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At least 469 records · Page 26Linked to original sources
USGS2005

Arsenate adsorption mechanisms at the allophane: Water interface

We investigated arsenate (As(V)) reactivity and surface speciation on amorphous aluminosilicate mineral (synthetic allophane) surfaces using batch adsorption experiments, powder X-ray diffraction (XRD), and X-ray absorption spectroscopy (XAS). The adsorption isotherm experiments indicated that As(V) uptake increased with increasing [As(V)] o from 50 to 1000 μM (i.e., Langmuir type adsorption isotherm) and that the total As adsorption slightly decreased with increasing NaCl concentrations from 0.01 to 0.1 M. Arsenate adsorption was initially (0−10 h) rapid followed by a slow continuum uptake, and the adsorption processes reached the steady state after 720 h. X-ray absorption spectroscopic analyses suggest that As(V) predominantly forms bidentate binuclear surface species on aluminum octahedral structures, and these species are stable up to 11 months. Solubility calculations and powder XRD analyses indicate no evidence of crystalline Al−As(V) precipitates in the experimental systems. Overall, macroscopic and spectroscopic evidence suggest that the As(V) adsorption mechanisms at the allophane−water interface are attributable to ligand exchange reactions between As(V) and surface-coordinated water molecules and hydroxyl and silicate ions. The research findings imply that dissolved tetrahedral oxyanions (e.g., H 2 PO 4 2 - and H 2 AsO 4 2 - ) are readily retained on amorphous aluminosilicate minerals in aquifer and soils at near neutral pH. The inner-sphere adsorption mechanisms might be important in controlling dissolved arsenate and phosphate in amorphous aluminosilicate-rich low-temperature geochemical environments.

Environmental Science & Technology↗
USGS2005

Climate dependency of tree growth suppressed by acid deposition effects on soils in Northwest Russia

Increased tree growth in temperate and boreal forests has been proposed as a direct consequence of a warming climate. Acid deposition effects on nutrient availability may influence the climate dependency of tree growth, however. This study presents an analysis of archived soil samples that has enabled changes in soil chemistry to be tracked with patterns of tree growth through the 20th century. Soil samples collected in 1926, 1964, and 2001, near St. Petersburg, Russia, showed that acid deposition was likely to have decreased root-available concentrations of Ca (an essential element) and increased root-available concentrations of Al (an inhibitor of Ca uptake). These soil changes coincided with decreased diameter growth and a suppression of climate-tree growth relationships in Norway spruce. Expected increases in tree growth from climate warming may be limited by decreased soil fertility in regions of northern and eastern Europe, and eastern North America, where Ca availability has been reduced by acidic deposition. ?? 2005 American Chemical Society.

Environmental Science & Technology↗
USGS2005

Role for Fe(III) minerals in nitrate-dependent microbial U(IV) oxidation

Microbiological reduction of soluble U(VI) to insoluble U(IV) is a means of preventing the migration of that element in groundwater, but the presence of nitrate in U(IV)-containing sediments leads to U(IV) oxidation and remobilizaton. Nitrite or iron(III) oxyhydroxides may oxidize U(IV) under nitrate-reducing conditions, and we determined the rate and extent of U(IV) oxidation by these compounds. Fe(III) oxidized U(IV) at a greater rate than nitrite (130 and 10 μM U(IV)/day, respectively). In aquifer sediments, Fe(III) may be produced during microbial nitrate reduction by oxidation of Fe(II) with nitrite, or by enzymatic Fe(II) oxidation coupled to nitrate reduction. To determine which of these mechanisms was dominant, we isolated a nitrate-dependent acetate- and Fe(II)-oxidizing bacterium from a U(VI)- and nitrate-contaminated aquifer. This organism oxidized U(IV) at a greater rate and to a greater extent under acetate-oxidizing (where nitrite accumulated to 50 mM) than under Fe(II)-oxidizing conditions. We show that the observed differences in rate and extent of U(IV) oxidation are due to mineralogical differences between Fe(III) produced by reaction of Fe(II) with nitrite (amorphous) and Fe(III) produced enzymatically (goethite or lepidocrocite). Our results suggest the mineralogy and surface area of Fe(III) minerals produced under nitrate-reducing conditions affect the rate and extent of U(IV) oxidation. These results may be useful for predicting the stability of U(IV) in aquifers.

