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The geochemistry of water near a surficial organic-rich uranium deposit, northeastern Washington State, U.S.A.

The chemistry of three stream, three spring and six near-surface waters in the vicinity of a Holocene organic-rich uranium deposit is described, with particular emphasis on the chemistry of U. Results characterize the solution behavior of uranium as U-bearing water interacts with relatively undecomposed, surficial organic matter. Of the measured major and trace chemical species, only U is consistently highly enriched (17-318 ppb) relative to reported values for regional waters, or to literature values for waters in largely granitic terrains. R-mode factor analysis of the chemical data suggests that most U is present in a soluble form, but that some U is also associated with fine suspended particulates of clay, organic matter, or hydrous oxides. Calculations that apply thermodynamic data to predict U speciation in solution indicate the relative importance of uranyl carbonate and uranyl phosphate complexes. Analysis of more finely filtered samples (0.05 ??m vs. 0.45 ??m), and direct radiographic observations using fission-track detectors suspended in the waters indicate the presence of some uraniferous particulate matter. Application of existing thermodynamic data for uranous- and uranyl-bearing minerals indicates that all waters are undersaturated with U minerals as long as ambient Eh ??? +0.1 v. If coexisting surface and near-surface waters are sufficiently oxidizing, initial fixation of U in the deposit should be by a mechanism of adsorption. Alternatively, more reducing conditions may prevail in deeper pore waters of the organic-rich host sediments, perhaps leading to direct precipitation or diagenetic formation of U4+ minerals. A 234U 238U alpha activity ratio of 1.08 ?? 0.02 in a spring issuing from a hillslope above the deposit suggests a relatively soluble source of U. In contrast, higher activity ratios of 234U 238U (??? 1.3) in waters in contact with the uraniferous valley-fill sediments suggest differences in the nature of interaction between groundwater and the local, U-rich source rocks. ?? 1987.

Chemical Geology

The water, deuterium, gas and uranium content of tektites

The water content, deuterium concentration of the water, total gas and uranium contents were determined on tektite samples and other glass samples from Texas, Australia, Philippine Islands, Java, French Indo-China, Czechoslovakia, Libyan Desert, Billiton Island, Thailand, French West Africa, Peru, and New Mexico. The water content ranges from 0.24 per cent for the Peru tektite, to 0.0002 per cent for a moldavite. The majority of the tektites have less than 0.05 per cent water, and average 0.005 per cent H 2 O by weight. No other gases were detected, the lower detection limit being about 1 p.p.m. by weight. The deuterium content of the water in tektites is in the same range as that in terrestrial waters, and varies from 0.010 mole per cent to 0.0166 mole per cent deuterium. The uranium content is about from 1 to 3 p.p.m. The possible origin of tektites is discussed. The experimental data presented favour their being originally terrestrial, but produced by some catastrophic event. An extra-terrestrial source is not ruled out.

Geochimica et Cosmochimica Acta

Release of 226Ra from uranium mill tailings by microbial Fe(III) reduction

Uranium mill tailings were anaerobically incubated in the presence of H 2 with Alteromonas putrefaciens , a bacterium known to couple the oxidation of H 2 and organic compounds to the reduction of Fe(III) oxides. There was a direct correlation between the extent of Fe(III) reduction and the accumulation of dissolved 226 Ra. In sterile tailings in which Fe(III) was not reduced, there was negligible leaching of 226 Ra. The behavior of Ba was similar to that of Ra in inoculated and sterile systems. These results demonstrate that under anaerobic conditions, microbial reduction of Fe(III) may result in the release of dissolved 226 Ra from uranium mill tailings.

