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1.
The present work summarises the results of a 2‐year study of wet‐only sequential deposition in 2 rural areas (Alcan¯iz and Morella) located at different distances from a large coal‐fired power station. Precipitation chemistry was characterised by relatively high , Ca2+ and average concentrations. Sequential study of single precipitation events showed that concentrations of most of the ions studied decreased exponentially throughout single precipitation events, with a sharper decrease in concentrations at the beginning of the event. Usually, 40 to 80% of the wet‐only deposition of major ions occurred in the first 2 mm. pH measurements, ranging from 5.6 to 8.1, showed a decrease in the pH values throughout a precipitation event. Deposition levels of Ca2+ and accounted for the neutralisation of major acidic species in the precipitation events except in 5 rain episodes sampled at Morella. The sequential study of the evolution of the ratio during a single precipitation allowed us to identify potential acidic rainfall fractions after an initial volume of precipitation, after most of the Ca2+ in atmospheric particles had been scavenged. A higher neutralisation capacity was deduced for Alcan¯iz owing to the higher atmospheric levels of natural carbonates and .  相似文献   

2.
Deposition of atmospheric particulate PCBs in suburban site of Turkey   总被引:2,自引:1,他引:2  
Dry deposition and air concentration samples were collected from July 2004 to May 2005 at a suburban site in Turkey. A water surface sampler (WSS) was used to measure directly the dry deposition flux of particulate polychlorinated biphenyls (PCBs) while a high volume air sampler (HVAS) was employed to collect air samples. Particulate PCB concentrations accounted for 15% of total PCBs (gas + particle phase) at the site. The overall particulate phase PCB flux ranged from 2 to 160 ng m− 2 d− 1 with an average of 46.3 ± 40.6 ng m− 2 d− 1. Forty one PCB congeners were targeted in the samples while twenty one congeners were found to be higher than detection limits in deposition samples. Fluxes for homolog groups ranged between 0.9 (7-CBs) and 21.0 (3-CBs) ng m− 2 d− 1. Measured dry deposition fluxes were lower than the ones usually reported for urban sites. Average PCB dry deposition velocity, calculated using flux values and concurrently measured atmospheric concentrations, was 1.26 ± 1.86 cm s− 1 depended on size distribution of particles, atmospheric PCB concentrations and meteorological conditions.  相似文献   

3.
Polychlorinated biphenyls (PCBs) as Σ21 congeners, were investigated in atmospheric bulk deposition over one year, along a northern transect of France, including 5 sites from the Atlantic coast to the east of Paris. Evidence was obtained for an easterly rise of the PCB concentrations, from 3 to 76 ng L−1. The PCB patterns were depleted in low chlorinated congeners in rural areas whereas at urban sites, the profiles were typical of local sources. The seasonal variations of concentrations were mainly controlled by the temperature. Next, at Paris, PCB distribution between the gaseous and the particulate phases was studied, considering seasonal parameters and different fate processes. Their distribution showed a prevalence of congeners in the gaseous phase (0.15–1.17 ng m−3) which occurrence decreased from 93 to 68% with the rise of congener chlorination level. In the particulate phase, they ranged from 0.01 to 0.27 ng m−3, only. Rainwater concentrations ranged from 3.1 to 13.1 ng L−1. A total rain water/air washout ratio was determined and showed a negative correlation with those reported in the literature. That might be attributed to the importance of particle scavenging. The annual bulk deposition ranged from 8 to 29 μg m−2. A decreasing trend of PCB atmospheric levels over the last fifteen years was confirmed in the studied area.  相似文献   

