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P. C. Van Metre

Publications and source records attributed to P. C. Van Metre.

At least 19 recordsLinked to original sources

Increased atmospheric deposition of mercury in reference lakes near major urban areas

Atmospheric deposition of Hg is the predominant pathway for Hg to reach sensitive ecosystems, but the importance of emissions on near-field deposition remains unclear. To better understand spatial variability in Hg deposition, mercury concentrations were analyzed in sediment cores from 12 lakes with undeveloped watersheds near to (<50 km) and remote from (>150 km) several major urban areas in the United States. Background and focusing corrected Hg fluxes and flux ratios (modern to background) in the near-urban lakes (68 ± 6.9 μg m −2 yr −1 and 9.8 ± 4.8, respectively) greatly exceed those in the remote lakes (14 ± 9.3 μg m −2 yr −1 and 3.5 ± 1.0) and the fluxes are strongly related to distance from the nearest major urban area ( r 2 = 0.87) and to population and Hg emissions within 50–100 km of the lakes. Comparison to monitored wet deposition suggests that dry deposition is a major contributor of Hg to lakes near major urban areas.

Environmental Pollution↗

Influence of coal-tar sealcoat and other carbonaceous materials on polycyclic aromatic hydrocarbon loading in an urban watershed

Carbonaceous material (CM) particles are the principal vectors transporting polycyclic aromatic hydrocarbons (PAHs) into urban waters via runoff; however, characteristics of CM particles in urban watersheds and their relative contributions to PAH contamination remain unclear. Our objectives were to identify the sources and distribution of CM particles in an urban watershed and to determine the types of CMs that were the dominant sources of PAHs in the lake and stream sediments. Samples of soils, parking lot and street dust, and streambed and lake sediment were collected from the Lake Como watershed in Fort Worth, Texas. Characteristics of CM particles determined by organic petrography and a significant correlation between PAH concentrations and organic carbon in coal tar, asphalt, and soot indicate that these three CM particle types are the major sources and carriers of PAHs in the watershed. Estimates of the distribution of PAHs in CM particles indicate that coal-tar pitch, usedinsomepavementsealcoats, isadominant source of PAHs in the watershed, and contributes as much as 99% of the PAHs in sealed parking lot dust, 92% in unsealed parking lot dust, 88% in commercial area soil, 71% in streambed sediment, and 84% in surficial lake sediment. ?? 2010 American Chemical Society.

Environmental Science & Technology↗

Coal-tar-based parking lot sealcoat: An unrecognized source of PAH to settled house dust

Despite much speculation, the principal factors controlling concentrations of polycyclic aromatic hydrocarbons (PAH) in settled house dust (SHD) have not yet been identified. In response to recent reports that dust from pavement with coaltar-based sealcoat contains extremely high concentrations of PAH, we measured PAH in SHD from 23 apartments and in dust from their associated parking lots, one-half of which had coal-tar-based sealcoat (CT). The median concentration of total PAH (T-PAH) in dust from CT parking lots (4760 ??g/g, n = 11) was 530 times higher than that from parking lots with other pavement surface types (asphalt-based sealcoat, unsealed asphalt, concrete [median 9.0 ??g/g, n = 12]). T-PAH in SHD from apartments with CT parking lots (median 129 ??g/g) was 25 times higher than that in SHD from apartments with parking lots with other pavement surface types (median 5.1 ??g/g). Presence or absence of CT on a parking lot explained 48% of the variance in log-transformed T-PAH in SHD. Urban land-use intensity near the residence also had a significant but weaker relation to T-PAH. No other variables tested, including carpeting, frequency of vacuuming, and indoor burning, were significant. ?? 2010 American Chemical Society.