Applied Geochemistry

Improved enrichment factor calculations through principal component analysis: Examples from soils near breccia pipe uranium mines, Arizona, USA

The enrichment factor (EF) is a widely used metric for determining how much the presence of an element in a sampling media has increased relative to average natural abundance because of human activity. Calculation of an EF requires the selection of both a background composition and a reference element, choices that can strongly influence the result of the calculation. Here, it is shown how carefully applied, classical principal component analysis (PCA) examined via biplots can guide the selections of background compositions and reference elements. Elemental data were treated using the centered log ratio (CLR) transformation, and multiple subsets of major and trace elements were examined to gain different perspectives. The methodology was applied to a dataset of elemental soil concentrations from around breccia pipe uranium mines in Arizona, U.S.A., with most samples collected via incremental sampling methodology. Storage of ore at the surface creates the potential for wind dispersal of ore-derived material. Uranium was found to be the best individual tracer of dispersal of ore-derived material to nearby soils, with EF values up to 75. Sulfur, As, Mo, and Cu were also enriched but to lesser degrees. The results demonstrate several practical benefits of a PCA in these situations: (1) the ability to identify one or more elements best suited to distinguish a specific source of enrichment from background composition; (2) understanding how background compositions vary within and between sites; (3) identification of samples containing enriched or anthropogenic materials based upon their integrated, multi-element composition. Calculating the most representative EF values is useful for numerical assessment of enrichment, whether anthropogenic or natural. As shown here, however, the PCA and biplot method provide a visual approach that integrates information from all elements for a given subset of data in a manner that yields geochemical insights beyond the power of the EF.

Arizona

Approaches to surface complexation modeling of Uranium(VI) adsorption on aquifer sediments

Uranium(VI) adsorption onto aquifer sediments was studied in batch experiments as a function of pH and U(VI) and dissolved carbonate concentrations in artificial groundwater solutions. The sediments were collected from an alluvial aquifer at a location upgradient of contamination from a former uranium mill operation at Naturita, Colorado (USA). The ranges of aqueous chemical conditions used in the U(VI) adsorption experiments (pH 6.9 to 7.9; U(VI) concentration 2.5 · 10 −8 to 1 · 10 −5 M; partial pressure of carbon dioxide gas 0.05 to 6.8%) were based on the spatial variation in chemical conditions observed in 1999–2000 in the Naturita alluvial aquifer. The major minerals in the sediments were quartz, feldspars, and calcite, with minor amounts of magnetite and clay minerals. Quartz grains commonly exhibited coatings that were greater than 10 nm in thickness and composed of an illite-smectite clay with occluded ferrihydrite and goethite nanoparticles. Chemical extractions of quartz grains removed from the sediments were used to estimate the masses of iron and aluminum present in the coatings. Various surface complexation modeling approaches were compared in terms of the ability to describe the U(VI) experimental data and the data requirements for model application to the sediments. Published models for U(VI) adsorption on reference minerals were applied to predict U(VI) adsorption based on assumptions about the sediment surface composition and physical properties (e.g., surface area and electrical double layer). Predictions from these models were highly variable, with results overpredicting or underpredicting the experimental data, depending on the assumptions used to apply the model. Although the models for reference minerals are supported by detailed experimental studies (and in ideal cases, surface spectroscopy), the results suggest that errors are caused in applying the models directly to the sediments by uncertain knowledge of: 1) the proportion and types of surface functional groups available for adsorption in the surface coatings; 2) the electric field at the mineral-water interface; and 3) surface reactions of major ions in the aqueous phase, such as Ca 2+ , Mg 2+ , HCO 3 − , SO 4 2− , H 4 SiO 4 , and organic acids. In contrast, a semi-empirical surface complexation modeling approach can be used to describe the U(VI) experimental data more precisely as a function of aqueous chemical conditions. This approach is useful as a tool to describe the variation in U(VI) retardation as a function of chemical conditions in field-scale reactive transport simulations, and the approach can be used at other field sites. However, the semi-empirical approach is limited by the site-specific nature of the model parameters.

