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Pyrrolidinium Imides: Promising Ionic Liquids for Direct Capture of Elemental Mercury from Flue Gas Texte intégral
2008
Ji, Lei | Thiel, Stephen W | Pinto, Neville G
A new approach to vapor phase elemental mercury capture has been explored; this approach exploits an ionic liquid coating layer to oxidize elemental mercury for subsequent immobilization by chelating ligands. The room temperature ionic liquid 1-butyl-1-methyl pyrrolidinium bis(trifluoromethane sulfonyl)imide (P₁₄) was selected for study based on its oxidation potential window, thermal stability, and low vapor pressure. Tests were also completed in which KMnO₄ was added to P₁₄ to form a new ionic liquid, P₁₄-KMnO₄, with a higher oxidation potential. In room-temperature bulk liquid phase capture experiments, 59% of the elemental mercury in the inlet gas was captured using P₁₄ alone; mercury capture using P₁₄-KMnO₄ was quantitative. P₁₄ and P₁₄-KMnO₄ coatings were successfully applied to mesoporous silica substrates and to silica substrates functionalized with mercury chelating ligands. The coating layers were found to be thermally stable up to 300°C. Fixed-bed tests of nonfunctionalized silica coated with P₁₄ showed an elemental mercury uptake of 2.7 mg/g adsorbent at 160°C; at the same temperature, functionalized silica coated with P₁₄-KMnO₄ showed an elemental mercury capacity of at least 7.2 mg/g adsorbent, several times higher than that of activated carbon. The empty bed gas residence time in these tests was 0.04 s. A chelating adsorbent incorporating P₁₄ in the coating layer, may be capable of simultaneous removal of elemental and oxidized mercury from coal combustion flue gases.
Afficher plus [+] Moins [-]Dry and Wet Deposition of Nitrogen Emitted in Buenos Aires City to Waters of de la Plata River Texte intégral
2008
Pineda Rojas, Andrea L. | Venegas, Laura E.
Dry and Wet Deposition of Nitrogen Emitted in Buenos Aires City to Waters of de la Plata River Texte intégral
2008
Pineda Rojas, Andrea L. | Venegas, Laura E.
Dry and wet deposition of atmospheric nitrogen species (NO₂ and HNO₃) coming from nitrogen oxides emissions in Buenos Aires city to surface waters of de la Plata River were estimated. Atmospheric dispersion models DAUMOD-RD (v.2) and CALPUFF were applied to area and point sources, respectively. These models were run considering 1 year of hourly meteorological data. Emission information included a typical diurnal variation of area source emissions. Annual atmospheric nitrogen (N-NO₂ + N-HNO₃) deposition to 1,763 km² of the river was 35,600 kg-N year⁻¹. Dry deposition processes accounted for 89% of this value. The small contribution of wet deposition was a consequence of the very few cases (5%) of rain events during offshore wind conditions. Monthly dry deposition to 1,763 km² of the river varied from 1,628 kg-N month⁻¹ in February to 3,799 kg-N month⁻¹ in December, following the monthly occurrence of offshore winds. Monthly wet deposition varied from 1 kg-N month⁻¹ in June to 1,162 kg-N month⁻¹ in February. These results came from the combination of favorable conditions for formation of HNO₃ and the occurrence of precipitation during offshore wind situations. Spatial distribution of annual atmospheric N deposition showed a strong coastal gradient. Deposition values reached a maximum of 137.1 kg-N km⁻² year⁻¹ near the shoreline, which was reduced to the half at 4 km from the coast.
