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Arsenic mobility controlled by solid calcium arsenates: A case study in Mexico showcasing a potentially widespread environmental problem
2013
Martínez-Villegas, Nadia | Briones-Gallardo, Roberto | Ramos-Leal, José A. | Avalos-Borja, Miguel | Castañón-Sandoval, Alan D. | Razo-Flores, Elías | Villalobos, Mario
An As-contaminated perched aquifer under an urban area affected by mining was studied over a year to determine the contamination source species and the mechanism of As mobilization. Results show that the dissolution of calcium arsenates in residues disposed on an inactive smelter has caused high levels of As pollution in the adjoining downgradient 6-km perched aquifer, reaching up to 158 mg/L of dissolved As, and releasing a total of ca. 7.5 tons of As in a year. Furthermore, free calcium ion availability was found to control As mobility in the aquifer through the diagenetic precipitation of calcium arsenates (Ca5H2(AsO4)4·cH2O) preventing further mobilization of As. Results shown here represent a model for understanding a highly underreported mechanism of retention of arsenate species likely to dominate in calcium-rich environments, such as those in calcareous sediments and soils, where the commonly reported mechanism of adsorption to iron(III) oxyhydroxides is not the dominant process.
Mostrar más [+] Menos [-]The impact of oscillating redox conditions: Arsenic immobilisation in contaminated calcareous floodplain soils
2013
Parsons, Christopher T. | Couture, Raoul-Marie | Omoregie, Enoma O. | Bardelli, Fabrizio | Greneche, Jean-Marc | Roman-Ross, Gabriela | Charlet, Laurent
Arsenic contamination of floodplain soils is extensive and additional fresh arsenic inputs to the pedosphere from human activities are ongoing.We investigate the cumulative effects of repetitive soil redox cycles, which occur naturally during flooding and draining, on a calcareous fluvisol, the native microbial community and arsenic mobility following a simulated contamination event.We show through bioreactor experiments, spectroscopic techniques and modelling that repetitive redox cycling can decrease arsenic mobility during reducing conditions by up to 45%. Phylogenetic and functional analyses of the microbial community indicate that iron cycling is a key driver of observed changes to solution chemistry. We discuss probable mechanisms responsible for the arsenic immobilisation observed in-situ. The proposed mechanisms include, decreased heterotrophic iron reduction due to the depletion of labile particulate organic matter (POM), increases to the proportion of co-precipitated vs. aqueous or sorbed arsenic with α-FeOOH/Fe(OH)3 and potential precipitation of amorphous ferric arsenate.
Mostrar más [+] Menos [-]Photochemical trajectory modeling of ozone concentrations in Hong Kong
2013
Cheng, H.R. | Saunders, S.M. | Guo, H. | Louie, P.K.K. | Jiang, F.
In this study, tropical cyclones over the East and South China Seas were found to be the most predominant weather conditions associated with the occurrence of high ozone (O3) episodes in Hong Kong in 2005–2009. A photochemical trajectory model coupled with Master Chemical Mechanism (MCM) was adapted to simulate the O3 concentrations during two O3 pollution episodes. The results agreed well with the observed data. A representative backward air mass trajectory was used to determine the contribution of each volatile organic compound (VOC) to the O3 levels. After taking into account both reactivity and mass emission of each VOC, 10 species were found to be the key O3 precursors in Hong Kong. Further analysis identified solvent related products accounting for 70% of the modeled O3 concentration in Hong Kong. The results highlight the importance of considering together reactivity and source sector emissions in developing targeted VOC reduction for O3 abatement strategies.
Mostrar más [+] Menos [-]Migration of polybrominated diphenyl ethers in biosolids-amended soil
2013
Gorgy, Tamer | Li, Loretta Y. | Grace, John R. | Ikonomou, Michael G.
A field investigation was carried out to determine PBDE concentrations over a one-year period in agricultural soils onto which 80 tonnes biosolids/hectare had been applied. The PBDE concentrations increased from 80 to 300 pg/g dry weight basis to 300 × 103–600 × 103 pg/g dw due to biosolids application, and PBDEs migrated downwards to depths of at least 0.85 m. Concentrations decreased non-uniformly with depth. PBDE levels decreased exponentially in the topmost biosolids-amended soils layer, while increasing in the next underlying soil layer over the one-year period. The rate of decrease of total PBDE mass in the top 0.00–0.05 m layer was almost two orders of magnitude greater than the rates of increase in total PBDE mass in the lower layers, indicating that effects such as photodegradation and/or volatilization likely were to have been significant in the surface layer.
Mostrar más [+] Menos [-]Protective role of fine silts for PAH in a former industrial soil
2013
Pernot, Audrey | Ouvrard, Stéphanie | Leglize, Pierre | Faure, Pierre
An original combined organic geochemistry and soil science approach was used to elucidate PAH availability controlling factors in a multi-contaminated industrial soil. Water granulodensimetric fractionation was applied to obtain five water-stable material fractions. These were characterized by elemental, molecular and mineral analysis, and microscopic observations. Among the different fractions, fine silts distinguished themselves by higher carbon and nitrogen contents, lower C/N ratio, an enrichment in total PAH and especially high molecular weight compounds, a coal tar signature and the lowest PAH availability. This fine silt fraction seemed to play a protective role for PAH that might be explained by its size and/or its specific reactivity. The mineral phases present in this fraction were proposed to explain the protection of organic matter. This led to a specific molecular signature of OM, having higher sorption properties both processes (sorption and mineral-bound protection) resulting in a lower PAH availability.