Geochimica et Cosmochimica Acta

The effect of calcium on aqueous uranium(VI) speciation and adsorption to ferrihydrite and quartz

Recent studies of uranium(VI) geochemistry have focused on the potentially important role of the aqueous species, CaUO 2 (CO 3 ) 3 2− and Ca 2 UO 2 (CO 3 ) 3 0 (aq), on inhibition of microbial reduction and uranium(VI) aqueous speciation in contaminated groundwater. However, to our knowledge, there have been no direct studies of the effects of these species on U(VI) adsorption by mineral phases. The sorption of U(VI) on quartz and ferrihydrite was investigated in NaNO 3 solutions equilibrated with either ambient air (430 ppm CO 2 ) or 2% CO 2 in the presence of 0, 1.8, or 8.9 mM Ca 2+ . Under conditions where the Ca 2 UO 2 (CO 3 ) 3 0 (aq) species predominates U(VI) aqueous speciation, the presence of Ca in solution lowered U(VI) adsorption on quartz from 77% in the absence of Ca to 42% and 10% at Ca concentrations of 1.8 and 8.9 mM, respectively. U(VI) adsorption to ferrihydrite decreased from 83% in the absence of Ca to 57% in the presence of 1.8 mM Ca. Surface complexation model predictions that included the formation constant for aqueous Ca 2 UO 2 (CO 3 ) 3 0 (aq) accurately simulated the effect of Ca 2+ on U(VI) sorption onto quartz and ferrihydrite within the thermodynamic uncertainty of the stability constant value. This study confirms that Ca 2+ can have a significant impact on the aqueous speciation of U(VI), and consequently, on the sorption and mobility of U(VI) in aquifers.

Geochimica et Cosmochimica Acta

Microbial carbon cycling in oligotrophic regional aquifers near the Tono Uranium Mine, Japan as inferred from δ13C and Δ14C values of in situ phospholipid fatty acids and carbon sources

Microorganisms are ubiquitous in deep subsurface environments, but their role in the global carbon cycle is not well-understood. The natural abundance δ 13 C and Δ 14 C values of microbial membrane phospholipid fatty acids (PLFAs) were measured and used to assess the carbon sources of bacteria in sedimentary and granitic groundwaters sampled from three boreholes in the vicinity of the Tono Uranium Mine, Gifu, Japan. Sample storage experiments were performed and drill waters analyzed to characterize potential sources of microbial contamination. The most abundant PLFA structures in all waters sampled were 16:0, 16:1ω7 c , cy 17:0, and 18:1ω7 c . A PLFA biomarker for type II methanotrophs, 18:1ω8 c , comprised 3% and 18% of total PLFAs in anoxic sedimentary and granitic waters, respectively, sampled from the KNA-6 borehole. The presence of this biomarker was unexpected given that type II methanotrophs are considered obligate aerobes. However, a bacterium that grows aerobically with CH 4 as the sole energy source and which also produces 56% of its total PLFAs as 18:1ω8 c was isolated from both waters, providing additional evidence for the presence of type II methanotrophs. The Δ 14 C values determined for type II methanotroph PLFAs in the sedimentary (−861‰) and granite (−867‰) waters were very similar to the Δ 14 C values of dissolved inorganic carbon (DIC) in each water (∼−850‰). This suggests that type II methanotrophs ultimately derive all their carbon from inorganic sources, whether directly from DIC and/or from CH 4 produced by the reduction of DIC. In contrast, δ 13 C values of type II PLFAs in the sedimentary (−93‰) and granite (−60‰) waters indicate that these organisms use different carbon assimilation schemes in each environment despite very similar δ 13 C CH 4 "> δ13CCH4 values (∼−95‰) for each water. The δ 13 C PLFA values (−28‰ to −45‰) of non-methanotrophic bacteria in the KNA-6 LTL water do not clearly distinguish between heterotrophic and autotrophic metabolisms, but Δ 14 C PLFA values indicate that >65% of total bacteria filtered from the KNA-6 LTL water are heterotrophs. Ancient Δ 14 C values (∼−1000‰) of some PLFAs suggest that many heterotrophs utilize ancient organic matter, perhaps from lignite seams within the sedimentary rocks. The more negative range of δ 13 C PLFA values determined for the KNA-6 granitic water (−42‰ to −66‰) are likely the result of a microbial ecosystem dominated by chemolithoautotrophy, perhaps fuelled by abiogenic H 2 . Results of sample storage experiments showed substantial shifts in microbial community composition and δ 13 C PLFA values (as much as 5‰) during 2–4 days of dark, refrigerated, aseptic storage. However, water samples collected and immediately filtered back in the lab from freshly drilled MSB-2 borehole appeared to maintain the same relative relationships between δ 13 C PLFA values for sedimentary and granitic host rocks as observed for samples directly filtered under artesian flow from the KNA-6 borehole of the Tono Uranium Mine.