Afficher plus [+] Moins [-]Dry and Wet Deposition of Nitrogen Emitted in Buenos Aires City to Waters of de la Plata River Texte intégral
2008
Pineda Rojas, Andrea Laura | Venegas, Laura Esperanza
Dry and wet deposition of atmospheric nitrogen species (NO2 and HNO3) coming from nitrogen oxides emissions in Buenos Aires city to surface waters of de la Plata River were estimated. Atmospheric dispersion models DAUMOD-RD (v.2) and CALPUFF were applied to area and point sources, respectively. These models were run considering one year of hourly meteorological data. Emission information included a typical diurnal variation of area source emissions. Annual atmospheric nitrogen (N-NO2 + N-HNO3) deposition to 1763 km2 of the river was 35600 kg-N yr-1. Dry deposition processes accounted for 89% of this value. The small contribution of wet deposition was a consequence of the very few cases (5%) of rain events during offshore wind conditions. Monthly dry deposition to 1763 km2 of the river varied from 1628 kg-N month-1 in February to 3799 kg-N month-1 in December, following the monthly occurrence of offshore winds. Monthly wet deposition varied from 1 kg-N month-1 in June to 1162 kg-N month-1 in February. These results came from the combination of favorable conditions for formation of HNO3 and the occurrence of precipitation during offshore wind situations. Spatial distribution of annual atmospheric N deposition showed a strong coastal gradient. Deposition values reached a maximum of 137.1 kg-N km-2 yr-1 near the shoreline, which was reduced to the half at 4 km from the coast. | Fil: Pineda Rojas, Andrea Laura. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Centro de Investigaciones del Mar y la Atmósfera. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Centro de Investigaciones del Mar y la Atmósfera; Argentina | Fil: Venegas, Laura Esperanza. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Departamento de Ciencias de la Atmósfera y los Océanos; Argentina
Afficher plus [+] Moins [-]Elemental Mercury Control by Novel Oxidant and Sorbent in an Entrained-Flow System Texte intégral
2008
Lee, Sang-Sup | Lee, Joo-Youp | Keener, Tim C
An entrained-flow system has been designed and constructed to simulate in-flight mercury capture by sorbents in ducts of coal-fired utility plants. The test conditions of 1.5 s residence time, 140°C temperature, 4.5 ppbv inlet Hg⁰ concentration, and 0-20 lb/MMacf sorbent injection rates were chosen to simulate conditions in the ducts. Novel oxidants developed in previous fixed-bed tests and novel sorbents derived from the novel oxidants were tested for their Hg⁰ capture in the entrained-flow system to examine the possibility of using those sorbents in a full-scale system. Darco-FGD and Darco Hg-LH served as benchmark sorbents with which mercury control capability of the novel oxidants and novel sorbents could be compared. The test results showed that the novel oxidants have remarkable Hg⁰ oxidation capability, and the novel sorbents showed a better performance in Hg⁰ removal than Darco Hg-LH.
Afficher plus [+] Moins [-]Sources and Mass Flows of Xenobiotics in Urban Water Cycles--an Overview on Current Knowledge and Data Gaps Texte intégral
2008
Bester, K | Scholes, L | Wahlberg, C | McArdell, C. S
In this study, several emerging compounds of concern in waste water are identified and discussed in relation to data available on their sources and mass flows in urban waters. In most western European situations, the highest contributions to the mass flow of xenobiotics to the urban water cycle stems from household and services applications (e.g. personal care compounds, pharmaceuticals, steroid hormones, flame retardants, fluorinated detergents etc.) as well as building and constructing environments (e.g. flame retardants, plasticizers, UV-blockers and biocides). The contribution from industrial point sources such as incineration industries e.g. coal, tar, steel and gas production (such as PAHs, PCBs, dioxins, etc.) and chemical industries are decreasing in relevance in terms of input and are hence currently of more local relevance only. In relation to identified compounds, this paper considers current data availability and its use in a range of management strategies for the mitigation or controlling of xenobiotics 'at source'. However it also identifies major knowledge gaps relating to the behaviour and fate of organic pollutants in various sectors of the urban water cycle including stormwater management, bank- and soil infiltration as well as underground and soil passage of polluted waters. It is also discussing the major sources of a range of current day urban pollutants. The paper considers the sources of emerging pollutants in a qualitative way.