Mostrar más [+] Menos [-]An intercomparison of satellite-derived ground-level NO2 concentrations with GMSMB modeling results and in-situ measurements – A North American study
2013
Wang, Baozhen | Chen, Zhi
This paper investigates the biases associated with the ground-level nitrogen dioxide (NO2) concentrations derived from the satellite Ozone Monitoring Instrument (OMI) NO2 data through comparisons with the modeling and the monitoring results for the state of California in 2008. The seasonal and annual average ground-level NO2 concentrations are both analyzed from the OMI using the local NO2 profile obtained from the GEOS-Chem simulation. The OMI-derived ground-level NO2 concentrations are then compared with the NO2 concentrations predicted by a GIS-Based Multi-Source and Multi-Box model (GMSMB) and the in-situ measurements, correlation coefficients among the three sets of results are all above 0.84 with an average slope of 0.81 ± 0.04. Particularly, various biases associated with the three data sets have been analyzed, and the OMI-derived NO2 concentrations and the GMSMB modeling results have been proven to be essential for assessing regional air pollutant exposure risks with the aid of the extensive remote sensing database.
Mostrar más [+] Menos [-]Abiotic degradation of antibiotic ionophores
2013
Bohn, Pernille | Bak, Søren A. | Björklund, Erland | Krogh, Kristine A. | Hansen, Martin
Hydrolytic and photolytic degradation were investigated for the ionophore antibiotics lasalocid, monensin, salinomycin, and narasin. The hydrolysis study was carried out by dissolving the ionophores in solutions of pH 4, 7, and 9, followed by incubation at three temperatures of 6, 22, and 28 °C for maximum 34 days. Using LC–MS/MS for chemical analysis, lasalocid was not found to hydrolyse in any of the tested environments. Monensin, salinomycin, and narasin were all stable in neutral or alkaline solution but hydrolysed in the solution with a pH of 4. Half-lives at 25 °C were calculated to be 13, 0.6, and 0.7 days for monensin, salinomycin, and narasin, respectively.Absorbance spectra from each compound indicated that only lasalocid is degraded by photolysis (half-life below 1 h) due to an absorbance maximum around 303 nm, and monensin, salinomycin, and narasin are resistant to direct photolysis because they absorb light of environmentally irrelevant wavelengths.
Mostrar más [+] Menos [-]Biphasic dose responses in biology, toxicology and medicine: Accounting for their generalizability and quantitative features
2013
Calabrese, Edward J.
The most common quantitative feature of the hormetic-biphasic dose response is its modest stimulatory response which at maximum is only 30–60% greater than control values, an observation that is consistently independent of biological model, level of organization (i.e., cell, organ or individual), endpoint measured, chemical/physical agent studied, or mechanism. This quantitative feature suggests an underlying “upstream” mechanism common across biological systems, therefore basic and general. Hormetic dose response relationships represent an estimate of the peak performance of integrative biological processes that are allometrically based. Hormetic responses reflect both direct stimulatory or overcompensation responses to damage induced by relatively low doses of chemical or physical agents. The integration of the hormetic dose response within an allometric framework provides, for the first time, an explanation for both the generality and the quantitative features of the hormetic dose response.
Mostrar más [+] Menos [-]Influence of contact time and sediment composition on the bioavailability of Cd in sediments
2013
Zhong, Huan | Kraemer, Lisa | Evans, Douglas
Stable isotope 111Cd was spiked into sediments of different organic content levels for 3 days to 2 months. Bioavailability of spiked Cd to deposit-feeders, assessed by in vitro Cd solubilization, generally decreased with contact time but became comparable with that of background Cd after 2 months. This could be explained by the gradual transfer of Cd from the more mobile geochemical phase (carbonate associated phase) to more refractory phases (Fe–Mn oxide associated phase, and organic associated phase) within 2 months. The sedimentary organic content had a weak effect on Cd solubilization, while the distribution of Cd in carbonate or Fe–Mn oxide associated phase could have a larger influence on the solubilization of sedimentary Cd and its change with contact time. The observations in this study emphasize the need to consider Cd sequestration over time in sediments of various compositions, which would be useful in risk assessment of contaminated sediments.
Mostrar más [+] Menos [-]Titanium distribution in swimming pool water is dominated by dissolved species
2013
David Holbrook, R. | Motabar, Donna | Quiñones, Oscar | Stanford, Ben | Vanderford, Brett | Moss, Donna
The increased use of titanium dioxide nanoparticles (nano-TiO2) in consumer products such as sunscreen has raised concerns about their possible risk to human and environmental health. In this work, we report the occurrence, size fractionation and behavior of titanium (Ti) in a children's swimming pool. Size-fractionated samples were analyzed for Ti using ICP-MS. Total titanium concentrations ([Ti]) in the pool water ranged between 21 μg/L and 60 μg/L and increased throughout the 101-day sampling period while [Ti] in tap water remained relatively constant. The majority of [Ti] was found in the dissolved phase (<1 kDa), with only a minor fraction of total [Ti] being considered either particulate or microparticulate. Simple models suggest that evaporation may account for the observed variation in [Ti], while sunscreen may be a relevant source of particulate and microparticule Ti. Compared to diet, incidental ingestion of nano-Ti from swimming pool water is minimal.
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