Tono Uranium Mine

Anthropogenic and geologic causes of anomalously high uranium concentrations in groundwater used for drinking water supply in the southeastern San Joaquin Valley, CA

Concentrations of uranium (U) >30 µg/L in groundwater are relatively uncommon in drinking water in the United States but can be of concern in those areas where complex interactions of aquifer materials and anthropogenic alterations of the natural flow regime mobilize uranium. High concentrations (>30 µg/L) of U in the southeastern San Joaquin Valley, California, USA, have been detected in 24 percent of 257 domestic, irrigation, and public-supply wells sampled across an approximately 110,000 km2 area. The location of high concentrations depends on the interactions of U sources from fluvial fans that originate in the Sierra Nevada to the east and seepage of irrigation water that contains high concentrations of HCO3 that leaches U from the sediments. In addition, interactions with phosphate (PO4) from fertilized irrigated fields may sequester U in the aquifer. Principal component analysis of the data demonstrates that HCO3 and ions associated with high total dissolved solids in the aquifer and the percentage of agriculture near the well sampled are associated with high U concentrations. Nitrate concentrations do not appear to control release of U to the aquifer. Age dating of the groundwater and generally increasing U concentrations of the past 25 years in resampled wells where irrigation is prevalent suggests that high U concentrations are associated with younger water, indicating that irrigation of fields over the past 100 years has significantly contributed to increasing concentrations and mobilizing U. In some places, the groundwater is supersaturated with uranyl-containing minerals, as would be expected in roll front deposits. In general, the interaction of natural geological sources high in U, the anthropogenically driven addition of HCO3 and possibly phosphate fertilizer, control the location and concentration of U in each individual fluvial fan, but the addition of nitrate in fertilizer does not appear control the location of high U. These geochemical interactions can be used to determine controls on anomalously high U in alluvial aquifers

California

Reconstructing the paleoceanographic and redox conditions responsible for variations in uranium content in North American Devonian black shales

The uranium (U) content, and more recently, the ratio between 238 U and 235 U in black shales are commonly applied as a proxy to determine redox conditions and infer organic-richness. Uranium contents typically display a linear relationship with total organic carbon (TOC) in shales. This relationship is due to the processes and mechanisms responsible for the incorporation of U into the sediment during the deposition and remineralization of organic matter. This U/TOC relationship can vary, however, and some shales display uncharacteristically low U content despite having high TOC content, while others show large enrichments of U relative to TOC. Here we examine the U to TOC ratios and U-isotope compositions of three Upper Devonian-Lower Mississippian shales: the Woodford Shale, the Cleveland Shale, and the Bakken Shale, with two study sites in Oklahoma, one site in eastern Kentucky, and three sites in eastern Montana and western North Dakota, respectively. The U/TOC ratios of each shale are distinct from one another exhibiting average ratios ranging from 3 in the Cleveland Shale, to over 10 in the Bakken Shale. The distinct geochemical composition of the three shales suggests that, although lithologically similar, each study site represents a markedly different and dynamic depositional environment. The low average U/TOC (~3) along with the relatively high δ 238 U values (~0.03‰) of the Cleveland Shale core suggests deposition along the basin margin under normal marine conditions with periods of reduced bottom water oxygenation, likely due to fluctuations in the location of the pycnocline. The Woodford Shale on the other hand, shows higher U/TOC ratios (~4, George core, ~9, Poe core) and δ 238 U (~0.02‰ average, George core, ~0.06‰ average, Poe core), which suggests an unrestricted setting with intermittent euxinic conditions. In contrast, high U/TOC ratios (2–15), and very high δ 238 U values (up to 0.55‰) in the Bakken Shale cores indicate intense metal draw-down into sediments under sulfidic waters. The results show that when the U/TOC ratios and U-isotopic compositions of each studied shale are compared to modern anoxic basins and upwelling areas, it allows for an enhanced understanding of the paleoenvironmental conditions such as basin restriction and redox state of waters within the Late Devonian epicontinental seas of North America.