Environmental Science & Technology↗

Potential contributions of asphalt and coal tar to black carbon quantification in urban dust, soils, and sediments

Measurements of black carbon (BC) using either chemical or thermal oxidation methods are generally thought to indicate the amount of char and/or soot present in a sample. In urban environments, however, asphalt and coal-tar particles worn from pavement are ubiquitous and, because of their pyrogenic origin, could contribute to measurements of BC. Here we explored the effect of the presence of asphalt and coal-tar particles on the quantification of BC in a range of urban environmental sample types, and evaluated biases in the different methods used for quantifying BC. Samples evaluated were pavement dust, residential and commercial area soils, lake sediments from a small urban watershed, and reference materials of asphalt and coal tar. Total BC was quantified using chemical treatment through acid dichromate (Cr2O7) oxidation and chemo-thermal oxidation at 375??C (CTO-375). BC species, including soot and char/charcoal, asphalt, and coal tar, were quantified with organic petrographic analysis. Comparison of results by the two oxidation methods and organic petrography indicates that both coal tar and asphalt contribute to BC quantified by Cr2O7 oxidation, and that coal tar contributes to BC quantified by CTO-375. These results are supported by treatment of asphalt and coal-tar reference samples with Cr2O7 oxidation and CTO-375. The reference asphalt is resistant to Cr2O7 oxidation but not to CTO-375, and the reference coal tar is resistant to both Cr2O7 oxidation and CTO-375. These results indicate that coal tar and/or asphalt can contribute to BC measurements in samples from urban areas using Cr2O7 oxidation or CTO-375, and caution is advised when interpreting BC measurements made with these methods. ?? 2010 Elsevier Ltd.

Geochimica et Cosmochimica Acta↗

Assessment of multiple sources of anthropogenic and natural chemical inputs to a morphologically complex basin, Lake Mead, USA

Lakes with complex morphologies and with different geologic and land-use characteristics in their sub-watersheds could have large differences in natural and anthropogenic chemical inputs to sub-basins in the lake. Lake Mead in southern Nevada and northern Arizona, USA, is one such lake. To assess variations in chemical histories from 1935 to 1998 for major sub-basins of Lake Mead, four sediment cores were taken from three different parts of the reservoir (two from Las Vegas Bay and one from the Overton Arm and Virgin Basin) and analyzed for major and trace elements, radionuclides, and organic compounds. As expected, anthropogenic contaminant inputs are greatest to Las Vegas Bay reflecting inputs from the Las Vegas urban area, although concentrations are low compared to sediment quality guidelines and to other USA lakes. One exception to this pattern was higher Hg in the Virgin Basin core. The Virgin Basin core is located in the main body of the lake (Colorado River channel) and is influenced by the hydrology of the Colorado River, which changed greatly with completion of Glen Canyon Dam upstream in 1963. Major and trace elements in the core show pronounced shifts in the early 1960s and, in many cases, gradually return to concentrations more typical of pre-1960s by the 1980s and 1990s, after the filling of Lake Powell. The Overton Arm is the sub-basin least effected by anthropogenic contaminant inputs but has a complex 137Cs profile with a series of large peaks and valleys over the middle of the core, possibly reflecting fallout from nuclear tests in the 1950s at the Nevada Test Site. The 137Cs profile suggests a much greater sedimentation rate during testing which we hypothesize results from greatly increased dust fall on the lake and Virgin and Muddy River watersheds. The severe drought in the southwestern USA during the 1950s might also have played a role in variations in sedimentation rate in all of the cores. ?? 2009.

Palaeogeography, Palaeoclimatology, Palaeoecology↗

Effects of uranium mining discharges on water quality in the Puerco River basin, Arizona and New Mexico

From 1967 until 1986, uranium mine dewatering increased dissolved gross alpha, gross beta, uranium and radium activities and dissolved selenium and molybdenum concentrations in the Puerco River as indicated by time trends, areal patterns involving distance from the mines and stream discharge. Additionally, increased dissolved uranium concentrations were identified in groundwater under the Puerco River from where mine discharges entered the river to approximately the Arizona-New Mexico State line about 65 km downstream. Total mass of uranium and gross alpha activity released to the Puerco River by mine dewatering were estimated as 560 Mg (560 × 10 6 g) and 260 Ci, respectively. In comparison, a uranium mill tailings pond spill on 16 July 1979, released an estimated 1.5 Mg of uranium and 46 Ci of gross alpha activity. Mass balance calculations for alluvial ground water indicate that most of the uranium released did not remain in solution. Sorption of uranium on sediments and uptake of uranium by plants probably removed the uranium from solution.