4.
Gas and particle phase concentrations of atmospheric polychlorinated biphenyls (PCBs) were measured at an urban/industrial site in the city of Bursa, Turkey. PCB concentration levels were presented between July 2004 and May 2005. Average particle and gas phase concentrations of individual PCB congeners ranged from 0.08 (PCB-183) to 6.86 (PCB-49) pg m− 3 and from 0.01 (PCB-209) to 47.2 (PCB-33) pg m− 3, respectively. The mean concentration of total (gas + particle) PCBs varied between 24.27 and 666.21 pg m− 3 with an average of 287.27 ± 174.80 pg m− 3. PCB concentrations at the sampling site were higher than the concentrations reported at non-urban sites. PCBs partitioned between gas and particle phases and the partitioning was examined according to different approaches such as logKp–logPLo, logKp–logKOA and the Junge–Pankow model. In order to present possible interactions, a correlation matrix based on PCB congeners and meteorological parameters was constructed. Application of the Clausius–Clapeyron equation yielded a low slope value indicating possible emissions from local and regional sources originating mainly from urban/industrial areas, landfill and waste incineration plant. Then, likely dry deposition fluxes were estimated depending on reported dry deposition velocity and atmospheric concentration values.  相似文献   

5.
The second Aerosol Characterisation Experiment (ACE‐2) was aimed at investigating the physical, chemical and radiative properties of aerosol and their evolution in the North Atlantic region. In the 2nd "Lagrangian" experiment, an air mass was tracked over a 30‐h period during conditions of extensive stratocumulus cover. Boundary‐layer measurements of the aerosol size distribution obtained with a passive cavity aerosol spectrometer probe (PCASP) during the experiment show a gradual growth in size of particles in the 0.1–0.2 μm diameter mode. Simultaneously, SO2 concentrations were found to decrease sharply from 800 to 20 ppt. The fraction of sulphate in aerosol ionic mass increased from 0.68±0.07 to 0.82±0.09 for small particles (diameter below 1.7 μm) and from 0.21±0.04 to 0.34±0.03 for large particles (diameter above 1.7 μm). The measurements were compared with a multicyclic parcel model of gas phase diffusion into cloud droplets and aqueous phase chemical reactions. The model was able to broadly reproduce the observed transformation in the aerosol spectra and the timescale for the transformation of SO2 to sulphate aerosol. The modelled SO2 concentration in the boundary layer fell to below half its initial value over a 6.5‐h time period due to a combination of the entrainment of cleaner tropospheric air and cloud chemical reactions. NH3 and HCl gas were also found to play an important rôle in cloud processing in the model.  相似文献   

6.
A 3rd‐generation smart balloon designed at National Oceanic and Atmospheric Administration, Air Resources Laboratory Field Research Division, in collaboration with the University of Hawaii, was released from ship‐board during the recent Second Aerosol Characterization Experiment (ACE‐2) to provide Lagrangian air‐mass tracking data. ACE‐2 is the 3rd in a series of field experiments designed to study the chemical, physical, and radiative properties and processes of atmospheric aerosols and their role in climate and is organized by the international global atmospheric chemistry (IGAC) program. The adjective smart in the title of this paper refers to the fact that the buoyancy of the balloon automatically adjusts through the act of pumping air into or releasing air from the ballast portion of the balloon when it travels vertically outside a barometric pressure range set prior to release. The smart balloon design provides GPS location, barometric pressure, temperature, relative humidity, and other data via a transponder to a C130 research aircraft flying in the vicinity of the balloon. The addition of 2‐way communication allows interactive control of the balloon operating parameters by an observer. A total of 3 cloudy Lagrangian experiments were conducted during the ACE‐2 field program which lasted from 16 June through 26 July 1997. This paper reviews the design and capability of the smart balloons and their performance during the ACE‐2 Lagrangian experiments. Future development and applications of the technology are discussed.  相似文献   

7.
We report on clear‐sky column closure experiments (CLEARCOLUMN) performed in the Canary Islands during the second Aerosol Characterization Experiment (ACE‐2) in June/July 1997. We present CLEARCOLUMN results obtained by combining airborne sunphotometer and in‐situ (optical particle counter, nephelometer, and absorption photometer) measurements taken aboard the Pelican aircraft, space‐borne NOAA/AVHRR data and ground‐based lidar and sunphotometer measurements. During both days discussed here, vertical profiles flown in cloud‐free air masses revealed 3 distinctly different layers: a marine boundary layer (MBL) with varying pollution levels, an elevated dust layer, and a very clean layer between the MBL and the dust layer. A key result of this study is the achievement of closure between extinction or layer aerosol optical depth (AOD) computed from continuous in‐situ aerosol size‐distributions and composition and those measured with the airborne sunphotometer. In the dust, the agreement in layer AOD (λ=380–1060 nm) is 3–8%. In the MBL there is a tendency for the in‐situ results to be slightly lower than the sunphotometer measurements (10–17% at λ=525 nm), but these differences are within the combined error bars of the measurements and computations.  相似文献   