Environmental Science & Technology↗
USGS2005

Why is metal bioaccumulation so variable? Biodynamics as a unifying concept

Ecological risks from metal contaminants are difficult to document because responses differ among species, threats differ among metals, and environmental influences are complex. Unifying concepts are needed to better tie together such complexities. Here we suggest that a biologically based conceptualization, the biodynamic model, provides the necessary unification for a key aspect in risk: metal bioaccumulation (internal exposure). The model is mechanistically based, but empirically considers geochemical influences, biological differences, and differences among metals. Forecasts from the model agree closely with observations from nature, validating its basic assumptions. The biodynamic metal bioaccumulation model combines targeted, high-quality geochemical analyses from a site of interest with parametrization of key physiological constants for a species from that site. The physiological parameters include metal influx rates from water, influx rates from food, rate constants of loss, and growth rates (when high). We compiled results from 15 publications that forecast species-specific bioaccumulation, and compare the forecasts to bioaccumulation data from the field. These data consider concentrations that cover 7 orders of magnitude. They include 7 metals and 14 species of animals from 3 phyla and 11 marine, estuarine, and freshwater environments. The coefficient of determination ( R 2 ) between forecasts and independently observed bioaccumulation from the field was 0.98. Most forecasts agreed with observations within 2-fold. The agreement suggests that the basic assumptions of the biodynamic model are tenable. A unified explanation of metal bioaccumulation sets the stage for a realistic understanding of toxicity and ecological effects of metals in nature.

Environmental Science & Technology↗
USGS2005

Loosely bound oxytetracycline in riverine sediments from two tributaries of the Chesapeake Bay

The fate of antibiotics that bind to riverine sediment is not well understood. A solution used in geochemical extraction schemes to determine loosely bound species in sediments, 1 M MgCl 2 (pH 8), was chosen to determine loosely bound, and potentially bioavailable, tetracycline antibiotics (TCs), including oxytetracycline (5-OH tetracycline) (OTC) in sediment samples from two rivers on the eastern shore of the Chesapeake Bay. Bottom sediments were collected at sites upstream from, at, and downstream from municipal sewage-treatment plants (STPs) situated on two natural waterways, Yellow Bank Stream, MD, and the Pocomoke River, MD. Concentrations of easily desorbed OTC ranged from 0.6 to approximately 1.2 μg g -1 dry wt sediment in Yellow Bank Stream and from 0.7 to approximately 3.3 μg g -1 dry wt sediment in the Pocomoke River. Concentrations of easily desorbable OTC were generally smaller in sediment upstream than in sediment downstream from the STP in the Pocomoke River. STPs and poultry manure are both potential sources of OTC to these streams. OTC that is loosely bound to sediment is subject to desorption. Other researchers have found desorbed TCs to be biologically active compounds.

Chesapeake Bay↗
USGS2005

Speciation of mercury and mode of transport from placer gold mine tailings

Historic placer gold mining in the Clear Creek tributary to the Sacramento River (Redding, CA) has highly impacted the hydrology and ecology of an important salmonid spawning stream. Restoration of the watershed utilized dredge tailings contaminated with mercury (Hg) introduced during gold mining, posing the possibility of persistent Hg release to the surrounding environment, including the San Francisco Bay Delta. Column experiments have been performed to evaluate the extent of Hg transport under chemical conditions potentially similar to those in river restoration projects utilizing dredge tailings such as at Clear Creek. Physicochemical perturbations, in the form of shifts in column influent ionic strength and the presence of a low molecular weight organic acid, were applied to coarse and fine sand placer tailings containing 109-194 and 69-90 ng of Hg/g, respectively. Significant concentrations of mercury, up to 16 ??g/L, leach from these sediments in dissolved and particle-associated forms. Sequential chemical extractions (SCE) of these tailings indicate that elemental Hg initially introduced during gold mining has been transformed to readily soluble species, such as mercury oxides and chlorides (3-4%), intermediately extractable phases that likely include (in)organic sorption complexes and amalgams (75-87%), and fractions of highly insoluble forms such as mercury sulfides (6-20%; e.g., cinnabar and metacinnabar). Extended X-ray absorption fine structure (EXAFS) spectroscopic analysis of colloids obtained from column effluent identified cinnabar particles as the dominant mobile mercury-bearing phase. The fraction of intermediately extractable Hg phases also likely includes mobile colloids to which Hg is adsorbed. ?? 2005 American Chemical Society.

