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791.
The presence of polybrominated diphenyl ethers (PBDEs) from mono to hepta brominated and 11 hydroxylated (OH-) and methoxylated (MeO-) PBDEs was examined in 37 breast milk samples collected from 11 mothers living in Barcelona. An extraction method based on accelerated solvent extraction followed by gas chromatography coupled to high resolution mass spectrometry was used to inequivocally identify all target compounds at the low pg g(-1) lw level. Data obtained were examined for absolute and relative concentrations and specific PBDE, OH- and MeO-PBDE congener patterns. Sigma PBDE concentration ranged between 1,161 and 1,372,797 pg g(-1) lw and BDEs 47, 99, 100, 153 and 183 accounted for more than 80% of the total PBDEs. All tri and tetra OH- and MeO-PBDEs compounds were detected at levels between 6 and 14,984 pg g(-1)lw. The median ratio OH/PBDE and MeO-PBDEs/PBDEs was from 2.9% to 1.6%, respectively, suggesting either that PBDE metabolism to OH- and MeO- derivatives is not an important degradation route in humans or either OH- and MeO-PBDEs are rapidly excreted. No significant correlation was observed between PBDEs and OH- and MeO-PBDE, although OH- and OMe-PBDEs co-occurred in mothers' milk (R(2)=0.5349). According to the daily intake of PBDEs and OH- and MeO-PBDEs, which was between 0.47 and 363 ng d(-1) (excluding a smoking donor), potential health risks associated with these compounds are assessed. 相似文献
792.
T.G. Soares Neto J.A. Carvalho C.A.G. Veras E.C. Alvarado R. Gielow E.N. Lincoln T.J. Christian R.J. Yokelson J.C. Santos 《Atmospheric environment (Oxford, England : 1994)》2009,43(2):438-446
Biomass consumption and CO2, CO and hydrocarbon gas emissions in an Amazonian forest clearing fire are presented and discussed. The experiment was conducted in the arc of deforestation, near the city of Alta Floresta, state of Mato Grosso, Brazil. The average carbon content of dry biomass was 48% and the estimated average moisture content of fresh biomass was 42% on wet weight basis. The fresh biomass and the amount of carbon on the ground before burning were estimated as 528 t ha?1 and 147 t ha?1, respectively. The overall biomass consumption for the experiment was estimated as 23.9%. A series of experiment in the same region resulted in average efficiency of 40% for areas of same size and 50% for larger areas. The lower efficiency obtained in the burn reported here occurred possibly due to rain before the experiment. Excess mixing ratios were measured for CO2, CO, CH4, C2–C3 aliphatic hydrocarbons, and PM2.5. Excess mixing ratios of CH4 and C2–C3 hydrocarbons were linearly correlated with those of CO. The average emission factors of CO2, CO, CH4, NMHC, and PM2.5 were 1,599, 111.3, 9.2, 5.6, and 4.8 g kg?1 of burned dry biomass, respectively. One hectare of burned forest released about 117,000 kg of CO2, 8100 kg of CO, 675 kg of CH4, 407 kg of NMHC and 354 kg of PM2.5. 相似文献
793.
S. Szopa G. Foret L. Menut A. Cozic 《Atmospheric environment (Oxford, England : 1994)》2009,43(6):1189-1195
In this study, we investigate the benefit for European ozone simulation of using day-to-day varying chemical boundary conditions produced by a global chemical weather forecast platform instead of climatological monthly means at the frontiers of a regional model. We performed two simulations over Europe using the regional (0.5 × 0.5°) CHIMERE CTM forced by global scale simulations based on the LMDz-INCA CTM. For summer 2005, ozone differences exceeding 20 ppb can be punctually found between these two simulations in the borders of the domain. The mean of the differences ranges between 0 and 3 ppb beyond 15° of the frontiers of the regional model.Correlations with ground-based ozone measurements at more than 400 stations are slightly increased by the use of daily boundary conditions. The simulation of the temporal variability is significantly enhanced in particular for the daily means and daily maxima. As expected, the gain is higher at the borders of the regional domain.The change of percentile distribution shows that the net impact of high temporal resolution boundary conditions is not of major concern for surface ozone peaks which are mainly due to local photochemistry. The use of daily boundary conditions is however necessary to correctly simulate concentrations in the 20–35 ppb range which are of crucial interest for human and vegetation exposure effects. 相似文献
794.
