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1.
The annual cycles of hydrogen peroxide (H2O2) and methylhydroperoxide (MHP) have been investigated at a remote site in Antarctica in order to study seasonal variations as well as chemical processes in the troposphere. The measurements have been performed from March 1997 to January 1998 and in February 1999 at the German Antarctic research station Neumayer which is located at 70°39′S, 8°15′W. The obtained time series for hydrogen peroxide and methylhydroperoxide in near-surface air represents the first all-year measurements in Antarctica and indicates clearly the occurrence of seasonal variations. During polar night mean values of 0.054±0.046 ppbv (range<0.03–0.11 ppbv) for hydrogen peroxide and 0.089±0.052 ppbv (range<0.05–0.14 ppbv) for methylhydroperoxide were detected. At the sunlit period higher Mixing ratios were found, 0.20±0.13 ppbv (range<0.03–0.91 ppbv) for hydrogen peroxide and 0.19±0.10 ppbv (range<0.05–0.89 ppbv) for methylhydroperoxide. Occasional long-range transport of air masses from mid-latitudes caused enhanced peroxide concentrations at polar night. During the period of stratospheric ozone depletion we observed peroxide mixing ratios comparable to typical winter levels.  相似文献   

2.
Six years (1998–2003) of measurements of ambient air concentrations of total suspended particulate (TSP) measured at a rural background monitoring station in Tenerife (Canary Islands), the El Río station (ER, 28°08′35″N, 16°39′20″W, 500 m a.s.l.) were studied. African dust outbreaks were objectively identified using a new quantitative tool, called the African Index. This index indicates the percentage of time that an air mass remained over an African region at one of three possible height intervals of the lower troposphere. After identifying these episodes, a study of the background TSP levels at the ER station and of direct and indirect (those which cause vertical deposition of dust) African air mass intrusion impacts was performed. Taking into account both direct and indirect episodes, a total of 322 days of African dust intrusion were objectively identified (a mean of 54 episodes per year) in the period 1998–2003, some of them caused by “transition episodes” or “return African air masses”. A subjective method confirmed that 256 of these days were caused by direct impacts of African dust on the ER station. A mean TSP value of 21.6 μg m−3 was found at the station during this period. All the episodes occurred when the TSP concentration was >28.5 μg m−3. The TSP background (14 μg m−3) can be assumed to be representative of the MBL of the Eastern North Atlantic subtropical region. The highest number of dust gravitational settlement (or indirect) episodes occurs in summer, but the highest contribution of these episodes to the TSP levels is in March with a monthly mean TSP contribution of up to 30.5 μg m−3.  相似文献   

3.
Asia is one of the major sources of not only mineral dust but also anthropogenic aerosols. Continental air masses associated with the East Asian winter monsoon always contain high contents of mineral dust and anthropogenic species and transported southeastward to Taiwan, which have significant influences on global atmospheric radiation transfer directly by scattering and absorbing solar radiation in each spring. However, few measurements for the long-range transported aerosol and its optical properties were announced in this area, between the Western Pacific and the southeastern coast of Mainland China. The overall objective of this work is to quantify the optical characteristics of different aerosol types in the Eastern Asian. In order to achieve this objective, meteorological parameters, concentrations of PM10 and its soluble species, and optical property of atmospheric scattering coefficients were measured continuously with 1 h time-resolved from 11 February to 7 April 2004 in Taipei Basin (25°00′N, 121°32′E). In this work, the dramatic changes of meteorological parameters such as temperature and winds were used to determine the influenced period of each air mass. Continental, strong continental, marine, and stagnant air masses defined by the back-trajectory analysis and local meteorology were further characterized as long-range transport pollution, dust, clean marine, and local pollution aerosols, respectively, according to the diagnostic ratios. The aerosol mass scattering efficiency of continental pollution, dust, clean marine, and local pollution aerosols were ranged from 1.3 to 1.6, 0.7 to 1.0, 1.4 and 1.4 to 2.3 m2 g−1, respectively. Overall, there are two distinct populations of aerosol mass scattering efficiencies, one for an aerosol chemical composition dominated by dust (<1.0 m2 g−1) and the other for an aerosol chemical composition dominated by anthropogenic pollutants (1.3–2.3 m2 g−1), which were similar to the previous measurements with high degree of temporal resolution.  相似文献   