Arizona, New Mexico↗

Fipronil and its degradates in indoor and outdoor dust

Fipronil is a potent insecticide used for control of termites, fleas, roaches, ants, and other pests. We measured fipronil, fipronil sulfide, and desulfinyl fipronil concentrations in indoor and outdoor dust from 24 residences in Austin, Texas. At least one of these three fipronil compounds was detected in every sample. Fipronil accounted for most of the total fipronil (T-fipronil; fipronil+desulfinyl fipronil+fipronil sulfide), followed by desulfinyl fipronil and fipronil sulfide. Nineteen of 24 samples of indoor dust had T-fipronil concentrations less than 270 ??g/kg; the remaining five had concentrations from 1320 to 14,200 ??g/kg. All three of the residences with a dog on which a flea-control product containing fipronil was used were among the five residences with elevated fipronil concentrations. In outdoor dust, all concentrations of T-fipronil were less than 70??g/kg with one exception (430??g/kg). For every residence, the concentration of T-fipronil in indoor dust exceeded that in outdoor dust, and the median concentration of T-fipronil was 15 times higher indoors than outdoors.

Environmental Science & Technology↗

Enantiomer fractions of chlordane components in sediment from U.S. Geological Survey sites in lakes and rivers

Spatial, temporal, and sediment-type trends in enantiomer signatures were evaluated for cis - and trans -chlordane (CC, TC) in archived core, suspended, and surficial-sediment samples from six lake, reservoir, and river sites across the United States. The enantiomer fractions (EFs) measured in these samples are in good agreement with those reported for sediment, soil, and air samples in previous studies. The chlordane EFs were generally close to the racemic value of 0.5, with CC values ranging from 0.493 to 0.527 (usually >0.5) and TC values from 0.463 to 0.53 (usually <0.5). EF changes with core depth were detected for TC and CC in some cores, with the most non-racemic values near the top of the core. Surficial and suspended sediments generally have EF values similar to the top core layers but are often more non-racemic, indicating that enantioselective degradation is occurring before soils are eroded and deposited into bottom sediments. We hypothesize that rapid losses (desorption or degradation) from suspended sediments of the more bioavailable chlordane fraction during transport and initial deposition could explain the apparent shift to more racemic EF values in surficial and top core sediments. Near racemic CC and TC in the core profiles suggest minimal alteration of chlordane from biotic degradation, unless it is via non-enantioselective processes. EF values for the heptachlor degradate, heptachlor epoxide (HEPX), determined in surficial sediments from one location only were always non-racemic (EF ≈ 0.66), were indicative of substantial biotic processing, and followed reported EF trends.

Science of the Total Environment↗

Dual-core mass-balance approach for evaluating mercury and 210 Pb atmospheric fallout and focusing to lakes

Determining atmospheric deposition rates of mercury and other contaminants using lake sediment cores requires a quantitative understanding of sediment focusing. Here we present a novel approach that solves mass-balance equations for two cores algebraically to estimate contaminant contributions to sediment from direct atmospheric fallout and from watershed and in-lake focusing. The model is applied to excess 210 Pb and Hg in cores from Hobbs Lake, a high-altitude lake in Wyoming. Model results for excess 210 Pb are consistent with estimates of fallout and focusing factors computed using excess 210 Pb burdens in lake cores and soil cores from the watershed and model results for Hg fallout are consistent with fallout estimated using the soil-core-based 210 Pb focusing factors. The lake cores indicate small increases in mercury deposition beginning in the late 1800s and large increases after 1940, with the maximum at the tops of the cores of 16-20 ??g/m 2 year. These results suggest that global Hg emissions and possibly regional emissions in the western United States are affecting the north-central Rocky Mountains. Hg fallout estimates are generally consistent with fallout reported from an ice core from the nearby Upper Fremont Glacier, but with several notable differences. The model might not work for lakes with complex geometries and multiple sediment inputs, but for lakes with simple geometries, like Hobbs, it can provide a quantitative approach for evaluating sediment focusing and estimating contaminant fallout.