Environmental Science & Technology↗
USGS2005

Vapor-phase exchange of perchloroethene between soil and plants

Tree core concentrations of tetrachloroethylene (perchloroethene, PCE) at the Riverfront Superfund Site in New Haven, MO, were found to mimic the profile of soil phase concentrations. The observed soil-tree core relationship was stronger than that of groundwater PCE to tree core concentrations at the same site. Earlier research has shown a direct, linear relationship between tree core and groundwater concentrations of chlorinated solvents and other organics. Laboratory-scale experiments were performed to elucidate this phenomenon, including determining partitioning coefficients of PCE between plant tissues and air and between plant tissues and water, measured to be 8.1 and 49 L/kg, respectively. The direct relationship of soil to tree core PCE concentrations was hypothesized to be caused by diffusion between tree roots and the soil vapor phase in the subsurface. The central findings of this research are discovering the importance of subsurface vapor-phase transfer for VOCs and uncovering a direct relationship between soil vapor-phase chlorinated solvents and uptake rates that impact contaminant translocation from the subsurface and transfer into the atmosphere. ?? 2005 American Chemical Society.

Environmental Science & Technology↗
USGS2004

Stable metal isotopes reveal copper accumulation and loss dynamics in the freshwater bivalve Corbucula

Characterization of uptake and loss dynamics is critical to understanding risks associated with contaminant exposure in aquatic animals. Dynamics are especially important in addressing questions such as why coexisting species in nature accumulate different levels of a contaminant. Here we manipulated copper (Cu) stable isotopic ratios (as an alternative to radioisotopes) to describe for the first time Cu dynamics in a freshwater invertebrate, the bivalve Corbicula fluminea . In the laboratory, Corbicula uptake and loss rate constants were determined from an environmentally realistic waterborne exposure to 65 Cu (5.7 μg L - 1 ). That is, we spiked deionized water with Cu that was 99.4% 65 Cu. Net tracer uptake was detectable after 1 day and strongly evident after 4 days. Thus, short-term exposures necessary to determine uptake dynamics are feasible with stable isotopes of Cu. In Corbicula , 65 Cu depuration was biphasic. An unusually low rate constant of loss (0.0038 d - 1 ) characterized the slow component of efflux, explaining why Corbicula strongly accumulates copper in nature. We incorporated our estimates of rate constants for dissolved 65 Cu uptake and physiological efflux into a bioaccumulation model and showed that dietary exposure to Cu is likely an important bioaccumulation pathway for Corbicula .

Environmental Science & Technology↗
USGS2004

Methyl tert-butyl ether occurrence and related factors in public and private wells in southeast New Hampshire

The occurrence of methyl tert -butyl ether (MTBE) in water from public wells in New Hampshire has increased steadily over the past several years. Using a laboratory reporting level of 0.2 μg/L, 40% of samples from public wells and 21% from private wells in southeast New Hampshire have measurable concentrations of MTBE. The rate of occurrence of MTBE varied significantly for public wells by establishment type; for example, 63% of public wells serving residential properties have MTBE concentrations above 0.2 μg/L, whereas lower rates were found for schools (21%). MTBE concentrations correlate strongly with urban factors, such as population density. Surprisingly, MTBE was correlated positively with well depth for public supply wells. Well depth is inversely related to yield in New Hampshire bedrock wells, which may mean that there is less opportunity for dilution of MTBE captured by deep wells. Another possibility is that the source(s) of water to low-yield wells may be dominated by leakage from potentially contaminated shallow groundwater through near-surface fractures or along the well casing. These wells may also have relatively large contributing areas (due to low recharge at the bedrock surface) and therefore have a greater chance of intersecting MTBE sources. This finding is significant because deep bedrock wells are often considered to be less vulnerable to contamination than shallow wells, and in southeast New Hampshire, wells are being drilled deeper in search of increased supply.

