首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 31 毫秒
1.
This contribution presents characterisation efforts of the gas phase and particle phase main components during the FEBUKO orographic cloud passage experiments in autumn 2001 and 2002 in the Thüringer Wald (Germany). Three events out of a total of 14 were chosen as the best events considering all meteorological conditions. Gas phase and size-segregated particle phase data obtained from physical (dry size distribution) and chemical (particle mass, main ions, OCEC, and water-soluble metals) measurements are presented for the upwind site. The total particulate mass concentration (PM10) was found to be between 8 and 17 μg m−3. Particles with an aerodynamic diameter up to 1.2 μm contribute about 80% of the mass concentration. About 90% of the total ion concentration consists of nitrate, sulphate and ammonium. The OC concentration in all three events amounts to about 1.0 μg m−3, whereas EC concentrations were between 0.40 and 1.0 μg m−3. The contribution of OC and EC to stage mass ranged from 5% to 35% and from 2% to 17%, respectively. The water content of particles was estimated to be 16–18%. Physical and chemical mass closure is discussed in detail and the results are in a reasonable agreement. The complex data set obtained for each event can be used in the initialisation of models for the multiphase processes during and after the cloud passage of the characterised air mass.  相似文献   

2.
3.
Size-resolved fog drop chemical composition measurements were obtained during a radiation fog campaign near Davis, California in December 1998/January 1999 (reported in Reilly et al., Atmos. Environ. 35(33) (2001) 5717; Moore et al., Atmos. Environ. this issue). Here we explore how knowledge of this size-dependent drop composition—particularly from the newly developed Colorado State University 5-Stage cloud water collector—helps to explain additional observations in the fog environment. Size-resolved aerosol measurements before and after fog events indicate relative depletion of large (>2 μm in diameter) particles during fog accompanied by a relative increase in smaller aerosol particle concentrations. Fog equivalent air concentrations suggest that entrainment of additional particles and in-fog sedimentation contributed to observed changes in the aerosol size distribution. Calculated deposition velocities indicate that sedimentation was an important atmospheric removal mechanism for some species. For example, nitrite typically has a larger net deposition velocity than water and its mass is found preferentially in the largest drops most likely to sediment rapidly. Gas–liquid equilibria in fog for NO3/HNO3, NH4+/NH3, and NO2/HONO were examined. While these systems appear to be close to equilibrium or relative equilibrium during many time periods, divergences are observed, particularly for low liquid water content (<0.1 g m−3) fogs and in different drop sizes. Knowledge of the drop size-dependent composition provided additional data useful to the interpretation of these deviations. The results suggest that data from multi-stage cloud water collectors are useful to understanding fog processes as many depend upon drop size.  相似文献   

4.
Operator splitting applied to cloud micro-physical and multiphase chemical process causes the so-called operator splitting errors in addition to other numerical errors when used in numerical models. Operator splitting is mainly used due to limited computer resources or for historical reasons. Unfortunately, it is impossible so far to theoretically estimate either the order of magnitude or the tendency of the splitting errors in complex non-linear systems such as mutually interacting cloud chemical and micro-physical processes.The present study systematically investigates the splitting error mentioned above, by numerical means to define valid ranges of the applicability of the method of operator splitting to those systems. Results of the current study show that de-coupling intervals larger than 100 s cause an underestimation of the total liquid water content as well as the particle radius of the order of 10% for simulation periods of 1000 s. The maximum overprediction of the total content of dissolved material in the particles is of the order of about 20% for de-coupling intervals of 10–15 min. The error in the sulphate production contributes about 50% to the discrepancy in total aerosol content. Since the de-coupling intervals between dynamical, micro-physical, and chemical processes in most recent air quality models are considerably longer than 15 min, the consequences of the application of operator splitting requires further investigation with respect to predicted aerosol formation, cloud water content, deposition rates, photo-chemistry, cloud optical properties, etc.  相似文献   

5.
Airborne measurements of the growth of the marine accumulation mode after multiple cycles through stratocumulus cloud are presented. The nss-sulphate cloud residual mode was log-normal in spectral shape and it’s mode radius was observed to progressively increase in size from 0.78 to 0.94 μm over 155 min of air parcel evolution through the cloudy marine boundary layer. The primary reason for this observed growth was thought to result from aqueous phase oxidation of SO2 to aerosol sulphate in activated cloud drops. An aqueous phase aerosol–cloud-chemistry model was used to simulate this case study of aerosol growth and was able to closely reproduce the observed growth. The model simulations illustrate that aqueous phase oxidation of SO2 in cloud droplets was able to provide enough additional sulphate mass to increase the size of activated aerosol. During a typical cloud cycle simulation, ≈4.6 nmoles kg-1air (0.44 μg m-3) of sulphate mass was produced with ≈70% of sulphate production occurring in cloud droplets activated upon sea-salt nuclei and ≈30% occurring upon nss-sulphate nuclei, even though sea-salt nuclei contributed less than 15% to the activated droplet population. The high fraction of nss-sulphate mass internally mixed with sea-salt aerosol suggests that aqueous phase oxidation of SO2 in cloud droplets activated upon sea-salt nuclei is the dominant nss-sulphate formation mechanism and that sea-salt aerosol provides the primary chemical sink for SO2 in the cloudy marine boundary layer.  相似文献   