Environmental Science & Technology↗

PAHs underfoot: Contaminated dust from coal-tar sealcoated pavement is widespread in the United States

We reported in 2005 that runoff from parking lots treated with coal-tar-based sealcoat was a major source of polycyclic aromatic hydrocarbons (PAHs) to streams in Austin, Texas. Here we present new data from nine U. S. cities that show nationwide patterns in concentrations of PAHs associated with sealcoat Dust was swept from parking lots in six cities in the central and eastern U. S., where coal-tar-based sealcoat dominates use, and three cities in the western U. S., where asphalt-based sealcoat dominates use. For six central and eastern cities, median ?? PAH concentrations in dust from sealcoated and unsealcoated pavement are 2200 and 27 mg/kg, respectively. For three western cities, median ?? PAH concentrations in dust from sealcoated and unsealcoated pavement are similar and very low (2. 1 and 0. 8 mg/kg, respectively). Lakes in the central and eastern cities where pavement was sampled have bottom sediments with higher PAH concentrations than do those in the western cities relative to degree of urbanization. Bottom-sediment PAH assemblages are similar to those of sealcoated pavement dust regionally, implicating coal-tar-based sealcoat as a PAH source to the central and eastern lakes. Concentrations of benzo[a]pyrene in dust from coal-tar sealcoated pavement and adjacent soils greatly exceed generic soil screening levels, suggesting that research on human-health risk is warranted.

Environmental Science & Technology↗

Origins of sediment-associated contaminants to the Marais Vernier, the Seine Estuary, France

The Marais Vernier is the largest freshwater wetland in the Seine Estuary in northern France. It is in a heavily urbanized and industrialized region and could be affected by atmospheric deposition and by fluvial input of contaminants in water diverted from the Seine River. To evaluate contaminant histories in the wetland and the region, sediment cores were collected from two open-water ponds in the Marais Vernier: the Grand-Mare, which was connected to the Seine by a canal from 1950 to 1996, and the Petite Mare, which has a small rural watershed. Diversions from the Seine to the Grand-Mare increased sedimentation rates but mostly resulted in low contaminant concentrations and loading rates, indicating that the sediment from the Seine was predominantly brought upstream by tidal currents from the estuary and was not from the watershed. Atmospheric sources of metals dominate inputs to the Petite Mare; however, runoff of metals from vehicle-related sources in the watershed might contribute to the upward trends in concentrations of Cr, Cu, and Zn. Estimates of atmospheric deposition using the Petite Mare core are consistent with measured deposition in the region and are mixed (similar for Hg and Pb; larger for Cd, Cu, and Zn) compared with deposition estimated from sediment cores in the northeastern United States. A local source of PAHs in the watershed of the Petite Mare is indicated by higher concentrations, higher accumulation rates, and a different, more petrogenic, PAH assemblage than in the Grand-Mare. The study illustrates how diverse sources and transport pathways can affect wetlands in industrial regions and can be evaluated using sediment cores from the wetland ponds. ?? 2008 Springer Science+Business Media B.V.

Water, Air, & Soil Pollution↗

Atmospheric mercury accumulation and washoff processes on impervious urban surfaces