Francisco Payri Vicente R. Bermúdez Bernardo Tormos Waldemar G. Linares 《Atmospheric environment (Oxford, England : 1994)》2009,43(6):1273-1279
Diesel engine emissions are composed of a long list of organic compounds, ranging from C2 to C12+, and coming from the hydrocarbons partially oxidized in combustion or produced by pyrolisis. Many of these are considered as ozone precursors in the atmosphere, since they can interact with nitrogen oxides to produce ozone under atmospheric conditions in the presence of sunlight. In addition to problematic ozone production, Brookes, P., and Duncan, M. [1971. Carcinogenic hydrocarbons and human cells in culture. Nature.] and Heywood, J. [1988. Internal Combustion Engine Fundamentals.Mc Graw-Hill, ISBN 0-07-1000499-8.] determined that the polycyclic aromatic hydrocarbons present in exhaust gases are dangerous to human health, being highly carcinogenic.The aim of this study was to identify by means of gas chromatography the amount of each hydrocarbon species present in the exhaust gases of diesel engines operating with different biodiesel blends. The levels of reactive and non-reactive hydrocarbons present in diesel engine exhaust gases powered by different biodiesel fuel blends were also analyzed.Detailed speciation revealed a drastic change in the nature and quantity of semi-volatile compounds when biodiesel fuels are employed, the most affected being the aromatic compounds. Both aromatic and oxygenated aromatic compounds were found in biodiesel exhaust. Finally, the conservation of species for off-side analysis and the possible influence of engine operating conditions on the chemical characterization of the semi-volatile compound phase are discussed.The use of oxygenated fuel blends shows a reduction in the Engine-Out emissions of total hydrocarbons. But the potential of the hydrocarbon emissions is more dependent on the compositions of these hydrocarbons in the Engine-Out, to the quantity; a large percent of hydrocarbons existing in the exhaust, when biodiesel blends are used, are partially burned hydrocarbons, and are interesting as they have the maximum reactivity, but with the use of pure biodiesel and diesel, the most hydrocarbons are from unburned fuel and they have a less reactivity. The best composition in the fuel, for the control of the hydrocarbon emissions reactivity, needs to be a fuel with high-saturated fatty acid content. 相似文献
795.
Huiqun Wang Daniel J. Jacob Philippe Le Sager David G. Streets Rokjin J. Park Alice B. Gilliland A. van Donkelaar 《Atmospheric environment (Oxford, England : 1994)》2009,43(6):1310-1319
We use a global chemical transport model (GEOS-Chem) with 1° × 1° horizontal resolution to quantify the effects of anthropogenic emissions from Canada, Mexico, and outside North America on daily maximum 8-hour average ozone concentrations in US surface air. Simulations for summer 2001 indicate mean North American and US background concentrations of 26 ± 8 ppb and 30 ± 8 ppb, as obtained by eliminating anthropogenic emissions in North America vs. in the US only. The US background never exceeds 60 ppb in the model. The Canadian and Mexican pollution enhancement averages 3 ± 4 ppb in the US in summer but can be occasionally much higher in downwind regions of the northeast and southwest, peaking at 33 ppb in upstate New York (on a day with 75 ppb total ozone) and 18 ppb in southern California (on a day with 68 ppb total ozone). The model is successful in reproducing the observed variability of ozone in these regions, including the occurrence and magnitude of high-ozone episodes influenced by transboundary pollution. We find that exceedances of the 75 ppb US air quality standard in eastern Michigan, western New York, New Jersey, and southern California are often associated with Canadian and Mexican pollution enhancements in excess of 10 ppb. Sensitivity simulations with 2020 emission projections suggest that Canadian pollution influence in the Northeast US will become comparable in magnitude to that from domestic power plants. 相似文献
796.
P. Bogaert G. Christakos M. Jerrett H.-L. Yu 《Atmospheric environment (Oxford, England : 1994)》2009,43(15):2471-2480
This paper is concerned with the spatiotemporal mapping of monthly 8-h average ozone (O3) concentrations over California during a 15-years period. The basic methodology of our analysis is based on the spatiotemporal random field (S/TRF) theory. We use a S/TRF decomposition model with a dominant seasonal O3 component that may change significantly from site to site. O3 seasonal patterns are estimated and separated from stochastic fluctuations. By means of Bayesian Maximum Entropy (BME) analysis, physically meaningful and sufficiently detailed space–time maps of the seasonal O3 patterns are generated across space and time. During the summer and winter months the seasonal O3 concentration maps exhibit clear and progressively changing geographical patterns over time, suggesting the existence of relationships in accordance with the typical physiographic and climatologic features of California. BME mapping accuracy can be superior to that of other techniques commonly used by EPA; its framework can rigorously assimilate useful data sources that were previously unaccounted for; the generated maps offer valuable assessments of the spatiotemporal O3 patterns that can be helpful in the identification of physical mechanisms and their interrelations, the design of human exposure and population health models, and in risk assessment. As they focus on the seasonal patterns, the maps are not contingent on short-time and locally prevalent weather conditions, which are of no interest in a global and non-forecasting framework. Moreover, the maps offer valuable insight about the space–time O3 concentration patterns and are, thus, helpful for disentangling the influence of explanatory factors or even for identifying some influential ones that could have been otherwise overlooked. 相似文献
797.