4.
In this paper, the continuous (1994–2001) and discrete air sample (1991–2001) measurements of atmospheric CH4 from the Waliguan Baseline Observatory located in western China (36°17′N, 100°54′E, 3816 m asl) are presented and characterized. The CH4 time series show large episodic events on the order of 100 ppb throughout the year. During spring, a diurnal cycle with average amplitude of 7 ppb and a morning maximum and late afternoon minimum is observed. In winter, a diurnal cycle with average amplitude of 14 ppb is observed with an afternoon maximum and morning minimum. Unlike most terrestrial observational sites, no obvious diurnal patterns are present during the summer or autumn. A background data selection procedure was developed based on local horizontal and vertical winds. A selected hourly data set representative of “baseline” conditions was derived with approximately 50% of the valid hourly data. The range of CH4 mixing ratios, annual means, annual increases and mean annual cycle at Waliguan during the 1992–2001 were derived from discrete and continuous data representative of “baseline” conditions and compared to air samples collected at other Northern Hemisphere sites. The range of CH4 monthly means of 1746–1822 ppb, average annual means of 1786.7±10.8 ppb and mean annual increase of 4.5±4.2 ppb yr−1 at Waliguan were inline with measurements from sites located between 30° and 60°N. There were variations observed in the CH4 annual increase patterns at Waliguan that were slightly different from the global pattern. The mean CH4 annual cycle at Waliguan shows an unusual pattern of two gentle peaks in summer and February along with two small valleys in early winter and spring and a mean peak-to-peak amplitude of 11 ppb, much smaller than amplitudes observed at most other mid- and high-northern latitude sites. The Waliguan CH4 data are strongly influenced by continental Asian CH4 emissions and provide key information for global atmospheric CH4 models.  相似文献   

5.
The hexachlorocyclohexane-isomers (HCH), hexachlorobenzene (HCB), the polychlorinated biphenyls (PCB), 1,1,1-trichloro-2,2-bis(p-chlorophenyl)ethane (4,4′-DDT) and 1,1-dichloro-2,2-bis(p-chlorophenyl)ethene (4,4′-DDE) have been measured in urban and rural air around the city of Ulm (F. R. G., 48.4° N, 10.0° E). The sampling stations are typical for continental air in the westerlies of the northern hemisphere including local and regional influences. The analytical method consists of adsorptive sampling of large volumes (1000 m3) of air on silica gel, solvent desorption with CH2Cl2, preseparation of the collected chlorinated C6/C14 hydrocarbons by liquid adsorption chromatography on silica gel, and high resolution capillary gas chromatography with electron capture-(HRGC/ECD) or mass-selective detection (HRGC/MSD). The concentrations found in the lower troposphere under different meteorological conditions reflect regional input and long range transport. The levels found range from 1 pg/m3 for 4,4′-DDT to 10 ng/m3 for gamma HCH.  相似文献   

6.
The objective of this study is to investigate the air ventilation impacts of the so called “wall effect” caused by the alignment of high-rise buildings in complex building clusters. The research method employs the numerical algorithm of computational fluid dynamics (CFD – FLUENT) to simulate the steady-state wind field in a typical Hong Kong urban setting and investigate pollutant dispersion inside the street canyon utilizing a pollutant transport model. The model settings of validation study were accomplished by comparing the simulation wind field around a single building block to wind tunnel data. The results revealed that our model simulation is fairly close to the wind tunnel measurements. In this paper, a typical dense building distribution in Hong Kong with 2 incident wind directions (0° and 22.5°) is studied. Two performance indicators are used to quantify the air ventilation impacts, namely the velocity ratio (VR) and the retention time (Tr) of pollutants at the street level. The results indicated that the velocity ratio at 2 m above ground was reduced 40% and retention time of pollutants increased 80% inside the street canyon when high-rise buildings with 4 times height of the street canyon were aligned as a “wall” upstream. While this reduction of air ventilation was anticipated, the magnitude is significant and this result clearly has important implications for building and urban planning.  相似文献   