8.
Multiple‐angle micro‐pulse lidar (MPL) observations were made at Las Galletas on Tenerife, Canary Islands during the Aerosol Characterization Experiment‐2 (ACE‐2) conducted June–July, 1997. A principal objective of the MPL observations was to characterize the temporal/spatial distributions of aerosols in the region, particularly to identify and profile elevated Saharan dust layers which occur intermittently during the June–July time period. Vertical and slant angle measurements taken 16 and 17 July characterize such an occurrence, providing aerosol backscatter, extinction, and optical depth profiles of the dust layer between 1 and 5 km above mean sea level (MSL). Additionally, horizontal measurements taken in Las Galletas throughout the 6‐week period provide a time profile of the varying aerosol extinction at the surface. This profile exhibits the alternating periods of clean maritime air and pollution outbreaks that typified the region. Horizontal measurements also provide some evidence suggesting the possible influx of Saharan dust from the free troposphere to the surface. This paper presents estimates of aerosol optical properties retrieved from the multi‐angle MPL measurements in addition to an outline of the methodologies employed to obtain these results.  相似文献   

9.
Mass concentrations of total, organic and black carbon were derived by analyzing the supermicron and submicron aerosol fractions of shipboard collected samples in the easternAtlantic Ocean as part of the second Aerosol Characterization Experiment (ACE‐2). These analyses were complemented by experiments intended to estimate the water‐soluble fraction of the submicron carbonaceous material. Our results can be summarized as follows. Depending on the sample, between 35% and 80% of total aerosol carbon is associated with the submicron fraction. Total submicron carbon was well correlated with black carbon, a unique tracer for incomplete combustion. These correlations and the approximately constant total to black carbon ratios, suggest that the majority of submicron total carbon is of primary combustion derived origin. No systematic relationship between total submicron aerosol carbon and sulfate concentrations was found. Sulfate concentrations were, with a few exceptions, significantly higher than total carbon. Our experiments have demonstrated that water exposure removed between 36% and 72% of total carbon from the front filter, suggesting that a substantial fraction of the total submicron aerosol organic carbon is water‐soluble. An unexpected result of this study is that water exposure of filter samples caused substantial removal of, nominally insoluble, submicron black carbon. Possible reasons for this observation are discussed.  相似文献   

10.
The POLDER instrument is devoted to global observations of the solar radiation reflected by the Earth–atmosphere system. The airborne version of the instrument was operated during the ACE‐2 experiment, more particularly as a component of the CLOUDYCOLUMN project of ACE‐2 that was conducted in summer 1997 over the subtropical northeastern Atlantic ocean. CLOUDYCOLUMN is a coordinated project specifically dedicated to the study of the indirect effect of aerosols. In this context, the airborne POLDER was assigned to remote measurements of the cloud optical and radiative properties, namely the cloud optical thickness and the cloud albedo. This paper presents the retrievals of those 2 cloud parameters for 2 golden days of the campaign 26 June and 9 July 1997. Coincident spaceborne ADEOS‐POLDER data from 2 orbits over the ACE‐2 area on 26 June are also analyzed. 26 June corresponds to a pure air marine case and 9 July is a polluted air case. The multidirectional viewing capability of airborne POLDER is here demonstrated to be very useful to estimate the effective radius of cloud droplet that characterizes the observed stratocumulus clouds. A 12 μm cloud droplet size distribution appears to be a suitable cloud droplet model in the pure marine cloud case study. For the polluted case the mean retrieved effective droplet radius is of the order of 6–10 μm. This only preliminary result can be interpreted as a confirmation of the indirect effect of aerosols. It is consistent with the significant increase in droplet concentration measured in polluted marine clouds compared to clean marine ones. Further investigations and comparisons to in‐situ microphysical measurements are now needed.  相似文献   

