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Mercury Cycling in an Urbanized Watershed: The Influence of Wind Distribution and Regional Subwatershed Geometry in Central Indiana, USA Texte intégral
2011
Hatcher, Carrie Lynne | Filippelli, Gabriel Michael
The global cycle of mercury (Hg) is reasonably well-understood, as are some of the natural and anthropogenic sources of Hg to the atmosphere. Less well understood are the regional and local characteristics of Hg deposition and subsequent watershed-scale transport, important parameters for assessing human risk to various avenues of Hg exposure. This study employed a two-part strategy for understanding coupled deposition and transport processes in central Indiana (USA), including Indianapolis, a typical large city with multiple coal-fired electric utilities and other Hg emission sources. A spatial analysis of Hg concentrations in surface soils revealed elevated Hg proximal to many of the large emission sources, with a distribution aligned along a southwest-northeast axis corresponding to the mean wind direction in this region. This soil distribution suggests some local depositional impact from local utilities, with wind modification affecting the regional pattern. Post-depositional transport of Hg was assessed using a series of streambank sampling arrays as the White River and various tributaries travelled through the urban core of Indianapolis. Streambank sediments had peak Hg concentrations in the urban core, where several local sources are present and where a number of subwatersheds join the main trunk of the White River, suggesting local emission and/or rapid Hg transport from urban subwatersheds due to their relatively high proportion of impervious surfaces. High Hg values persist in White River sediments into rural areas tens of kilometers south of Indianapolis, raising concerns for anglers collecting fish in this apparently “pristine” environment.
Afficher plus [+] Moins [-]Phosphorus Mass Balance and Internal Load in an Impacted Subtropical Isolated Wetland Texte intégral
2011
Bhadha, Jehangir H. | Jawitz, James W. | Min, Joong-Hyuk
Internal loading is a critical component of the phosphorus (P) budget of aquatic systems that can control trophic conditions. While diffusion across the soil–water interface is generally considered the dominant process controlling P load to the water column, advection due to water table fluctuations can also be significant. Our objective was to evaluate the role of diffusive and advective fluxes in relation to the total P (TP) loads entering and exiting an impacted wetland in the Lake Okeechobee drainage basin. The average diffusive flux of TP was 0.32 ± 0.14 mg m−2 day−1 and occurred for 240 days out of 314, while advective flux was 1.31 ± 4.03 mg m−2 day−1 and occurred for only 57 days. Phosphorus load to the wetland via internal modes was estimated to be 2.3 and 4.0 g day−1 from diffusion and advection respectively, accounting for 18% of the total P input, while overland flow (51%) was the major input pathway to the wetland. Ditch flow and groundwater outflow accounted for 49% (18.0 g day−1) and 14% (5.0 g day−1) of the total P output, respectively. This study shows the importance of advective flux in addition to diffusive flux and that the former should not be neglected when estimating internal P load of transiently flooded isolated wetlands. The monthly P budget-based retention and release patterns were consistent with previous findings, showing that intermittent flooding and drying cycling significantly reduces the P retention capacity of a wetland.
Afficher plus [+] Moins [-]Solubility and Fractionation of Different Metals in Fly Ash of Powder River Basin Coal Texte intégral
2011
Bhattacharyya, Pradip | Reddy, Jothi | Attili, Viswatej
Coal is one of the major sources of fuel for electricity production and will continue to be used for many more decades. Thus, it is important to study the effects of disposal of coal burning byproducts including fly ash into the environment. In this study, the solubility of cations and anions from the fly ash in water is discussed. Also, the fractionation of different metals from fly ash in water is studied to understand which fraction of the metals would likely be mobilized. The results from these studies suggested that the metals in the fly ash are bound mostly to carbonate, organic, and residual fractions. Also, when water solubility data are modeled with a geochemical model (Visual MINTEQ), the saturation index predictions suggested that brucite (Mg(OH)2) and calcite (CaCO3) could potentially precipitate and mineralize the atmospheric CO2. Such mineralization process could potentially reduce the leaching of toxic metals from fly ash. Results from this study will be helpful in understanding the fate of different metals from fly ash land disposal environments.