7.
A flux estimate of PCDDs and PCDFs through a waste water treatment plant has been made on an annual basis. The samples were collected from different steps in the treatment procedure within the plant i.e. inlet and outlet water, different sludge types and air samples. From the surroundings of the plant were collected samples of urban air, storm sewer water (urban runoff), plant discharge water and settling particulates from a sediment trap downstream the plant discharge. Differences in congener profiles were found between the samples taken within the plant compared to those collected outside. The flux of PCDD and PCDF equivalents through the plant was found to be approximately 0.4 – 0.5 g/year and the major part was taken away as digested sludge.  相似文献   

8.
Over the western North Pacific, a large amount of land aerosols from Asian-Pacific countries is transported by the prevailing westerlies. This transport makes the radiative characteristics of these aerosols diverse, particularly when one compares those characteristics over the coastal sea with those over the open sea. In this paper we discuss a method that uses satellite data to obtain the single-scattering albedo (ω) and asymmetry factor (g) of atmospheric aerosols for two large-scale subdivisions—the coastal sea (within 250 km from the coast) and the open sea (the remaining area)—over the western North Pacific (110°E–180°, 20°N–50°N). Our estimation method uses satellite measurements, obtained over a six-year period (2000–2005), of aerosol optical depth (AOD) and shortwave fluxes at both the surface and the top of the atmosphere (TOA); the measurements are obtained using the Moderate Resolution Imaging Spectroradiometer (MODIS) and the Clouds and the Earth's Radiant Energy System (CERES). For the two subdivisions, the estimated annual means of (ω,g) at 630 nm are significantly different: (0.94, 0.65) over the coastal sea and (0.97, 0.70) over the open sea. From a quantitative viewpoint, this result indicates that in comparison with aerosols over the open sea, those over the coastal sea show greater absorption and lesser forward scattering of solar radiation. The estimated optical properties are responsible for the aerosol surface cooling observed by MODIS and CERES, which is approximately 138 and 108 W m−2 per AOD over the coastal sea and open sea, respectively.  相似文献   

9.
Soil and atmospheric concentrations, dry deposition and soil-air gas exchange of organochlorine pesticides (OCPs) were investigated at an industrial site in Aliaga, Izmir, Turkey. Current-use pesticides, endosulfan and chlorpyrifos, had the highest atmospheric levels in summer and winter. Summertime total (gas + particle) OCP concentrations in air were higher, probably due to increased volatilization at higher temperatures and seasonal local/regional applications of current-use pesticides. Particle deposition fluxes were generally higher in summer than in winter. Overall average dry particle deposition velocity for all the OCPs was 4.9 ± 4.1 cm s−1 (average ± SD). ΣDDXs (sum of p,p′-DDT, p,p′-DDD, and p,p′-DDE) were the most abundant OCPs in Aliaga soils (= 48), probably due to their heavy historical use and persistence. Calculated fugacity ratios and average net gas fluxes across the soil-air interface indicated volatilization for α-CHL, γ-CHL, heptachlorepoxide, cis-nonachlor, trans-nonachlor, and p,p′-DDT in summer, and for α-CHL, γ-CHL, trans-nonachlor, endosulfan sulfate, and p,p′-DDT in winter. For the remaining OCPs, soil acted as a sink during both seasons. Comparison of the determined fluxes showed that dry particle, gas-phase, and wet deposition are significant OCP input mechanisms to the soil in the study area.  相似文献   

10.
Subsurface solute transport through structured soil is studied by model interpretation of experimental breakthrough curves from tritium and phosphorus tracer tests in three intact soil monoliths. Similar geochemical conditions, with nearly neutral pH, were maintained in all the experiments. Observed transport differences for the same tracer are thus mainly due to differences in the physical transport process between the different monoliths. The modelling is based on a probabilistic Lagrangian approach that decouples physical and chemical mass transfer and transformation processes from pure and stochastic advection. Thereby, it enables explicit quantification of the physical transport process through preferential flow paths, honouring all independently available experimental information. Modelling of the tritium breakthrough curves yields a probability density function of non-reactive solute travel time that is coupled with a reaction model for linear, non-equilibrium sorption–desorption to describe the phosphorus transport. The tritium model results indicate that significant preferential flow occurs in all the experimental soil monoliths, ranging from 60–100% of the total water flow moving through only 25–40% of the total water content. In agreement with the fact that geochemical conditions were similar in all experiments, phosphorus model results yield consistent first-order kinetic parameter values for the sorption–desorption process in two of the three soil monoliths; phosphorus transport through the third monolith cannot be modelled because the apparent mean transport rate of phosphorus is anomalously rapid relative to the non-adsorptive tritium transport. The occurrence of preferential flow alters the whole shape of the phosphorus breakthrough curve, not least the peak mass flux and concentration values, and increases the transported phosphorus mass by 2–3 times relative to the estimated mass transport without preferential flow in the two modelled monoliths.  相似文献   