11.
During the ACE‐2 field campaign in the summer of 1997 an intensive, ground‐based physical and chemical characterisation of the clean marine and continentally polluted aerosol was performed at Sagres, Portugal. Number size distributions of the dry aerosol in the size range 3–10 000 nm were continuously measured using DMPS and APS systems. Impactor samples were regularly taken at 60% relative humidity (RH) to obtain mass size distributions by weighing the impactor foils, and to derive a chemical mass balance by ion and carbon analysis. Hygroscopic growth factors of the metastable aerosol at 60% RH were determined to estimate the number size distribution at a relative humidity of 60%. A size segregated 3‐way mass closure study was performed in this investigation for the first time. Mass size distributions at 60% RH derived from number size distribution measurements and impactors samples (weighing and chemical analysis) are compared. A good agreement was found for the comparison of total gravimetrically‐determined mass with both number distribution‐derived (slope=1.23/1.09; R2>0.97; depending on the parameters humidity growth and density) and chemical mass concentration (slope=1.02; R2= 0.79) for particles smaller than 3 μm in diameter. Except for the smallest impactor size range relatively good correlations (slope=0.86–1.42) with small deviations (R2=0.76–0.98) for the different size fractions were found. Since uncertainties in each of the 3 methods are about 20% the observed differences in the size‐segregated mass fractions can be explained by the measurement uncertainties. However, the number distribution‐derived mass is mostly higher than the chemically and gravimetrically determined mass, which can be explained by sampling losses of the impactor, but as well with measurement uncertainties as, e.g., the sizing of the DMPS/APS.  相似文献   

12.
In‐situ aerosol measurements were performed in the northern hemispheric stratosphere up to altitudes of 21 km between 13 November 1996 and 14 January 1997, inside and outside of the polar vortex during the Airborne Polar Experiment (APE) field campaign. These are measurements of particle size distributions with a laser optical particle counter of the FSSP‐300 type operated during 9 flights on the Russian M‐55 high‐altitude research aircraft Geophysika. For specific flights, the FSSP‐300 measurements are compared with balloon‐borne data (launched from Kiruna, Sweden). It was found that the stratospheric aerosol content reached levels well below the background concentrations measured by the NASA operated ER‐2 in 1988/89 in the northern hemisphere. During the APE campaign, no PSC particle formation was observed at flight altitudes although the temperatures were below the NAT condensation point during one flight. The measured correlations between ozone and aerosol give an indication of the subsidence inside the 1996/97 polar vortex. Despite the lower aerosol content in the winter 1996/97 compared to the 1989 background, the heterogeneous reactivity of the aerosol (as calculated from the measured data with additional model input) is comparable. This is due to the dependency of the reactive uptake coefficients on the atmospheric water vapor content. Under the described assumptions the reaction rates on the background aerosol are significantly smaller than for competing gas phase chlorine activation, as can be expected for stratospheric background conditions especially inside the polar vortex.  相似文献   

13.
Polycyclic aromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs) were determined in urban air samples of Konya, Turkey between August 2006 and May 2007. The concentrations of pollutants in both the gas and particulate phase were separately analysed. The average total (gas + particulate) concentrations of PAHs, PCBs and OCPs were determined as 206 ng m− 3, 0.106 ng m− 3, 4.78 ng m− 3 respectively. All of the investigated target compounds were dominantly found in the gas phase except OCPs. Higher air concentrations of PAHs were found at winter season while the highest concentrations of PCBs were determined in September. The highest OCPs were detected in October and in March. In urban air of Konya, PCB 28 and PCB 52 congeners represent 46% and 35% of total PCBs while Phenanthrene, Fluoranthene, Pyrene accounted for 29%, 13%, 10% of total PAHs. HCH compounds (α + β + γ + δ-HCH), total DDTs (p,p′-DDE, p,p′-DDD, p,p′-DDT), Endosulfan compounds (Endosulfan I, Endosulfan II, Endosulfan sulfate) were dominantly determined as 30%, 21%, 20% of total OCPs respectively. Considering the relation between these compounds with temperature, there was no significant correlation observed. Despite banned/restricted use in Turkey, some OCPs were determined in urban air. These results demonstrated that they are either illegally being used in the course of agricultural activity and gardens in Konya or they are residues of past use in environment. According to these results, it can be suggested that Konya is an actively contributing region to persistent organic pollutants in Turkey.  相似文献   