Afficher plus [+] Moins [-]Occurrence of Azoxystrobin, Propiconazole, and Selected Other Fungicides in US Streams, 2005–2006 Texte intégral
2011
Battaglin, William A. | Sandstrom, Mark W. | Kuivila, Kathryn M. | Kolpin, Dana W. | Meyer, Michael T.
Fungicides are used to prevent foliar diseases on a wide range of vegetable, field, fruit, and ornamental crops. They are generally more effective as protective rather than curative treatments, and hence tend to be applied before infections take place. Less than 1% of US soybeans were treated with a fungicide in 2002 but by 2006, 4% were treated. Like other pesticides, fungicides can move-off of fields after application and subsequently contaminate surface water, groundwater, and associated sediments. Due to the constant pressure from fungal diseases such as the recent Asian soybean rust outbreak, and the always-present desire to increase crop yields, there is the potential for a significant increase in the amount of fungicides used on US farms. Increased fungicide use could lead to increased environmental concentrations of these compounds. This study documents the occurrence of fungicides in select US streams soon after the first documentation of soybean rust in the US and prior to the corresponding increase in fungicide use to treat this problem. Water samples were collected from 29 streams in 13 states in 2005 and/or 2006, and analyzed for 12 target fungicides. Nine of the 12 fungicides were detected in at least one stream sample and at least one fungicide was detected in 20 of 29 streams. At least one fungicide was detected in 56% of the 103 samples, as many as five fungicides were detected in an individual sample, and mixtures of fungicides were common. Azoxystrobin was detected most frequently (45% of 103 samples) followed by metalaxyl (27%), propiconazole (17%), myclobutanil (9%), and tebuconazole (6%). Fungicide detections ranged from 0.002 to 1.15 μg/L. There was indication of a seasonal pattern to fungicide occurrence, with detections more common and concentrations higher in late summer and early fall than in spring. At a few sites, fungicides were detected in all samples collected suggesting the potential for season-long occurrence in some streams. Fungicide occurrence appears to be related to fungicide use in the associated drainage basins; however, current use information is generally lacking and more detailed occurrence data are needed to accurately quantify such a relation. Maximum concentrations of fungicides were typically one or more orders of magnitude less than current toxicity estimates for freshwater aquatic organisms or humans; however, gaps in current toxicological understandings of the effects of fungicides in the environment limit these interpretations.
Afficher plus [+] Moins [-]Comparison of Relationships Between pH, Dissolved Oxygen and Chlorophyll a for Aquaculture and Non-aquaculture Waters Texte intégral
2011
Zang, Changjuan | Huang, Suiliang | Wu, Min | Du, Shenglan | Scholz, Miklas | Gao, Feng | Lin, Chao | Guo, Yong | Dong, Yu
The relationships between pH, dissolved oxygen (DO) and chlorophyll a in aquaculture and non-aquaculture waters are assessed in this paper. The research includes the evaluation of field and experimental studies at the Panjiakou Reservoir (between Aug and Oct 2009) and the review of international data covering two decades. The results indicated that typical eutrophic non-aquaculture water had mean concentrations of chlorophyll a of higher than 10 μg L−1, and significant positive correlations were found between pH, DO and chlorophyll a. When the mean concentration of chlorophyll a was less than 10 μg L−1, no correlation was found between DO and chlorophyll a for waters with a high exchange rate or heavily organically polluted natural waters. Diurnal variations were found for both pH and DO. A corresponding significant positive correlation was found between both water quality parameters. In general, when the mean concentration of chlorophyll a was less than 10 μg L−1 within aquaculture waters of low exchange rate, only a weak or no correlation at all was found between pH, DO and chlorophyll a during summer and autumn. On the other hand, a significant positive correlation between pH and chlorophyll a and a significant positive correlation or no correlation between DO and chlorophyll a were found for aquaculture waters with a high exchange rate during summer and autumn. Strong diurnal variations for both pH and DO were identified. A significant positive linear correlation between pH and DO was found for field enclosure experiments.
