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741.
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
742.
Improved measurements of ammonia losses from cattle feedlots are needed to quantify the national NH3 emissions inventory and evaluate management techniques for reducing emissions. Speciation cartridges composed of glass honeycomb denuders and filter packs were adapted to measure gaseous NH3 and aerosol NH4+ fluxes using relaxed eddy accumulation (REA). Laboratory testing showed that a cartridge equipped with four honeycomb denuders had a total capture capacity of 1800 μg of NH3. In the field, a pair of cartridges was deployed adjacent to a sonic anemometer and an open-path gas analyzer on a mobile tower. High-speed valves were attached to the inlets of the cartridges and controlled by a datalogger so that up- and down-moving eddies were independently sampled based on direction of the vertical wind speed and a user-defined deadband. Air flowed continuously through the cartridges even when not sampling by means of a recirculating air handling system. Eddy covariance measurement of CO2 and H2O, as measured by the sonic and open-path gas analyzer, were used to determine the relaxation factor needed to compute REA-based fluxes. The REA system was field tested at the Beef Research Unit at Kansas State University in the summer and fall of 2007. Daytime NH3 emissions ranged between 68 and 127 μg m?2 s?1; fluxes tended to follow a diurnal pattern correlated with latent heat flux. Daily fluxes of NH3 were between 2.5 and 4.7 g m?2 d?1 and on average represented 38% of fed nitrogen. Aerosol NH4+ fluxes were negligible compared with NH3 emissions. An REA system designed around the high-capacity speciation cartridges can be used to measure NH3 fluxes from cattle feedlots and other strong sources. The system could be adapted to measure fluxes of other gases and aerosols. 相似文献
743.
A.K. Georgoulias D. Balis M.E. Koukouli C. Meleti A. Bais C. Zerefos 《Atmospheric environment (Oxford, England : 1994)》2009,43(9):1693-1701
We present characteristics of the sulfur dioxide (SO2) loading over Thessaloniki, Greece, and seven other selected sites around the world using SO2 total column measurements from Brewer spectrophotometers together with satellite estimates of the Version 8 TOMS Sulfur Dioxide Index (SOI) over the same locations, retrieved from Nimbus 7 TOMS (1979–1993), Earth Probe TOMS (1996–2003) and OMI/Aura (2004–2006). Traditionally, the SOI has been used to quantify the SO2 quantities emitted during great volcanic eruptions. Here, we investigate whether the SOI can give an indication of the total SO2 load for areas and periods away from eruptive volcanic activity by studying its relative changes as a correlative measure to the SO2 total column. We examined time series from Thessaloniki and another seven urban and non-urban stations, five in the European Union (Arosa, De Bilt, Hohenpeissenberg, Madrid, Rome) and two in India (Kodaikanal, New Delhi). Based on the Brewer data, Thessaloniki shows high SO2 total columns for a European Union city but values are still low if compared to highly affected regions like those in India. For the time period 1983–2006 the SO2 levels above Thessaloniki have generally decreased with a rate of 0.028 Dobson Units (DU) per annum, presumably due to the European Union's strict sulfur control policies. The seasonal variability of the SO2 total column exhibits a double peak structure with two maxima, one during winter and the second during summer. The winter peak can be attributed to central heating while the summer peak is due to synoptic transport from sources west of the city and sources in the north of Greece. A moderate correlation was found between the seasonal levels of Brewer total SO2 and SOI for Thessaloniki, Greece (R = 0.710–0.763) and Madrid, Spain (R = 0.691) which shows that under specific conditions the SOI might act as an indicator of the SO2 total load. 相似文献
744.
K. Baetens Q.T. Ho D. Nuyttens M. De Schampheleire A. Melese Endalew M.L.A.T.M. Hertog B. Nicolaï H. Ramon P. Verboven 《Atmospheric environment (Oxford, England : 1994)》2009,43(9):1674-1682
Correct field drift prediction is a key element in environmental risk assessment of spraying applications. A reduced order drift prediction model based on the diffusion–advection equation is presented. It allows fast assessment of the drift potential of specific ground boom applications under specific environmental wind conditions that obey the logarithmic wind profile. The model was calibrated based on simulations with a validated Computational Fluid Dynamics (CFD) model. Validation of both models against 38 carefully conducted field experiments is successfully performed for distances up to 20 m from the field edge, for spraying on flat pasture land. The reduced order model succeeded in correct drift predictions for different nozzle types, wind velocities, boom heights and spray pressures. It used 4 parameters representing the physical aspects of the drift cloud; the height of the cloud at the field edge, the mass flux crossing the field edge, the settling velocity of the droplets and the turbulence. For the parameter set and range considered, it is demonstrated for the first time that the effect of the droplet diameter distribution of the different nozzle types on the amount of deposition spray drift can be evaluated by a single parameter, i.e., the volume fraction of droplets with a diameter smaller than 191 μm. The reduced order model can be solved more than 4 orders of magnitude faster than the comprehensive CFD model. 相似文献
745.