6.
Preliminary experimental results are presented from an aircraft-mounted probe designed to provide in situ data on cloud particle shape, size, and number concentration. In particular, the probe has been designed to facilitate discrimination between super-cooled water droplets and ice crystals of 1–25 μm size within mixed-phase clouds and to provide information on cloud interstitial aerosols. The probe acquires spatial light scattering data from individual particles at throughput rates of several thousand particles per second. These data are logged at 100 ms intervals to allow the distribution and number concentration of each particle type to be determined with 10 m spatial resolution at a typical airspeed of 100 m s−1. Preliminary results from flight data recorded in altocumulus castellanus, showing liquid water phase, mixed phase, and ice phase are presented to illustrate the probe's particle discrimination capabilities.  相似文献   

7.
8.
Black carbon (soot) concentrations have been measured in rain water, snow samples and near surface air at several locations in Nova Scotia, Canada. The average black carbon concentration in near surface air in summer was found to be 0.54 μg m-3 compared to 1.74 μg m-3 in the winter season. These values are comparable to black carbon concentrations found in other mid-size urban areas. The black carbon concentration in rain water and snow samples varied between an undetectable amount to about 20 μg kg-1 of rain (or melt) water. The relatively low concentrations of black carbon in precipitation are attributed to extratropical cyclones that often develop off-shore to the east and south of Nova Scotia in relatively clean conditions of the marine boundary layer.  相似文献   

9.
The goal of this modeling study is to determine how concentrations of ozone respond to changes in climate over the eastern USA. The sensitivities of average ozone concentrations to temperature, wind speed, absolute humidity, mixing height, cloud liquid water content and optical depth, cloudy area, precipitation rate, and precipitating area extent are investigated individually. The simulation period consists of July 12–21, 2001, during which an ozone episode occurred over the Southeast. The ozone metrics used include daily maximum 8 h average O3 concentration and number of grid cells exceeding the US EPA ambient air-quality standard. The meteorological factor that had the largest impact on both ozone metrics was temperature, which increased daily maximum 8 h average O3 by 0.34 ppb K−1 on average over the simulation domain. Absolute humidity had a smaller but appreciable effect on daily maximum 8 h average O3 (−0.025 ppb for each percent increase in absolute humidity). While domain-average responses to changes in wind speed, mixing height, cloud liquid water content, and optical depth were rather small, these factors did have appreciable local effects in many areas. Temperature also had the largest effect on air-quality standard exceedances; a 2.5 K temperature increase led to a 30% increase in the area exceeding the EPA standard. Wind speed and mixing height also had appreciable effects on ozone air-quality standard exceedances.  相似文献   

10.
Estimates of the atmospheric deposition to Galveston Bay of polycyclic aromatic hydrocarbons (PAHs) are made using precipitation and meteorological data that were collected continuously from 2 February 1995 to 6 August 1996 at Seabrook, TX, USA. Particulate and vapor phase PAHs in ambient air and particulate and dissolved phases in rain samples were collected and analyzed. More than 95% of atmospheric PAHs were in the vapor phase and about 73% of PAHs in the rain were in the dissolved phase. Phenanthrene and napthalene were the dominant compounds in air vapor and rain dissolved phases, respectively, while 5 and 6 ring PAH were predominant in the particulate phase of both air and rain samples. Total PAH concentrations ranged from 4 to 161 ng m−3 in air samples and from 50 to 312 ng l−1 in rain samples. Temporal variability in total PAH air concentrations were observed, with lower concentrations in the spring and fall (4–34 ng m −3) compared to the summer and winter (37–161 ng m−3). PAHs in the air near Galveston Bay are derived from both combustion and petroleum vaporization. Gas exchange from the atmosphere to the surface water is estimated to be the major deposition process for PAHs (1211 μg m− 2 yr− 1), relative to wet deposition (130 μg m−2 yr− 1) and dry deposition (99 μg m−2 yr− 1). Annual deposition of PAHs directly to Galveston Bay from the atmosphere is estimated as 2  t yr−1.  相似文献   

11.
Carbonyl compounds exist in the atmosphere as either gases or aerosols. Some of them are water soluble and known as oxidation products of biogenic and/or anthropogenic hydrocarbons. Five carbonyl compounds, glyoxal (GO), 4-oxopentanal (4-OPA), glycolaldehyde (GA), hydroxyacetone (HA) and methylglyoxal (MG) have been identified in a temporal series of 12 rain samples. The concentrations of the compounds in the samples were high at the beginning of the rain event and decreased with time to relatively low and fairly constant levels, indicating that the compounds were washed out from the atmosphere at the start of the rain event. Possibly, these compounds also existed in the cloud condensation nuclei (CCN). Wet deposition rates of the carbonyl compounds were calculated for nine samples collected during a 20 h period. The deposition rates ranged from 0 (4-OPA) to 1.2×10−1 mg C m−2 h−1 (MG) with the average of 2.9×10−2 mg C m−2 h−1. Production rates of isoprene oxidation products (GA, HA and MG) in the area surrounding the sampling site were estimated with a chemical box model. The deposition rates exceeded the production rates in most samples. This indicates that the rainfall causes a large net flux of the water soluble compounds from the atmosphere to the ground. Insoluble carbonyl compounds such as n-nonanal and n-decanal were expected to be present in the atmosphere, but were not detected in the rain during the sampling period, suggesting that an aerosol containing these insoluble compounds does not effectively act as a CCN.  相似文献   