Afficher plus [+] Moins [-]Non-destructive Analysis of Oil-Contaminated Soil Core Samples by X-ray Computed Tomography and Low-Field Nuclear Magnetic Resonance Relaxometry: a Case Study Texte intégral
2011
Nakashima, Yoshito | Mitsuhata, Yuji | Nishiwaki, Junko | Kawabe, Yoshishige | Utsuzawa, Shin | Jinguuji, Motoharu
Non-destructive measurements of contaminated soil core samples are desirable prior to destructive measurements because they allow obtaining gross information from the core samples without touching harmful chemical species. Medical X-ray computed tomography (CT) and time-domain low-field nuclear magnetic resonance (NMR) relaxometry were applied to non-destructive measurements of sandy soil core samples from a real site contaminated with heavy oil. The medical CT visualized the spatial distribution of the bulk density averaged over the voxel of 0.31 × 0.31 × 2 mm³. The obtained CT images clearly showed an increase in the bulk density with increasing depth. Coupled analysis with in situ time-domain reflectometry logging suggests that this increase is derived from an increase in the water volume fraction of soils with depth (i.e., unsaturated to saturated transition). This was confirmed by supplementary analysis using high-resolution micro-focus X-ray CT at a resolution of ∼10 μm, which directly imaged the increase in pore water with depth. NMR transverse relaxation waveforms of protons were acquired non-destructively at 2.7 MHz by the Carr-Purcell-Meiboom-Gill (CPMG) pulse sequence. The nature of viscous petroleum molecules having short transverse relaxation times (T2) compared to water molecules enabled us to distinguish the water-saturated portion from the oil-contaminated portion in the core sample using an M ₀-T2 plot, where M ₀ is the initial amplitude of the CPMG signal. The present study demonstrates that non-destructive core measurements by medical X-ray CT and low-field NMR provide information on the groundwater saturation level and oil-contaminated intervals, which is useful for constructing an adequate plan for subsequent destructive laboratory measurements of cores.
Afficher plus [+] Moins [-]Polycyclic Aromatic Hydrocarbons in Soils from European High Mountain Areas Texte intégral
2011
Quiroz, Roberto | Grimalt, Joan O. | Fernández, Pilar | Camarero, Lluis | Catalan, Jordi | Stuchlik, Evzen | Thies, Hansjoerg | Nickus, Ulrike
Polycyclic aromatic hydrocarbons (PAHs) were analyzed in 70 soils distributed in mountain areas such as Montseny (300–1,700 m), Pyrenees (1,500–2,900 m), Alps (1,100–2,500 m), and Tatras (1,400–1,960 m). Average total PAH concentrations, excluding retene and perylene, were about 400 ng/g in the Pyrenees and 1,300–1,600 ng/g in the other mountain ranges. No correlations between PAH concentrations and total organic carbon were observed. Retene was the major PAH in the Pyrenean soils of lower altitude. No altitudinal dependence was found between soil PAH concentrations and elevation for the whole dataset. However, in the Tatra soils a statistically significant correlation with altitude was observed involving higher concentrations at higher altitude. This correlation was due to the statistically significant altitudinal dependence of the more volatile PAHs. Another observed altitudinal trend concerned the benz[a]anthracene/(benz[a]anthracene + chrysene + triphenylene) and the benzo[a]pyrene/(benzo[a]pyrene + benzo[e]pyrene) ratios that exhibited a decrease in the more chemically labile compounds, benz[a]anthracene and benzo[a]pyrene, respectively, in the soils located at higher altitude. This observation is consistent with the expected higher photooxidation at higher mountain altitude.