14.
Analysis of the aerosol properties during 3 recent international field campaigns (ACE‐1, TARFOX and ACE‐2) are described using satellite retrievals from NOAA AVHRR data. Validation of the satellite retrieval procedure is performed with airborne, shipboard, and land‐based sunphotometry during ACE‐2. The intercomparison between satellite and surface optical depths has a correlation coefficient of 0.93 for 630 nm wavelength and 0.92 for 860 nm wavelength. The standard error of estimate is 0.025 for 630 nm wavelength and 0.023 for 860 nm wavelength. Regional aerosol properties are examined in composite analysis of aerosol optical properties from the ACE‐1, TARFOX and ACE‐2 regions. ACE‐1 and ACE‐2 regions have strong modes in the distribution of optical depth around 0.1, but the ACE‐2 tails toward higher values yielding an average of 0.16 consistent with pollution and dust aerosol intrusions. The TARFOX region has a noticeable mode of 0.2, but has significant spread of aerosol optical depth values consistent with the varied continental aerosol constituents off the eastern North American Coast.  相似文献   

15.
Aircraft measurements are presented of the Lagrangian evolution of a marine boundary layer over a 30‐h period during the ACE‐2 field campaign. At the start of the observational period, a 500‐m deep polluted marine internal boundary layer (MIBL) was overlain by the remnants of a polluted continental boundary layer extending to around 2 km below a clean, dry free troposphere. The MIBL grew rapidly to a thickness of 900–1000 m in response to increasing sea surface temperatures. No significant aerosol spectral evolution was observed in the boundary layer. Low concentrations of SO2 were observed in the MIBL suggesting that the air mass contained relatively aged aerosol. Aerosol spectra show a broad mode with a modal diameter of around 0.1μm. The polluted layer between the MIBL and the unpolluted free troposphere was only weakly and intermittently turbulent which prevented significant entrainment of clean air into the polluted layer from aloft. The polluted layer depth was thus controlled mainly by subsidence which as a result becomes shallower, decreasing from over 2000 m to around 1200 m during the observational period. The aerosol characteristics of the polluted layer were similar to those in the MIBL and so although the MIBL entrained considerable amounts of air from above the MIBL the aerosol characteristics underwent no significant change. This has important implications for the rate at which a polluted continental air mass is converted to a clean marine one. The dataset should prove useful in the validation of the modelling of continental pollution outbreaks.  相似文献   

16.
Microphysical measurements performed during 8 flights of the CLOUDYCOLUMN component of ACE‐2, with the Meteo‐France Merlin‐IV, are analyzed in terms of droplet number concentration and size. The droplet concentration is dependent upon the aerosol properties within the boundary layer. Its mean value over a flight varies from 55 cm−3, for the cleanest conditions, to 244 cm−3, for the most polluted one. For each flight, the variability of the concentration, in selected cloud regions that are not affected by mixing with dry air or drizzle scavenging, ranges from 0.5 to 1.5 of the mean value. The mean volume diameter increases with altitude above cloud base according to the adiabatic cloud model. The frequency distribution of mean droplet volume normalized by the adiabatic value, for the selected regions, shows the same dispersion as the distribution of normalized concentration. The values of droplet concentration versus mean volume diameter are then examined in sub‐adiabatic samples to characterize the effects of mixing and drizzle scavenging. Finally, the ratio of mean volume diameter to effective diameter is analyzed and a simple relationship between these 2 crucial parameters is proposed.  相似文献   

17.
Wet‐only rainwater composition, acid‐precursor gas mixing ratios and aerosol loading were determined from weekly‐averaged samples at Petaling Jaya, Malaysia, over the five year period from March 1993 to March 1998. Annual deposition fluxes of acidic sulfur and nitrogen species estimated from these data show this site to be heavily impacted by acidic deposition, with total oxidised sulfur plus nitrogen deposition in the range 277–480 meq m−2 yr−1. Average contributions were 56% as sulfur species, 44% as nitrogen species, with wet deposition in this region of high rainfall accounting for 67% of total deposition. Thus total acid deposition fluxes were equivalent to levels that provided motivation for emissions reduction programs in both Europe and North America. The possibility of adverse environmental effects in Malaysia caused by acid deposition therefore merits serious consideration and assessment.  相似文献   