New Hampshire↗
USGS2004

Effects of sediment characteristics on the toxicity of chromium(III) and chromium(VI) to the amphipod, Hyalella azteca

We evaluated the influence of sediment characteristics, acid-volatile sulfide (AVS) and organic matter (OM), on the toxicity of chromium (Cr) in freshwater sediments. We conducted chronic (28-42-d) toxicity tests with the amphipod Hyalella azteca exposed to Cr(VI) and Cr(III) in water and in spiked sediments. Waterborne Cr(VI) caused reduced survival of amphipods with a median lethal concentration (LC50) of 40 ??g/L. Cr(VI) spiked into test sediments with differing levels of AVS resulted in graded decreases in AVS and sediment OM. Only Cr(VI)-spiked sediments with low AVS concentrations (<1 ??mol/g) caused significant amphipod mortality. Waterborne Cr(III) concentrations near solubility limits caused decreased survival of amphipods at pH 7 and pH 8 but not at pH 6. Sediments spiked with high levels of Cr(III) did not affect amphipod survival but had minor effects on growth and inconsistent effects on reproduction. Pore waters of some Cr(III)-spiked sediments contained measurable concentrations of Cr(VI), but observed toxic effects did not correspond closely to Cr concentrations in sediment or pore waters. Our results indicate that risks of Cr toxicity are low in freshwater sediments containing substantial concentrations of AVS.

Environmental Science & Technology↗
USGS2004

Bioenergetics-based modeling of individual PCB congeners in nestling tree swallows from two contaminated sites on the Upper Hudson River, New York

A bioenergetics-based model was used to simulate the accumulation of total PCBs and 20 PCB congeners by nestling tree swallows at two contaminated sites on the Upper Hudson River, New York. PCB concentrations in birds were calculated as the sum of inherited residues and those acquired through consumption of contaminated insects. Close agreement between simulations and measured residues in 5-, 10-, and 15-day-old nestlings was obtained when PCB concentrations in the diet were set equal to those in food boli taken from adult birds. These simulations were further optimized by fitting the value of a dietary assimilation efficiency constant. Fitted constants for both sites were similar and averaged about 0.7. An evaluation of model performance for individual congeners provided no evidence of metabolic biotransformation. The results of this study are consistent with a companion effort in which principal components analysis was used to compare PCB congener patterns in insects and in tree swallow eggs, nestlings, and adults. Together, these studies establish a quantitative linkage between nestling tree swallows and the insects that they consume and provide strong support for the use of nestling swallows as a biomonitoring species for exposure assessment.

Environmental Science & Technology↗
USGS2004

Accumulation of PCB congeners in nestling tree swallows ( Tachycineta bicolor ) on the Hudson River, New York

Tree swallows (Tachycineta bicolor) were used as a sentinel species to monitor the contamination and bioavailability of polychlorinated biphenyls (PCBs) in the Hudson River watershed. Several tree swallow nest box colonies around and downstream from Hudson Falls, NY, were studied. Tree swallow eggs, adults, and 5-, 10-, and 15-day-old nestlings were collected and analyzed for 103 PCB congeners. Emergent insects collected by net (primarily Odonata) or as a food bolus (primarily Diptera) taken from the mouths of adult tree swallows returning to the nest were analyzed in the same manner. Total PCB concentrations (wet weight) in eggs from two contaminated sites ranged from 9000 to 25 000 ng/g and accumulated to 32 000 and 96 000 ng/g in 15-day-old nestling at two contaminated sites. The congener patterns of PCBs in eggs, nestlings, and adults were compared to those found in emergent insects (Odonata and Diptera) using principal components analysis. The PCB patterns of the biota differed from that of Aroclor technical mixtures. PCB patterns in adult tree swallows were similar to those in eggs, while the patterns in dietary insects were similar to nestling tree swallows. Uptake rate constants were determined for tree swallow nestlings and compared between the two contaminated sites. The estimated PCB congener uptake rate constants were 0.008-0.02 d-1 based on uptake in nestlings until day 15 post-hatch. The rate constants were comparable between the two study areas and may be used to predict nestling contamination at other locations. Our studies confirm the utility of nestling tree swallows to evaluate localized PCB contamination.