11.
A highly resolved temporal and spatial Pearl River Delta (PRD) regional emission inventory for the year 2006 was developed with the use of best available domestic emission factors and activity data. The inventory covers major emission sources in the region and a bottom–up approach was adopted to compile the inventory for those sources where possible. The results show that the estimates for SO2, NOx, CO, PM10, PM2.5 and VOC emissions in the PRD region for the year 2006 are 711.4 kt, 891.9 kt, 3840.6 kt, 418.4 kt, 204.6 kt, and 1180.1 kt, respectively. About 91.4% of SO2 emissions were from power plant and industrial sources, and 87.2% of NOx emissions were from power plant and mobile sources. The industrial, mobile and power plant sources are major contributors to PM10 and PM2.5 emissions, accounting for 97.7% of the total PM10 and 97.2% of PM2.5 emissions, respectively. Mobile, biogenic and VOC product-related sources are responsible for 90.5% of the total VOC emissions. The emissions are spatially allocated onto grid cells with a resolution of 3 km × 3 km, showing that anthropogenic air pollutant emissions are mainly distributed over PRD central-southern city cluster areas. The preliminary temporal profiles were established for the power plant, industrial and on-road mobile sources. There is relatively low uncertainty in SO2 emission estimates with a range of −16% to +21% from power plant sources, medium to high uncertainty for the NOx emissions, and high uncertainties in the VOC, PM2.5, PM10 and CO emissions.  相似文献   

12.
Groundwater nitrification is a poorly characterized process affecting the speciation and transport of nitrogen. Cores from two sites in a plume of contamination were examined using culture-based and molecular techniques targeting nitrification processes. The first site, located beneath a sewage effluent infiltration bed, received treated effluent containing O2 (> 300 µM) and NH4+ (51–800 µM). The second site was 2.5 km down-gradient near the leading edge of the ammonium zone within the contaminant plume and featured vertical gradients of O2, NH4+, and NO3 (0–300, 0–500, and 100–200 µM with depth, respectively). Ammonia- and nitrite-oxidizers enumerated by the culture-based MPN method were low in abundance at both sites (1.8 to 350 g− 1 and 33 to 35,000 g− 1, respectively). Potential nitrifying activity measured in core material in the laboratory was also very low, requiring several weeks for products to accumulate. Molecular analysis of aquifer DNA (nested PCR followed by cloning and 16S rDNA sequencing) detected primarily sequences associated with the Nitrosospira genus throughout the cores at the down-gradient site and a smaller proportion from the Nitrosomonas genus in the deeper anoxic, NH4+ zone at the down-gradient site. Only a single Nitrosospira sequence was detected beneath the infiltration bed. Furthermore, the majority of Nitrosospira-associated sequences represent an unrecognized cluster. We conclude that an uncharacterized group associated with Nitrosospira dominate at the geochemically stable, down-gradient site, but found little evidence for Betaproteobacteria nitrifiers beneath the infiltration beds where geochemical conditions were more variable.  相似文献   

13.
Accumulation and release kinetics from azalea leaves exposed at vapours of (γ- and γ-HCH, p,p′-DDT and DDE, and a PCB mixture (Fenclor 64) are reported. The use of plant foliage as an air contamination indicator is discussed.  相似文献   