Palaeogeography, Palaeoclimatology, Palaeoecology

Microbial biogeochemistry of uranium mill tailings

Uranium mill tailings (UMT) are the crushed ore residues from the extraction of uranium (U) from ores. Among the radioactive wastes associated with the nuclear fuel cycle, UMT are unique in terms of their volume and their limited isolation from the surficial environment. For this latter reason, their management and long-term fate has many interfaces with environmental microbial communities and processes. The interactions of microorganisms with UMT have been shown to be diverse and with significant consequences for radionuclide mobility and bioremediation. These radionuclides are associated with the U-decay series. The addition of organic carbon and phosphate is required to initiate the reduction of the U present in the groundwater down gradient of the mills. Investigations on sediment and water from the U-contaminated aquifer, indicates that the addition of a carbon source stimulates the rate of U removal by microbial reduction. Moreover, most attention with respect to passive or engineered removal of U from groundwaters focuses on iron-reducing and sulfate-reducing bacteria.

Advances in Applied Microbiology

Stability of dilute solutions of uranium, lead, and thorium ions

Standard solutions and samples containing a few micrograms of metallic ions per milliliter are frequently used in determination of trace elements. It is important to know whether the concentrations of such solutions remain constant from day to day. The stability of dilute solutions of three metallic ions-uranium, lead, and thorium-has been investigated. Solutions containing concentrations of metallic ions, ranging from 1000 to 0.1 γ per milliliter, were allowed to stand for approximately 2.5 months, and then the metallic ion content of those solutions that had lost strength was determined. Both adsorption and hydrolysis variously influenced the solute loss, but the minimum pH at which loss of concentration of lead and uranium occurred seemed to coincide with the pH at which the hydrolyzed metal ions began to precipitate. No increase in the stability of the solutions was obtained by substituting polyethylene containers for borosilicate glass. The solutions that lost strength could not be restored promptly to the original concentration by manual means, such as shaking them vigorously for several minutes.

Analytical Chemistry

Nitrate-stimulated release of naturally occurring sedimentary uranium

Groundwater uranium (U) concentrations have been measured above the U.S. EPA maximum contaminant level (30 μg/L) in many U.S. aquifers, including in areas not associated with anthropogenic contamination by milling or mining. In addition to carbonate, nitrate has been correlated to uranium groundwater concentrations in two major U.S. aquifers. However, to date, direct evidence that nitrate mobilizes naturally occurring U from aquifer sediments has not been presented. Here, we demonstrate that the influx of high-nitrate porewater through High Plains alluvial aquifer silt sediments bearing naturally occurring U(IV) can stimulate a nitrate-reducing microbial community capable of catalyzing the oxidation and mobilization of U into the porewater. Microbial reduction of nitrate yielded nitrite, a reactive intermediate, which was further demonstrated to abiotically mobilize U from the reduced alluvial aquifer sediments. These results indicate that microbial activity, specifically nitrate reduction to nitrite, is one mechanism driving U mobilization from aquifer sediments in addition to previously described bicarbonate-driven desorption from mineral surfaces, such as Fe(III) oxides.