The deposition and transport of mercury (Hg) has been studied extensively in rural environments but is less understood in urbanized catchments, where elevated atmospheric Hg concentrations and impervious surfaces may efficiently deliver Hg to waterways in stormwater runoff. We determined the rate at which atmospheric Hg accumulates on windows, identified the importance of washoff in removing accumulated Hg, and measured atmospheric Hg concentrations to help understand the relationship between deposition and surface accumulation. The main study location was Toronto, Ontario. Similar samples were also collected from Austin, Texas for comparison of Hg accumulation between cities. Windows provided a good sampling surface because they are ubiquitous in urban environments and are easy to clean/blank allowing the assessment of contemporary Hg accumulation. Hg Accumulation rates were spatially variable ranging from 0.82 to 2.7 ng m-2 d-1 in Toronto and showed similar variability in Austin. The highest accumulation rate in Toronto was at the city center and was 5?? higher than the rural comparison site (0.58 ng m-2 d-1). The atmospheric total gaseous mercury (TGM) concentrations were less than 2?? higher between the rural and urban locations (1.7 ?? 0.3 and 2.7 ?? 1.1 ng m-3, respectively). The atmospheric particulate bound fraction (HgP), however, was more than 3?? higher between the rural and urban sites, which may have contributed to the higher urban Hg accumulation rates. Windows exposed to precipitation had 73 ?? 9% lower accumulation rates than windows sheltered from precipitation. Runoff collected from simulated rain events confirmed that most Hg accumulated on windows was easily removed and that most of the Hg in washoff was HgP. Our results indicate that the Hg flux from urban catchments will respond rapidly to changes in atmospheric concentrations due to the mobilization of the majority of the surface accumulated Hg during precipitation events. ?? 2008 Elsevier Ltd.

Atmospheric Environment↗

The chemical response of particle-associated contaminants in aquatic sediments to urbanization in New England, U.S.A.

Relations between urbanization and particle-associated contaminants in New England were evaluated using a combination of samples from sediment cores, streambed sediments, and suspended stream sediments. Concentrations of PAHs, PCBs, DDT, and seven trace metals (Cd, Cr, Cu, Hg, Ni, Pb, Zn) were correlated strongly with urbanization, with the strongest relations to percentage commercial, industrial, and transportation (CIT) land use. Average PAH and metal concentrations in the most urbanized watersheds were approximately 30 and 6 times the reference concentrations, respectively, in remote, undeveloped watersheds. One-quarter to one-half of sampling sites had concentrations of PAHs, Cu, Pb, or Zn above the probable effects concentration, a set of sediment quality guidelines for adverse effects to aquatic biota, and sediments were predicted to be toxic, on average, when CIT land use exceeded about 10%. Trends in metals in cores from urban watersheds were dominantly downward, whereas trends in PAHs in a suburban watershed were upward. A regional atmospheric-fallout gradient was indicated by as much as order-of-magnitude-greater concentrations and accumulation rates of contaminants in cores from an undeveloped reference lake in Boston compared to those from remote reference watersheds. Contaminant accumulation rates in the lakes with urbanization in their watersheds, however, were 1-3 orders of magnitude greater than those of reference lakes, which indicate the dominance of local sources and fluvial transport of contaminants to urban lakes. These analyses demonstrate the magnitude of urban contamination of aquatic systems and air sheds, and suggest that, despite reductions in contaminant emissions in urban settings, streams and lakes will decline in quality as urbanization of their watersheds takes place. ?? 2006 Elsevier B.V. All rights reserved.

Journal of Contaminant Hydrology↗

Effects of hurricanes Katrina and Rita on the chemistry of bottom sediments in Lake Pontchartrain, Louisiana, USA

The effects of Hurricanes Katrina and Rita and the subsequent unwatering of New Orleans, Louisiana, on the sediment chemistry of Lake Pontchartrain were evaluated by chemical analysis of samples of street mud and suspended and bottom sediments. The highest concentrations of urban-related elements and compounds (e.g., Pb, Zn, polycyclic aromatic hydrocarbons, and chlordane) in bottom sediments exceeded median concentrations in U.S. urban lakes and sediment-quality guidelines. The extent of the elevated concentrations was limited, however, to within a few hundred meters of the mouth of the 17th Street Canal, similar to results of historical assessments. Chemical and radionuclide analysis of pre- and post-Hurricane Rita samples indicates that remobilization of near-shore sediment by lake currents and storms is an ongoing process. The effects of Hurricanes Katrina and Rita on the sediment chemistry of Lake Pontchartrain are limited spatially and are most likely transitory.