Nenad Aleksic K. Roy G. Sistla J. Dukett N. Houck P. Casson 《Atmospheric environment (Oxford, England : 1994)》2009,43(17):2709-2716
Federal and state programs over the past two decades have resulted in the reduction of emissions of precursors of acid rain. Concomitant with these changes, measured concentrations of acidity in precipitation and in watersheds have shown a downward trend or improvement. However, another pathway for these precursors is through cloud and fog events that often tend to occur at high-elevation regions affecting the fauna and flora as well. In this study we report on long-term measurements of cloud water and precipitation chemistry made from 1994 onwards at a high-elevation location, Whiteface Mountain NY, in the northeastern United States. Trends and inter-relationship between the ions were examined along with ambient SO2 measurements and Adirondack lakes chemistry data. 相似文献
798.
Juan G. Navea Shihe Xu Charles O. Stanier Mark A. Young Vicki H. Grassian 《Atmospheric environment (Oxford, England : 1994)》2009,43(26):4060-4069
We have carried out kinetic studies to characterize the heterogeneous decay of octamethylcyclotetrasiloxane (D4) and decamethylcyclopentasiloxane (D5) in the presence of representative mineral dust aerosol in order to obtain a better understanding of the atmospheric fate of these siloxanes. The heterogeneous chemistry of D4 and D5 with various mineral dusts was studied in an environmental aerosol reaction chamber using FTIR absorption spectroscopy to monitor the reaction. The apparent heterogeneous uptake coefficient, γapp, for D4 and D5 with various mineral dusts was measured under dry conditions and as a function of relative humidity (RH). In addition, the effect of initial D4 and D5 concentration on the rate and yield of the reaction was examined. The uptake coefficient, γapp, for D4 and D5 was similar for the most reactive aerosols tested, with kaolinite ≈hematite > silica. Limited uptake onto carbon black and calcite surfaces was observed for either siloxane. Reaction with hematite and kaolinite resulted in multilayer coverages, suggesting extensive polymerization of D4 and D5 on the aerosol surface. 相似文献
799.
Zheng Li Erin N. Porter Andreas Sjödin Larry L. Needham Sangil Lee Armistead G. Russell James A. Mulholland 《Atmospheric environment (Oxford, England : 1994)》2009,43(27):4187-4193
Twenty-eight polycyclic aromatic hydrocarbons (PAH) and methylated PAHs (Me-PAH) were measured in daily PM2.5 samples collected at an urban site, a suburban site, and a rural site in and near Atlanta during 2004 (5 samples/month/site). The suburban site, located near a major highway, had higher PM2.5-bound PAH concentrations than did the urban site, and the rural site had the lowest PAH levels. Monthly variations are described for concentrations of total PAHs (∑PAHs) and individual PAHs. PAH concentrations were much higher in cold months than in warm months, with average monthly ∑PAH concentrations at the urban and suburban-highway monitoring sites ranging from 2.12 to 6.85 ng m?3 during January–February and November–December 2004, compared to 0.38–0.98 ng m?3 during May–September 2004. ∑PAH concentrations were found to be well correlated with PM2.5 and organic carbon (OC) within seasons, and the fractions of PAHs in PM2.5 and OC were higher in winter than in summer. Methyl phenanthrenes were present at higher levels than their un-substituted homologue (phenanthrene), suggesting a petrogenic (unburned petroleum products) input. Retene, a proposed tracer for biomass burning, peaked in March, the month with the highest acreage and frequency of prescribed burning and unplanned fires, and in December, during the high residential wood-burning season, indicating that retene might be a good marker for burning of all biomass materials. In contrast, potassium peaked only in December, indicating that it might be a more specific tracer for wood-burning. 相似文献
800.