Nebraska

Dietary bioavailability of uranium to a model freshwater invertebrate

Uranium (U) mining increases environmental exposures. Understanding how U is taken up by organisms can aid in evaluating the potential for bioaccumulation and toxicity. Although the importance of aqueous geochemical speciation is well recognized for U bioavailability after dissolved exposures, far less is known about the processes controlling U bioavailability after dietary exposures. This study characterizes the biogeochemical drivers of dietary U uptake in the freshwater snail Lymnaea stagnalis in laboratory experiments. Solids tested included benthic diatoms pre-exposed to dissolved U(VI), soils from contaminated U mine sites, and colloidal hydrous ferric oxide (HFO) synthesized in the presence of dissolved U(VI) or with U complexed by natural organic matter (NOM). Results showed that U was bioavailable from all solids. Uranium assimilation efficiency (AE), a proxy for dietary U bioavailability, varied among solids. AE was lowest for the U-contaminated soils (25 ± 17%) and highest for the U-laden diatoms (71 ± 13%). AE varied slightly among HFO preparations, suggesting modest influences of NOM and iron on U bioavailability. Increases in dietary U exposures reduced feeding rates, and the extent of feeding inhibition appeared inversely related to U bioavailability. The high U assimilation and range of bioavailability have implications for toxicity risks inferred without considering dietary uptake.

Environmental Science and Technology

Molecular-scale characterization of uranium sorption by bone apatite materials for a permeable reactive barrier demonstration

Uranium binding to bone charcoal and bone meal apatite materials was investigated using U L III -edge EXAFS spectroscopy and synchrotron source XRD measurements of laboratory batch preparations in the absence and presence of dissolved carbonate. Pelletized bone char apatite recovered from a permeable reactive barrier (PRB) at Fry Canyon, UT, was also studied. EXAFS analyses indicate that U(VI) sorption in the absence of dissolved carbonate occurred by surface complexation of U(VI) for sorbed concentrations ≤ 5500 μg U(VI)/g for all materials with the exception of crushed bone char pellets. Either a split or a disordered equatorial oxygen shell was observed, consistent with complexation of uranyl by the apatite surface. A second shell of atoms at a distance of 2.9 Å was required to fit the spectra of samples prepared in the presence of dissolved carbonate (4.8 mM total) and is interpreted as formation of ternary carbonate complexes with sorbed U(VI). A U−P distance at 3.5−3.6 Å was found for most samples under conditions where uranyl phosphate phases did not form, which is consistent with monodentate coordination of uranyl by phosphate groups in the apatite surface. At sorbed concentrations ≥ 5500 μg U(VI)/g in the absence of dissolved carbonate, formation of the uranyl phosphate solid phase, chernikovite, was observed. The presence of dissolved carbonate (4.8 mM total) suppressed the formation of chernikovite, which was not detected even with sorbed U(VI) up to 12 300 μg U(VI)/g in batch samples of bone meal, bone charcoal, and reagent-grade hydroxyapatite. EXAFS spectra of bone char samples recovered from the Fry Canyon PRB were comparable to laboratory samples in the presence of dissolved carbonate where U(VI) sorption occurred by surface complexation. Our findings demonstrate that uranium uptake by bone apatite will probably occur by surface complexation instead of precipitation of uranyl phosphate phases under the groundwater conditions found at many U-contaminated sites.

Environmental Science & Technology

Evaluating chemical extraction techniques for the determination of uranium oxidation state in reduced aquifer sediments

Extraction techniques utilizing high pH and (bi)carbonate concentrations were evaluated for their efficacy in determining the oxidation state of uranium (U) in reduced sediments collected from Rifle, CO. Differences in dissolved concentrations between oxic and anoxic extractions have been proposed as a means to quantify the U(VI) and U(IV) content of sediments. An additional step was added to anoxic extractions using a strong anion exchange resin to separate dissolved U(IV) and U(VI). X-ray spectroscopy showed that U(IV) in the sediments was present as polymerized precipitates similar to uraninite and/or less ordered U(IV), referred to as non-uraninite U(IV) species associated with biomass (NUSAB). Extractions of sediment containing both uraninite and NUSAB displayed higher dissolved uranium concentrations under oxic than anoxic conditions while extractions of sediment dominated by NUSAB resulted in identical dissolved U concentrations. Dissolved U(IV) was rapidly oxidized under anoxic conditions in all experiments. Uraninite reacted minimally under anoxic conditions but thermodynamic calculations show that its propensity to oxidize is sensitive to solution chemistry and sediment mineralogy. A universal method for quantification of U(IV) and U(VI) in sediments has not yet been developed but the chemical extractions, when combined with solid-phase characterization, have a narrow range of applicability for sediments without U(VI).