14.
We used a dispersion model to analyze measurements made during a field study conducted by the U.S. EPA in July–August 2006, to estimate the impact of traffic emissions on air quality at distances of tens of meters from an eight-lane highway located in Raleigh, NC. The air quality measurements consisted of long path optical measurements of NO at distances of 7 and 17 m from the edge of the highway. Sonic anemometers were used to measure wind speed and turbulent velocities at 6 and 20 m from the highway. Traffic flow rates were monitored using traffic surveillance cameras. The dispersion model [Venkatram, A., 2004. On estimating emissions through horizontal fluxes. Atmospheric Environment 38, 2439–2446] explained over 60% of the variance of the observed path averaged NO concentrations, and over 90% of the observed concentrations were within a factor of two of the model estimates.Sensitivity tests conducted with the model indicated that the traffic flow rate made the largest contribution to the variance of the observed NO concentrations. The meteorological variable that had the largest impact on the near road NO concentrations was the standard deviation of the vertical velocity fluctuations, σw. Wind speed had a relatively minor effect on concentrations. Furthermore, as long as the wind direction was within ±45° from the normal to the road, wind direction had little impact on near road concentrations. The measurements did not allow us to draw conclusions on the impact of traffic-induced turbulence on dispersion. The analysis of air quality and meteorological observations resulted in plausible estimates of on-road emission factors for NO.  相似文献   

15.
Successions of lake ecosystems from clear-water, macrophyte-rich conditions into turbid states with abundant phytoplankton have taken place in many shallow lakes in China. However, little is know about the change of carbon fluxes in lakes during such processes. We conducted a case study in Lake Biandantang to investigate the change of carbon fluxes during such a regime shift. Dissolved aquatic carbon and gaseous carbon (methane (CH4) and carbon dioxide (CO2)) across air–water interface in three sites with different vegetation covers and compositions were studied and compared. CH4 emissions from three sites were 0.62±0.36, 0.70±0.36, and 1.31±0.57 mg m−2 h−1, respectively. Correlation analysis showed that macrophytes, rather than phytoplankton, directly positively affected CH4 emission. CO2 fluxes of three sites in Lake Biandantang were significantly different, and the average values were 77.8±20.4, 52.2±14.1 and 3.6±26.8 mg m−2 h−1, respectively. There were an evident trend that the larger macrophyte biomass, the lower CO2 emissions. Correlation analysis showed that in different sites, dominant plant controlled CO2 flux across air–water interface. In a year cycle, the percents of gaseous carbon release from lake accounting for net primary production were significantly different (from 39.3% to 2.8%), indicating that with the decline of macrophytes and regime shift, the lake will be a larger carbon source to the atmosphere.  相似文献   

16.
ABSTRACT

A study was conducted to estimate the changes in wintertime visual air quality in Dallas-Fort Worth (DFW) that might occur due to proposed reductions in SO2 emissions at two steam electric generating plants in eastern Texas, each over 100 km from the city. To provide information for designing subsequent investigations, the haze was characterized broadly during the first year of the study. Meteorological data acquired then demonstrated that, during haze episodes, emissions from only one of the two plants were likely to be transported directly to DFW. Therefore, the second year of the study was centered on just one of the power plants. Air quality was then characterized within the urban area and at rural locations that would be upwind and downwind of the plant during transport to DFW. An instrumented aircraft measured plume dispersion and the air surrounding the plume on selected days. A mathematical model was used to predict the change that would occur in airborne particulate matter concentrations in DFW if SO2 emissions were reduced to reflect the proposed limitations. The contribution of particles in the atmosphere to light extinction was estimated, and simulated photographs were produced to illustrate the visibility changes. The study concluded that the proposed emission reductions would, at most, subtly change perceived wintertime visibility.  相似文献   

17.
A study was conducted to estimate the changes in wintertime visual air quality in Dallas-Fort Worth (DFW) that might occur due to proposed reductions in SO2 emissions at two steam electric generating plants in eastern Texas, each over 100 km from the city. To provide information for designing subsequent investigations, the haze was characterized broadly during the first year of the study. Meteorological data acquired then demonstrated that, during haze episodes, emissions from only one of the two plants were likely to be transported directly to DFW. Therefore, the second year of the study was centered on just one of the power plants. Air quality was then characterized within the urban area and at rural locations that would be upwind and downwind of the plant during transport to DFW. An instrumented aircraft measured plume dispersion and the air surrounding the plume on selected days. A mathematical model was used to predict the change that would occur in airborne particulate matter concentrations in DFW if SO2 emissions were reduced to reflect the proposed limitations. The contribution of particles in the atmosphere to light extinction was estimated, and simulated photographs were produced to illustrate the visibility changes. The study concluded that the proposed emission reductions would, at most, subtly change perceived wintertime visibility.  相似文献   