do A Kehrig H Seixas TG Palermo EA Baêta AP Castelo-Branco CW Malm O Moreira I 《Environmental science and pollution research international》2009,16(1):10-24
Background, aim, and scope Selenium (Se) has been shown to reduce mercury (Hg) bioavailability and trophic transfer in aquatic ecosystems. The study
of methylmercury (MeHg) and Se bioaccumulation by plankton is therefore of great significance in order to obtain a better
understanding of the estuarine processes concerning Hg and Se accumulation and biomagnification throughout the food web. In
the western South Atlantic, few studies have documented trace element and MeHg in fish tissues. No previous study about trace
elements and MeHg in plankton has been conducted concerning tropical marine food webs. Se, Hg, and MeHg were determined in
two size classes of plankton, microplankton (70–290 μm) and mesoplankton (≥290 μm), and also in muscle tissues and livers
of four fish species of different trophic levels (Mugil liza, a planktivorous fish; Bagre spp., an omnivorous fish; Micropogonias furnieri, a benthic carnivorous fish; and Centropomus undecimalis, a pelagic carnivorous fish) from a polluted estuary in the Brazilian Southeast coast, Guanabara Bay. Biological and ecological
factors such as body length, feeding habits, and trophic transfer were considered in order to outline the relationships between
these two elements. The differences in trace element levels among the different trophic levels were investigated.
Materials and methods Fish were collected from July 2004 to August 2005 at Guanabara Bay. Plankton was collected from six locations within the bay
in August 2005. Total mercury (THg) was determined by cold vapor atomic absorption spectrometry (CV-AAS) with sodium borohydride
as a reducing agent. MeHg analysis was conducted by digesting samples with an alcoholic potassium hydroxide solution followed
by dithizone-toluene extraction. MeHg was then identified and quantified in the toluene layer by gas chromatography with an
electron capture detector (GC-ECD). Se was determined by AAS using graphite tube with Pin platform and Zeeman background correction.
Results and discussion Total mercury, MeHg, and Se increased with plankton size class. THg and Se values were below 2.0 and 4.8 μg g−1 dry wt in microplankton and mesoplankton, respectively. A large excess of molar concentrations of Se in relation to THg was
observed in both plankton size class and both fish tissues. Plankton presented the lowest concentrations of this element.
In fish, the liver showed the highest THg and Se concentrations. THg and Se in muscle were higher in Centropomus undecimalis (3.4 and 25.5 nmol g−1) than in Micropogonias furnieri (2.9 and 15.3 nmol g−1), Bagre spp (1.3 and 3.4 nmol g−1) and Mugil liza (0.3 and 5.1 nmol g−1), respectively. The trophic transfer of THg and Se was observed between trophic levels from prey (considering microplankton
and mesoplankton) to top predator (fish). The top predators in this ecosystem, Centropomus undecimalis and Micropogonias furnieri, presented similar MeHg concentrations in muscles and liver. Microplankton presented lower ratios of methylmercury to total
mercury concentration (MeHg/THg) (34%) than those found in mesoplankton (69%) and in the muscle of planktivorous fish, Mugil liza (56%). The other fish species presented similar MeHg/THg in muscle tissue (of around 100%). M. liza showed lower MeHg/THg in the liver than C. undecimalis (35%), M. furnieri (31%) and Bagre spp. (22%). Significant positive linear relationships were observed between the molar concentrations of THg and Se in the
muscle tissue of M. furnieri and M. liza. These fish species also showed significant inverse linear relationships between hepatic MeHg and Se, suggesting a strong
antagonistic effect of Se on MeHg assimilation and accumulation.
Conclusions Differences found among the concentrations THg, MeHg, and Se in microplankton, mesozooplankton, and fishes were probably related
to the preferred prey and bioavailability of these elements in the marine environment. The increasing concentration of MeHg
and Se at successively higher trophic levels of the food web of Guanabara Bay corresponds to a transfer between trophic levels
from the lower trophic level to the top-level predator, suggesting that MeHg and Se were biomagnified throughout the food
web. Hg and Se were positively correlated with the fish standard length, suggesting that larger and older fish bioaccumulated
more of these trace elements. THg, MeHg, and Se were a function of the plankton size.
Recommendations and perspectives There is a need to assess the role of selenium in mercury accumulation in tropical ecosystems. Without further studies of
the speciation of selenium in livers of fishes from this region, the precise role of this element, if any, cannot be verified
in positively affecting mercury accumulation. Further studies of this element in the study of marine species should include
liver samples containing relatively high concentrations of mercury. A basin-wide survey of selenium in fishes is also recommended. 相似文献