Inhalation of particulate pollutants below 10 μm in size (PM10) is associated with adverse health effects. Here we use magnetic remanence measurements of roadside tree leaves to examine levels of vehicle-derived PM around Lancaster, UK. Leaf saturation remanence (SIRM) values exhibit strong correlation with both the SIRM and particulate mass of co-located, pumped-air samples, indicating that these leaf magnetic values are an effective proxy for ambient PM10 concentrations. Biomagnetic monitoring using tree leaves can thus provide high spatial resolution data sets for assessment of particulate pollution levels at pedestrian-relevant heights. Leaf SIRM values not only increase with proximity to roads with higher traffic volumes, but are also ~100% higher at 0.3 m than at ~1.5–2 m height. Magnetic and SEM data indicate that the particle populations are dominated by spherical, iron-rich particles ~0.1–1 μm in diameter, with fewer larger, more angular, silica-rich particles. Comparison of the roadside leaf-calculated PM10 concentrations with PM10 concentrations predicted by a widely-used atmospheric dispersion model indicates some agreement between them. However, the model under-predicts PM10 concentrations at ‘urban hotspots’ such as major–minor road junctions and traffic lights. Conversely, the model over-predicts PM10 concentrations with distance from the road wherever one tree is screened by another, indicating the filtering/protective effect of roadside trees in leaf. 相似文献
746.
Chester W. Spicer Michael W. Holdren Kenneth A. Cowen Darrell W. Joseph Jan Satola Bradley Goodwin Howard Mayfield Alexander Laskin M. Lizabeth Alexander John V. Ortega Matthew Newburn Robert Kagann Ram Hashmonay 《Atmospheric environment (Oxford, England : 1994)》2009,43(16):2612-2622
Aircraft emissions affect air quality on scales from local to global. More than 20% of the jet fuel used in the U.S. is consumed by military aircraft, and emissions from this source are facing increasingly stringent environmental regulations, so improved methods for quickly and accurately determining emissions from existing and new engines are needed. This paper reports results of a study to advance the methods used for detailed characterization of military aircraft emissions, and provides emission factors for two aircraft: the F-15 fighter and the C-130 cargo plane. The measurements involved outdoor ground-level sampling downstream behind operational military aircraft. This permits rapid change-out of the aircraft so that engines can be tested quickly on operational aircraft. Measurements were made at throttle settings from idle to afterburner using a simple extractive probe in the dilute exhaust. Emission factors determined using this approach agree very well with those from the traditional method of extractive sampling at the exhaust exit. Emission factors are reported for CO2, CO, NO, NOx, and more than 60 hazardous and/or reactive organic gases. Particle size, mass and composition also were measured and are being reported separately. Comparison of the emissions of nine hazardous air pollutants from these two engines with emissions from nine other aircraft engines is discussed. 相似文献
747.
A.A. Karanasiou P.A. Siskos K. Eleftheriadis 《Atmospheric environment (Oxford, England : 1994)》2009,43(21):3385-3395
This study was conducted in order to investigate the differences observed in source profiles in the urban environment, when chemical composition parameters from different aerosol size fractions are subjected to factor analysis. Source apportionment was performed in an urban area where representative types of emission sources are present. PM10 and PM2 samples were collected within the Athens Metropolitan area and analysed for trace elements, inorganic ions and black carbon. Analysis by two-way and three-way Positive Matrix Factorization was performed, in order to resolve sources from data obtained for the fine and coarse aerosol fractions. A difference was observed: seven factors describe the best solution in PMF3 while six factors in PMF2. Six factors derived from PMF3 analysis correspond to those described by the PMF2 solution for the fine and coarse particles separately. These sources were attributed to road dust, marine aerosol, soil, motor vehicles, biomass burning, and oil combustion. The additional source resolved by PMF3 was attributed to a different type of road dust. Combustion sources (oil combustion and biomass burning) were correctly attributed by PMF3 solely to the fine fraction and the soil source to the coarse fraction. However, a motor vehicle's contribution to the coarse fraction was found only by three-way PMF. When PMF2 was employed in PM10 concentrations the optimum solution included six factors. Four source profiles corresponded to the previously identified as vehicles, road dust, biomass burning and marine aerosol, while two could not be clearly identified. Source apportionment by PMF2 analysis based solely on PM10 aerosol composition data, yielded unclear results, compared to results from PMF2 and PMF3 analyses on fine and coarse aerosol composition data. 相似文献
748.
Cora J. Young Michael D. Hurley Timothy J. Wallington Scott A. Mabury 《Atmospheric environment (Oxford, England : 1994)》2009,43(24):3717-3724
Relative rate techniques were used to determine k(Cl + CF3CFCFCF3) = (7.27 ± 0.88) × 10?12, k(Cl + CF3CF2CFCF2) = (1.79 ± 0.41) × 10?11, k(OH + CF3CFCFCF3) = (4.82 ± 1.15) × 10?13, and k(OH + CF3CF2CFCF2) = (1.94 ± 0.27) × 10?12 cm3 molecule?1 s?1 in 700 Torr of air or N2 diluent at 296 K. The chlorine atom- and OH radical-initiated oxidation of CF3CFCFCF3 in 700 Torr of air gives CF3C(O)F in molar yields of 196 ± 11 and 218 ± 20%, respectively. Chlorine atom-initiated oxidation of CF3CF2CFCF2 gives molar yields of 97 ± 9% CF3CF2C(O)F and 97 ± 9% COF2. OH radical-initiated oxidation of CF3CF2CFCF2 gives molar yields of 110 ± 15% CF3CF2C(O)F and 99 ± 8% COF2. The atmospheric fate of CF3CF2C(O)F and CF3C(O)F is hydrolysis to give CF3CF2C(O)OH and CF3C(O)OH. The atmospheric lifetimes of CF3CFCFCF3 and CF3CF2CFCF2 are determined by reaction with OH radicals and are approximately 24 and 6 days, respectively. The contribution of CF3CFCFCF3 and CF3CF2CFCF2 to radiative forcing of climate change will be negligible. 相似文献
749.
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
750.
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