Afficher plus [+] Moins [-]Soil Microbial Community Function and Structure in a Post-mining Chronosequence Texte intégral
2008
Temporal changes in microbial community function (enzymatic activities) and structure (phospholipid fatty acids) were studied in a post-mining chronosequence of coal discard sites of different rehabilitation ages. The objective was to determine whether temporal changes in microbial community function and structure were related to rehabilitation age or management practices. No trends consistent with the rehabilitation ages (1 to 11 years) of the respective sites were observed. A canonical correspondence analysis showed that sites clustered according to the time of sampling irrespective of their individual rehabilitation ages. Sites sampled in 2002 clustered together, while sites sampled in 2004 and 2005 clustered separately from the 2002 sites. This corresponded with a change in management practices applied after 2002. Dehydrogenase, β-glucosidase, acid phosphatase, and alkaline phosphatase activities for all sites were higher after 2002. Urease activities were lower after 2002, with the exception of Site 3 (4 years old in 2002). Phospholipid fatty acid data showed significant (p < 0.05) differences between sites of different rehabilitation ages over the study period. There was a decrease in microbial biomass in all sites from 2002 to 2004 but an increase in 2005. Fungal to bacterial abundance ratios for all sites decreased over the study period. The proportion of the total microbial community comprised of Gram positive bacteria increased from 2002 to 2005. These data show the value of microbial community function and structure to elucidate management effects that may not be apparent through traditional assessments of rehabilitation status such as aboveground indicators.
Afficher plus [+] Moins [-]Application of Adjoint-based Forecast Sensitivities to Asian Dust Transport Events in Korea Texte intégral
2008
Kim, Hyun Mee | Kay, Jun Kyung | Jung, Byoung-Joo
Sensitivities of the forecast to changes in the initial state are evaluated for an Asian dust event, which affected the Korean Peninsula on 7 to 9 April 2006, to understand the impact of initial condition uncertainties on the forecast and thence to suggest the sensitive regions for adaptive observations of the Asian dust. To assess the forecast sensitivities, adjoint-based sensitivities were used. Sensitive regions are located over the northwestern part of Mongolia at the initial time, then propagate to Inner Mongolia and Manchuria. Close to the verification time, sensitive regions as determined by adjoint-based forecast sensitivities coincide with the passage of the Asian dust. Forecast error for the atmospheric circulation during the dust event is reduced 57.4% by extracting properly weighted adjoint-based forecast sensitivity perturbations from the initial state, and the correction occurs primarily in the upper troposphere where the forecast error is the largest. The improvement in the overall forecast implies that adjoint-based forecast sensitivities would be beneficial in determining the observational sites and in improving the forecast of Asian dust events. An additional experiment with another Asian dust event confirms the validity of adjoint-based forecast sensitivities to Asian dust events.
Afficher plus [+] Moins [-]Identification of Odor Causing Compounds in a Commercial Dairy Farm Texte intégral
2008
Lu, Mingming | Lamichhane, Prabhat | Liang, Fuyan | Imerman, Eric | Chai, Ming
The odorous air emissions from confined animal feeding operations (CAFOs), such as swine, poultry and dairy farms, are increasingly raising community complaints. Odorous emissions can result in health damages, psychological discomforts and adverse aesthetic effects in the community. However, these emissions are not well characterized up to now due to the lack of legislation, the limitations in sampling and instrumentation techniques, and the complexity of the emissions themselves. This study is aimed at the development of a high volume sampler and sorbent assembly to identify the odor causing compounds from a diary CAFO. The sorbent was custom designed to target the potential compounds that may exist in a dairy farm and was validated in laboratory with a synthetic odor from the swine manure. The actual samples at the diary farm were collected in spring and summer of 2005. The sorbents were solvent extracted and individual odor compounds were identified using GC-MS (gas chromatography-mass spectroscopy). The data obtained indicated that high volume sampling can shorten the sampling time from days to within 4 h. Both volatile organic compounds (VOCs) and volatile fatty acids (VFAs) have been identified from the dairy farm, such as phenol, methylphenol, 4-ethyl phenol, indole, methyl indole, benzyl alcohol, hexanoic acid, valeric acid and iso-valeric acid, together with some nitrogen containing compounds that have not been reported before.