Environmental Science & Technology↗

Trends in metals in urban and reference lake sediments across the United States, 1970 to 2001

Trends in metals concentrations in sediment cores from 35 reservoirs and lakes in urban and reference settings were analyzed to determine the effects of three decades of legislation, regulation, and changing demographics and industrial practices in the United States on concentrations of metals in the environment. Decreasing trends outnumber increasing trends for all seven metals analyzed (Cd, Cr, Cu, Pb, Hg, Ni, and Zn). The most consistent trends are for Pb and Cr: For Pb, 83% of the lakes have decreasing trends and 6% have increasing trends; for Cr, 54% of the lakes have decreasing trends and none have increasing trends. Mass accumulation rates of metals in cores, adjusted for background concentrations, decrease from the 1970s to the 1990s, with median changes ranging from -46% (Pb) to -3% (Hg and Zn). The largest decreases are from lakes in dense urban watersheds where the overall metals contamination in recently deposited sediments has decreased to one-half its 1970s median value. However, anthropogenic mass accumulation rates in dense urban lakes remain elevated over those in lakes in undeveloped watersheds, in some cases by as much as two orders of magnitude (Cr, Cu, and Zn), indicating that urban fluvial source signals can overwhelm those from regional atmospheric sources. ?? 2006 SETAC.

Environmental Toxicology and Chemistry↗

Concentrations, loads, and yields of particle-associated contaminants in urban creeks, Austin, Texas, 1999-2004

Concentrations, loads, and yields of particle-associated (hydrophobic) contaminants (PACs) in urban runoff in creeks in Austin, Texas, were characterized using an innovative approach: large-volume suspended-sediment sampling. This approach isolates suspended sediment from the water column in quantities sufficient for direct chemical analysis of PACs. During 1999-2004, samples were collected after selected rain events from each of five stream sites and Barton Springs for a study by the U.S. Geological Survey, in cooperation with the City of Austin. Sediment isolated from composited samples was analyzed for major elements, metals, organochlorine compounds, and polycyclic aromatic hydrocarbons (PAHs). In addition, at the Shoal Creek and Boggy Creek sites, individual samples for some events were analyzed to investigate within-event variation in sediment chemistry. Organochlorine compounds detected in suspended sediment included chlordane, dieldrin, DDD, DDE, DDT, and polychlorinated biphenyls (PCBs). Concentrations of PACs varied widely both within and between sites, with higher concentrations at the more urban sites and multiple nondetections at the least-urban sites. Within-site variation for metals and PAHs was smaller than between-site variation, and concentrations and yields of these and the organochlorine compounds correlated positively to the percentage of urban land use in the watershed. Loads of most PACs tested correlated significantly with suspended-sediment loads. Concentrations of most PACs correlated strongly with three measures of urban land use. Variation in suspended-sediment chemistry during runoff events was investigated at the Shoal and Boggy Creek sites. Five of the eight metals analyzed, dieldrin, chlordane, PCBs, and PAHs were detected at the highest concentrations in the first sample collected at the Shoal Creek site, a first-flush effect, but not at the Boggy Creek site. Temporal patterns in concentrations of DDT and its breakdown products varied from one event to the next. In spite of the first-flush effect in concentrations at the Shoal Creek site, most of the contaminant load was transported at peak discharge, when suspended-sediment concentration and load are maximum.

Scientific Investigations Report↗

Parking lot sealcoat: An unrecognized source of urban polycyclic aromatic hydrocarbons

Polycyclic aromatic hydrocarbons (PAHs) are a ubiquitous contaminant in urban environments. Although numerous sources of PAHs to urban runoff have been identified, their relative importance remains uncertain. We show that a previously unidentified source of urban PAHs, parking lot sealcoat, may dominate loading of PAHs to urban water bodies in the United States. Particles in runoff from parking lots with coal-tar emulsion sealcoat had mean concentrations of PAHs of 3500 mg/kg, 65 times higher than the mean concentration from unsealed asphalt and cement lots. Diagnostic ratios of individual PAHs indicating sources are similar for particles from coal-tar emulsion sealed lots and suspended sediment from four urban streams. Contaminant yields projected to the watershed scale for the four associated watersheds indicate that runoff from sealed parking lots could account for the majority of stream PAH loads.

Environmental Science & Technology↗