Environmental Science & Technology↗
USGS2004

Transport of Cryptosporidium oocysts in porous media: Role of straining and physicochemical filtration

The transport and filtration behavior of Cryptosporidium parvum oocysts in columns packed with quartz sand was systematically examined under repulsive electrostatic conditions. An increase in solution ionic strength resulted in greater oocyst deposition rates despite theoretical predictions of a significant electrostatic energy barrier to deposition. Relatively high deposition rates obtained with both oocysts and polystyrene latex particles of comparable size at low ionic strength (1 mM) suggest that a physical mechanism may play a key role in oocyst removal. Supporting experiments conducted with latex particles of varying sizes, under very low ionic strength conditions where physicochemical filtration is negligible, clearly indicated that physical straining is an important capture mechanism. The results of this study indicate that irregularity of sand grain shape (verified by SEM imaging) contributes considerably to the straining potential of the porous medium. Hence, both straining and physicochemical filtration are expected to control the removal of C. parvum oocysts in settings typical of riverbank filtration, soil infiltration, and slow sand filtration. Because classic colloid filtration theory does not account for removal by straining, these observations have important implications with respect to predictions of oocyst transport.

Environmental Science & Technology↗
USGS2004

Contaminant trends in reservoir sediment cores as records of influent stream quality

When reconstructing water-quality histories from lake and reservoir cores, it is sometimes assumed that the chemical signatures in the cores reflect historical water quality in the influent streams. To investigate this assumption, concentrations of metals, PAHs, and organochlorine compounds in sediment cores were compared to those associated with an influent-stream suspended sediment for three reservoirs in Fort Worth, TX, and two reservoirs in Boston, MA, U.S.A., and interpreted in light of land-use and regulation histories. In evaluating relations between suspended sediments and cores, three levels of preservation were indicated: (1) influent concentrations and historical trends are preserved in cores (metals at all sites; some organic contaminants at some sites); (2) some loss occurs during transport and initial deposition but relative historical trends are preserved in cores (some organic contaminants at some sites); and (3) neither stream concentrations nor relative historical trends are preserved (dieldrin and p,p???-DDT). The degree of preservation of influent concentration histories varied between lakes, particularly for PAHs. The results support the use of sediment cores to infer streamwater-quality histories for many contaminants but indicate that reservoir-bottom sediment samples might underestimate concentrations of organic contaminants in some streams.

Environmental Science & Technology↗
USGS2004

Effects of particulate carbonaceous matter on the bioavailability of benzo[a]pyrene and 2,2‘,5,5‘-tetrachlorobiphenyl to the clam, Macoma balthica

We investigated the bioavailability via diet of spiked benzo[ a ]pyrene (BaP) and 2,2&lsquo;,5,5&lsquo;-tetrachlorobiphenyl (PCB-52) from different carbonaceous (non-carbonate, carbon containing) particle types to clams ( Macoma balthica ) collected from San Francisco Bay. Our results reveal significant differences in absorption efficiency between compounds and among carbonaceous particle types. Absorption efficiency for PCB-52 was always greater than that for BaP bound to a given particle type. Among particles, absorption efficiency was highest from wood and diatoms and lowest from activated carbon. Large differences in absorption efficiency could not be simply explained by comparatively small differences in the particles' total organic carbon content. BaP and PCB-52 bound to activated carbon exhibited less than 2% absorption efficiency and were up to 60 times less available to clams than the same contaminants associated with other types of carbonaceous matter. These results suggest that variations in the amount and type of sediment particulate carbonaceous matter, whether naturally occurring or added as an amendment, will have a strong influence on the bioavailability of hydrophobic organic contaminants. This has important implications for environmental risk assessment, sediment management, and development of novel remediation techniques.