Afficher plus [+] Moins [-]In-Stream Processing of Sediment-Associated Metals in Peatland Fluvial Systems Texte intégral
2008
Rothwell, J. J. | Evans, M. G. | Allott, T. E. H.
The interaction between fluvially transported, metal contaminated peat particulates and acidic waters draining peatland catchments has received limited attention. Potential in-stream processing of sediment-associated metals in acidic stream water was investigated in laboratory based mixing experiments, designed to represent conditions of fluvial sediment transport in a highly contaminated and severely eroding peatland catchment in the Peak District (UK). Over the initial 20 min of the first experiment, stream water Cr and Zn concentrations increased by at least an order-of-magnitude and remained elevated for the full duration (24 h) of the experiment. Stream water As, Mo, Pb, Ti and V concentrations increased between 43% (As) and 440% (V) over the first hour of the experiment. After 24 h most of the metals appeared to have reached equilibrium in the water column. Results of the second experiment revealed that when the concentration of metal contaminated peat particulates is increased, there is an associated increase in the stream water As, Cr, Mo, Pb, Ti, V and Zn concentrations. The experimental data suggest that As, Cr, Mo, Pb, Ti, V and Zn are liable to desorption from metal contaminated peat into acidic stream water. The solubilisation of contaminated peat particulates may also contribute to elevated stream water metal concentrations. The laboratory based approach used in this study may indicate that when there is erosion of metal contaminated peat into acidic fluvial systems there is a concomitant increase in dissolved metal levels, especially when suspended sediment concentrations are high. Further laboratory and field based experiments are required to evaluate the relative importance of physical and chemical processes in the interaction between contaminated peat particulates and stream water in peatland fluvial systems.
Afficher plus [+] Moins [-]Double Health Risk in Arsenic Contaminated Drinking Water - Evidence of Enhanced Alpha Radioactivity Texte intégral
2008
Ghosh, Dipak | Deb, Argha | Patra, Kanchan Kumar | Sengupta, Rosalima | Bera, Sukumar
The presence of alpha emitting radionuclides in the environment assumes importance since they are found to be carcinogenic. This paper reports the results of an exhaustive and systematic measurement of alpha radioactivity using solid state nuclear track detector (SSNTD) in drinking water in different parts of India covering the entire Ganges Basin - West Bengal, Bihar and Uttar Pradesh where arsenic contamination is severe. The alpha activity in the samples was found in the range of 8 to 800 Bq/l in West Bengal, 90 to 1,000 Bq/l in Uttar Pradesh and 60 to 1,000 Bq/l in Bihar - much higher alpha activity value than MCL value given by US EPA. The concentration of alpha activity has a positive correlation with that of arsenic.
Afficher plus [+] Moins [-]Atmospheric Impacts due to Anthropogenic Activities in Remote Areas: The Case Study of Admiralty Bay/King George Island/Antarctic Peninsula Texte intégral
2008
The aim of the present work is to characterize the local atmospheric emissions levels and compare them to the component derived from global pollution in a remote site at South Hemisphere (Admiralty Bay located at King George Island in Antarctic Peninsula). Airborne particles, snow and soil/sediments samples were analyzed. Local-produced atmospheric aerosol dispersion was estimated for metals originated by fossil fuel burning from the permanent scientific stations using a simplified Gaussian model. Validation of atmospheric dispersion was established by in situ measurements. Soluble and insoluble particles deposited in freshly snow and airborne particles were analyzed by PIXE (Particle Induced X-Ray Emission) for the determination of the elemental mass concentration and to obtain the Mass Median Aerodynamic Diameter (MMAD). The results showed significant correlation between the concentration of atmospheric aerosol and the freshly deposited particles in the snow, and permitted an estimate of the atmospheric snow deposition factor for K, Cu, Zn, Fe, Pb, and Ti. Results of long-term aerosol data compilation suggest that besides the local aerosol sources, the continental atmospheric transport of airborne particles is not significantly affected by the airborne particles produced by local human impacts at King George Island.
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