitation and elevation as well as forest density. Bivariate correlation analysis and two decision tree models showed moderate but significant associations between U in human urine and U levels in drinking water, stream sediments and upper and lower soils. Future investigations considering additional epidemiologically relevant data sets may differentiate the results. Furthermore, the sample design of future environmental epidemiology studies should take the spatial evaluation of the data into greater account.