Environmental Science & Technology↗
USGS2004

Zinc adsorption effects on arsenite oxidation kinetics at the birnessite-water interface

Arsenite is more toxic and mobile than As(V) in soil and sediment environments, and thus it is advantageous to explore factors that enhance oxidation of As(III) to As(V). Previous studies showed that manganese oxides, such as birnessite (??-MnO2), directly oxidized As(III). However, these studies did not explore the role that cation adsorption has on As(III) oxidation. Accordingly, the effects of adsorbed and nonadsorbed Zn on arsenite (As(III)) oxidation kinetics at the birnessite-water interface were investigated using batch adsorption experiments (0.1 g L-1; pH 4.5 and 6.0; I = 0.01 M NaCl). Divalent Zn adsorption on synthetic ??-MnO 2 in the absence of As(III) increased with increasing pH and caused positive shifts in electrophoretic mobility values at pH 4-6, indirectly suggesting inner-sphere Zn adsorption mechanisms. Arsenite was readily oxidized on birnessite in the absence of Zn. The initial As(III) oxidation rate constant decreased with increasing pH from 4.5 to 6.0 and initial As(III) concentrations from 100 to 300 ??M. Similar pH and initial As(III) concentration effects were observed in systems when Zn was present (i.e., presorbed Zn prior to As(III) addition and simultaneously added Zn-As(III) systems), but As(III) oxidation reactions were suppressed compared to the respective control systems. The suppression was more pronounced when Zn was presorbed on the ??-MnO 2 surfaces as opposed to added simultaneously with As(III). This study provides further understanding of As(III) oxidation reactions on manganese oxide surfaces under environmentally applicable conditions where metals compete for reactive sites.

Environmental Science & Technology↗
USGS2004

Are brook trout streams in Western Virginia and Shenandoah National Park recovering from acidification?

Streamwater composition data obtained through periodic sampling of streams that support brook trout ( Salvelinus fontinalis ) in the mountains of western Virginia were examined for evidence of recovery from acidification during the 1988−2001 period. Measurements of sulfate deposition in precipitation indicate that sulfate deposition in the region declined approximately 40% between 1985 and 2000. While no significant regional trends in acid−base constituents were observed for the set ( n = 65) of western Virginia study streams, significant regional trends were observed for a subset ( n = 14) of streams in Shenandoah National Park (SNP). For the subset of SNP streams, the median increase in acid-neutralizing capacity (ANC) was 0.168 μequiv L -1 year -1 and the median decrease in sulfate concentration was −0.229 μequiv L -1 year -1 . Although these trends are consistent with recovery from acidification, the degree of apparent recovery is small compared to estimates of historic acidification in SNP streams and much less than observed in other, more northern regions in the United States. Correlation between sulfate concentration trends and current sulfate concentrations in streamwater suggests that recovery from stream acidification in the western Virginia region is determined by sulfur retention processes in watershed soils. A transient increase in nitrate concentrations that occurred among some western Virginia streams following forest defoliation by the gypsy moth ( Lymantria dispar ) complicates interpretation of the observed patterns of change in acid−base status.

Virginia↗
USGS2004

Food web pathway determines how selenium affects aquatic ecosystems: A San francisco Bay case study

Chemical contaminants disrupt ecosystems, but specific effects may be under-appreciated when poorly known processes such as uptake mechanisms, uptake via diet, food preferences, and food web dynamics are influential. Here we show that a combination of food web structure and the physiology of trace element accumulation explain why some species in San Francisco Bay are threatened by a relatively low level of selenium contamination and some are not. Bivalves and crustacean zooplankton form the base of two dominant food webs in estuaries. The dominant bivalve Potamocorbula amurensis has a 10-fold slower rate constant of loss for selenium than do common crustaceans such as copepods and the mysid Neomysis mercedis (rate constant of loss, k e = 0.025, 0.155, and 0.25 d -1 , respectively). The result is much higher selenium concentrations in the bivalve than in the crustaceans. Stable isotope analyses show that this difference is propagated up the respective food webs in San Francisco Bay. Several predators of bivalves have tissue concentrations of selenium that exceed thresholds thought to be associated with teratogenesis or reproductive failure (liver Se >15 μg g - 1 dry weight). Deformities typical of selenium-induced teratogenesis were observed in one of these species. Concentrations of selenium in tissues of predators of zooplankton are less than the thresholds. Basic physiological and ecological processes can drive wide differences in exposure and effects among species, but such processes are rarely considered in traditional evaluations of contaminant impacts.

California↗