18.
During the 1st Lagrangian experiment of the North Atlantic Regional Aerosol Characterisation Experiment (ACE‐2), a parcel of air was tagged by releasing a smart, constant level balloon into it from the Research Vessel Vodyanitskiy . The Meteorological Research Flight's C‐130 aircraft then followed this parcel over a period of 30 h characterising the marine boundary layer (MBL), the cloud and the physical and chemical aerosol evolution. The air mass had originated over the northern North Atlantic and thus was clean and had low aerosol concentrations. At the beginning of the experiment the MBL was over 1500 m deep and made up of a surface mixed layer (SML) underlying a layer containing cloud beneath a subsidence inversion. Subsidence in the free troposphere caused the depth of the MBL to almost halve during the experiment and, after 26 h, the MBL became well mixed throughout its whole depth. Salt particle mass in the MBL increased as the surface wind speed increased from 8 m s−1 to 16 m s−1 and the accumulation mode (0.1μm to 3.0 μm) aerosol concentrations quadrupled from 50 cm−3 to 200 cm−3. However, at the same time the total condensation nuclei (>3 nm) decreased from over 1000 cm−3 to 750 cm−3. The changes in the accumulation mode aerosol concentrations had a significant effect on the observed cloud microphysics. Observational evidence suggests that the important processes in controlling the Aitken mode concentration which, dominated the total CN concentration, included, scavenging of interstitial aerosol by cloud droplets, enhanced coagulation of Aitken mode aerosol and accumulation mode aerosol due to the increased sea salt aerosol surface area, and dilution of the MBL by free tropospheric air.  相似文献   

19.
A micro‐pulse lidar system (MPL) was used to measure the vertical and horizontal distribution of aerosols during the Aerosol Characterization Experiment 2 (ACE‐2) in June and July of 1997. The MPL measurements were made at the Izaña observatory (IZO), a weather station located on a mountain ridge (28°18' N, 16°30' W, 2367 m asl) near the center of the island of Tenerife, Canary Islands. The MPL was used to acquire aerosol backscatter, extinction, and optical depth profiles for normal background periods and periods influenced by Saharan dust from North Africa. System tests and calibration procedures are discussed, and an analysis of aerosol optical profiles acquired during ACE‐2 is presented. MPL data taken during normal IZO conditions (no dust) showed that upslope aerosols appeared during the day and dissipated at night and that the layers were mostly confined to altitudes a few hundred meters above IZO. MPL data taken during a Saharan dust episode on 17 July showed that peak aerosol extinction values were an order of magnitude greater than molecular scattering over IZO, and that the dust layers extended to 5 km asl. The value of the dust backscatter–extinction ratio was determined to be 0.027±0.007 sr−1. Comparisons of the MPL data with data from other co‐located instruments showed good agreement during the dust episode.  相似文献   

20.
An air pollution prediction model system (APOPS) is developed and applied to northern Taiwan with complex terrain and local thermal circulations. It consists of a nonhydrostatic mesoscale meteoro‐logical model system (MMPMS) and a gas/aerosol transport and air quality model (GATAM). The basic processes relevant to modeling the urban air pollution problems such as meteorology, dispersion, chemistry and deposition are solved at the same time on practically the same grid. The APOPS was tested on a high‐ozone event in northern Taiwan on 16 November 1998. Comparison with observed surface winds shows able to predict local flow patterns such as sea/land breezes and mountain‐valley wind in this high air pollution episode. The predicted surface concentrations of ozone and other pollutants are compared with measured values, and a fairly good agreement with the mean normalized biases of −6%, −11%, for one‐day simulation and for daytime, respectively, is obtained for ozone. Thus, it is confirmed that the APOPS can be utilized to predict urban air quality in complex terrain area.  相似文献   

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