Colorado

Mobilization of radionuclides from uranium mill tailings and related waste materials in anaerobic environments

Specific extraction studies in our laboratory have shown that iron and manganese oxide- and alkaline earth sulfate minerals are important hosts of radium in uranium mill tailings. Iron- and sulfate-reducing bacteria may enhance the release of radium (and its analog barium) from uranium mill tailings, oil field pipe scale [a major technologically enhanced naturally occurring radioactive material (TENORM) waste], and jarosite (a common mineral in sulfuric acid processed-tailings). These research findings are reviewed and discussed in the context of nuclear waste forms (such as barium sulfate matrices), radioactive waste management practices, and geochemical environments in the Earth's surficial and shallow subsurface regions.

Journal of Radioanalytical and Nuclear Chemistry

Contribution of arsenic and uranium in private wells and community water systems to urinary biomarkers in US adults: The Strong Heart Study and the Multi-Ethnic Study of Atherosclerosis

Background Chronic exposure to inorganic arsenic (As) and uranium (U) in the United States (US) occurs from unregulated private wells and federally regulated community water systems (CWSs). The contribution of water to total exposure is assumed to be low when water As and U concentrations are low. Objective We examined the contribution of water As and U to urinary biomarkers in the Strong Heart Family Study (SHFS), a prospective study of American Indian communities, and the Multi-Ethnic Study of Atherosclerosis (MESA), a prospective study of racially/ethnically diverse urban U.S. communities. Methods We assigned residential zip code-level estimates in CWSs (µg/L) and private wells (90th percentile probability of As >10 µg/L) to up to 1485 and 6722 participants with dietary information and urinary biomarkers in the SHFS (2001–2003) and MESA (2000–2002; 2010–2011), respectively. Urine As was estimated as the sum of inorganic and methylated species, and urine U was total uranium. We used linear mixed-effects models to account for participant clustering and removed the effect of dietary sources via regression adjustment. Results The median (interquartile range) urine As was 5.32 (3.29, 8.53) and 6.32 (3.34, 12.48) µg/L for SHFS and MESA, respectively, and urine U was 0.037 (0.014, 0.071) and 0.007 (0.003, 0.018) µg/L. In a meta-analysis across both studies, urine As was 11% (95% CI: 3, 20%) higher and urine U was 35% (5, 73%) higher per twofold higher CWS As and U, respectively. In the SHFS, zip-code level factors such as private well and CWS As contributed 46% of variation in urine As, while in MESA, zip-code level factors, e.g., CWS As and U, contribute 30 and 49% of variation in urine As and U, respectively. Impact statement We found that water from unregulated private wells and regulated CWSs is a major contributor to urinary As and U (an estimated measure of internal dose) in both rural, American Indian populations and urban, racially/ethnically diverse populations nationwide, even at levels below the current regulatory standard. Our findings indicate that additional drinking water interventions, regulations, and policies can have a major impact on reducing total exposures to As and U, which are linked to adverse health effects even at low levels.

Journal of Exposure Science and Environmental Epid

Ground-water contamination near a uranium tailings disposal site in Colorado

Contaminants from uranium tailings disposed of at an active mill in Colorado have seeped into the shallow ground water onsite. This ground water discharges into the Arkansas River Valley through a superposed stream channel cut in the resistant sandstone ridge at the edge of a synclinal basin. In the river valley, seasonal surface-water irrigation has a significant impact on hydrodynamics. Water levels in residential wells fluctuate up to 20 ft and concentrations of uranium, molybdenum, and other contaminants also vary seasonally, with highest concentrations in the Spring, prior to irrigation, and lowest concentrations in the Fall. Results of a simple transient mixing cell model support the hypothesis that lateral ground-water inflow, and not irrigation recharge, is the source of ground-water contamination.

Colorado