Afficher plus [+] Moins [-]Smooth Brome (Bromus inermis Leyss) and Soil Chemical Response to Concrete Grinding Residue Application Texte intégral
2011
DeSutter, Tom | Goosen-Alix, Patricia | Prunty, Lyle | White, Paul, Jr | Casey, Frank
Concrete grinding residue (CGR) is a by-product created by concrete pavement maintenance operations. The application of CGR to roadside soils is not consistently regulated by state agencies across the USA, which is partially due to the lack of science-based information on its impacts to soils and plants. The objectives of this research were to determine the impact of CGR additions to soil on both smooth brome (Bromus inermis L.) biomass and plant and soil chemical parameters. In a greenhouse study, two soils were treated with two CGR by-products at 8% and 25% by weight. Shoot biomass was significantly influenced by the main effects (Soil, CGR, and Rate) and by all two-way interactions, but not consistently positively or negatively correlated. Trace metal concentrations in the shoot biomass were variable, but 68% of these metals had the same concentration or lower in the 25% CGR treatments compared with the controls. Soil pH and electrical conductivity were significantly influenced by the main effects and two-way interactions of Soil × Rate and CGR × Rate, and soil pH was significantly greater in the CGR-treated soils. Calcium, Na, Mg, Al, and S concentrations in soils were all influenced by additions of CGR, but trace metal levels in the treatments were all within the range for uncontaminated soils. Ecosystem impact of applying CGR will be dependent upon the quality of CGR and soil characteristics. Controlling the liming potential of CGR should be considered a best management practice.
Afficher plus [+] Moins [-]Sorption of Selected Aromatic Substances—Application of Kinetic Concepts and Quantum Mechanical Modeling Texte intégral
2011
Klepsch, Sabine | Aquino, Adélia J. A. | Haas, Ursula | Tunega, Daniel | Haberhauer, Georg | Gerzabek, Martin H. | Lischka, Hans
Prediction of the sorption behavior of environmental pollutants is of utmost importance within the framework of risk assessments. In this work two approaches are presented with the aim to describe sorption of aromatic substances to geosorbents. First, analytical solutions of kinetic models were fitted to experimental data of batch sorption experiments with aniline and 1-naphthylamine onto animal manure-treated soil and the soil mineral montmorillonite. The models, accounting for equilibrium and nonequilibrium sorption coupled to transformation and/or irreversible sorption processes, could well reproduce the concentration course of the sorbates. Results suggest that the amounts transformed/degraded and irreversibly bound were higher for the soil than for the clay mineral. In the second part, quantum chemical calculations were performed on aniline and 1-naphthylamine interacting with acetic acid, acetamide, imidazole, and phenol as models of functional groups present in humic substances. Molecular modeling showed that formation of hydrogen bonds is the dominating binding mechanism in all modeled complexes, which are energetically very similar between aniline and 1-naphthylamine.
Afficher plus [+] Moins [-]Quality Assurance Decisions with Air Models: A Case Study of Imputation of Missing Input Data Using EPA’s Multi-layer Model Texte intégral
2011
Bowker, George E. | Schwede, Donna B. | Lear, Gary G. | Warren-Hicks, William J. | Finkelstein, Peter L.
Environmental models are frequently used within regulatory and policy frameworks to estimate environmental metrics that are difficult or impossible to physically measure. As important decision tools, the uncertainty associated with the model outputs should impact their use in informing regulatory decisions and scientific inferences. In this paper, we present a case study illustrating a process for dealing with a key issue in the use and application of air quality models, the additional error in annual mean aggregations resulting from imputation of missing data from model data sets. The case study is based on the US Environmental Protection Agency’s Multi-layer Model, which estimates the hourly dry deposition velocity of air pollutants based on hourly measurements of meteorology and site characteristics. A simulation was implemented to evaluate the effect of substituting historical hour-specific average values for missing model deposition velocity predictions on annual mean aggregations. Sensitivity studies were performed to test the effects of different missing data patterns and evaluate the relative impact of the substitution procedure on annual mean SO2 deposition velocity estimates. The substitution procedure was shown to result generally in long-term unbiased estimates of the annual mean and contributed less than 20% additional error to the estimate even when all data were missing. Consequently, it may be possible to use the historical record of deposition velocities to provide reasonably accurate and unbiased annual estimates of deposition velocities for years without meteorological measurements.
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