18.
Thermal venting is a remediation technique suitable to the liquid unsaturated zone to enhance recovery of less-volatile residual hydrocarbon contaminants. Thermal venting is different to traditional soil venting because heated air instead of air at ambient conditions is applied to the contaminated zone. The vapor pressure of a less-volatile contaminants is typically increased by temperature causing the gas-phase concentrations to increase by three- to five-fold over a temperature increase of 20–30°C. The work described in this first paper provides the theoretical framework of analysis related to thermal venting. The analysis included nonisothermal gas flow, thermal energy transport and multicomponent mass transport in a multiphase porous medium. The transient gas flow analysis included the effect of temperature on fluid properties and gas compressibility. The heat energy transport analysis was performed under the thermodynamic equilibrium condition with phase-summed effective thermal properties. Multi-component mass transport was performed under local equilibrium for partitioning between phases. Model verification was performed to the extend possible using analytical and available experimental data for different physical processes. The second paper of this two-part series will demonstrate the applicability of thermal venting technique through numerical simulations of hypothetical laboratory and field-scale scenarios.  相似文献   

19.
The use of the oxygenate methyl tert-butyl ether (MTBE) in gasoline has led to detectable concentrations in urban and rural air up to 160 ppbV. Results from MTBE measurement in precipitation have not been reported so far. In the present study, 120 samples of precipitation collected at 17 sampling locations all over Germany have been analyzed for their MTBE content. Analysis is performed by a combination of headspace-solid-phase microextraction (HS-SPME) and gas chromatography/mass spectrometry (GC-MS). A 75 μm poly(dimethylsiloxane)/Carboxene fiber and a cryostat is used for SPME. The detection limit is 10 ng/l. In precipitation samples, MTBE was detected in wintertimes only with a maximum concentration of 85 ng/l. Measurement at Frankfurt/M City from 6 September 2000 to 12 March 2001 provided for 49% of the data concentrations in the range of 30–85 ng/l (n=17). Sampling in winter 2000/2001 at several German cities and rural locations showed that MTBE is more often detectable in urban (86%, n=78) than in rural (18%, n=42) precipitation. By comparing the results with corresponding temperatures and amounts of precipitation it can be concluded that the detection of MTBE in urban precipitation is observed at ambient temperatures lower than about 10–15°C. Moreover, the first precipitation after a dry period accumulates more MTBE than precipitation during or at the end of a wet period (wash-out effect). Highest concentrations occurred in snow samples. Corresponding mean air equilibrium concentrations of 0.04 ppbV (urban samples) and 0.01 ppbV (rural samples) are calculated. This is about one magnitude lower than year round and summertime measurements in the US and in Switzerland. Urban runoff (n=12) and corresponding precipitation sampling indicate that urban runoff might be composed of about 20% MTBE that is already transported by air and precipitation, whereas about 80% may be attributed to direct uptake of vehicle emissions and leakage near the road during precipitation.  相似文献   

20.
The 5-day forward and backward trajectories of air mass transport to three Russian Arctic points for each day in April and July over a 10-year period from 1986 to 1995 have been analyzed. The important features and seasonal differences in air exchange processes in various areas of the Arctic have been investigated. Taking into account seasonal variations in aerosol scavenging mechanisms and velocities, the average contributions of large highly industrialized regions of the Russian Arctic air pollution were estimated for April and July. Reasonable correspondence between the calculated mean concentrations for six anthropogenic chemical elements (As, Ni, Pb, V, Zn, Cd) and experimentally determined values have been obtained. The atmospheric pollution transport from the Arctic was studied as yet another way of cleaning the Arctic atmosphere, in addition to the traditionally considered wet and dry depositions onto the surface. The average apportionment of conservative contaminants after passing the observation points was estimated for spring and summer. The air masses passing through the observation points in spring may take about 20–40% of pollutants out of the Arctic. In summer, however, more than 90% of pollutants transported into the Russian Arctic deposit within 5 days onto the surface inside the Arctic region. The monthly average fluxes of six anthropogenic elements onto the surface in the Russian Arctic were estimated for April and July.  相似文献   

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