12.
A chemical mass balance of fine aerosol (<1.5 μm AED) collected at three European sites was performed with reference to the water solubility of the different aerosol classes of components. The sampling sites are characterised by different pollution conditions and aerosol loading in the air. Aspvreten is a background site in central Sweden, K-puszta is a rural site in the Great Hungarian Plain and San Pietro Capofiume is located in the polluted Po Valley, northern Italy. The average fine aerosol mass concentration was 5.9 μg m-3 at the background site Aspvreten, 24 μg m-3 at the rural K-puszta and 38 μg m-3 at the polluted site San Pietro Capofiume. However, a similarly high soluble fraction of the aerosol (65–75%) was measured at the three sites, while the percentage of water soluble organic species with respect to the total soluble mass was much higher at the background site (ca. 50%) than at the other two sites (ca. 25%). A very high fraction (over 70%) of organic compounds in the aerosol consisted of polar species. The presence of water soluble macromolecular compounds was revealed in the samples from K-puszta and San Pietro Capofiume. At both sites these species accounted for between ca. 20–50% of the water soluble organic fraction. The origin of the compounds was tentatively attributed to biomass combustion.  相似文献   

13.
During April 1999 and March 2000, intensive field campaigns were performed on a mid-level mountain (Rax, 1644 m a.s.l.) in Central Europe both under out-of-cloud and in-cloud conditions. The black carbon (BC) content of both aerosol and cloud water as well as BC scavenging efficiencies of Rax clouds were measured. As a tracer for the non-carbonaceous aerosol, sulfate was used. Although BC concentrations on Rax were low (April 1999 out-of-cloud average: 0.43 μg/m3, March 2000: 0.72 μg/m3), the BC mass fraction of the aerosol was fairly high (1999: 3.5%, 2000: 6.4%). Average BC concentrations in cloud water were 1.09 μg/ml (1999) and 1.4 μg/ml (2000). These values are far higher than literature values, but comparable to those found in an earlier study (J. Geophys. Res. 105 (D20) (2000) 24637) at a high-level mountain (Sonnblick, 3106 m a.s.l.) some 200 km distant from Rax. The average BC scavenging efficiency of the Rax clouds in March 2000 was 0.54. The increase of scavenging efficiency with increasing liquid water content of the clouds found earlier on Sonnblick for sulfate and aerosol carbon (J. Atmos. Chem 35 (2000) 33), organic carbon (J. Geophys. Res. 105 (2000) 19857), and BC (J. Geophys. Res. 105 (D20) (2000) 24637) was also confirmed on Rax.  相似文献   

14.
A water surface sampler (WSS) was employed in combination with greased knife-edge surface deposition plates (KSSs) to measure the vapor phase deposition rates of PCBs to the sampler at an urban site, Chicago, IL. This sampler employed a water circulation system that continuously removed deposited PCBs. Total (gas+particle) and particulate PCB fluxes were collected with the WSS and KSSs, respectively. Gas phase PCB fluxes were then calculated by subtracting the KSS fluxes (particulate) from the WSS fluxes (gas+particle). The calculated gas phase PCB fluxes averaged 830±910 ng m−2d−1. This flux value is, in general, higher than the fluxes determined using simultaneously measured air–water concentrations in natural waters and is in the absorption direction. This difference is primarily because the PCBs were continuously removed from the WSS water keeping the water PCB concentration near zero.Concurrently, ambient air samples were collected using a modified high volume air sampler. The gas phase PCB concentrations ranged between 1.10 and 4.46 ng m−3 (average±SD, 2.29±1.28 ng m−3). The gas phase fluxes were divided by the simultaneously measured gas phase ambient concentrations to determine the overall gas phase mass transfer coefficients (MTCs) for PCBs. The average gas phase overall MTCs (Kg) for each homolog group ranged between 0.22 and 1.32 cm s−1 (0.54±0.47 cm s−1). The average MTC was in good agreement with those determined using similar techniques.  相似文献   

15.
The PM2.5 concentrations and the size distributions of dicarboxylic acids in Hong Kong were studied. Eleven sets of daily PM2.5 samples were obtained at a downtown sampling site during the period of 5–16 December 2000 using an R&P speciation PM2.5 sampler. About 6–12% of the total oxalic acid was found in the gas phase in some samples. A good correlation between succinate and sulfate (R2=0.88) and a moderate correlation between oxalate and sulfate (R2=0.74) were found. Sampling artifacts of oxalate, malonate and succinate were found to be negligible. A total of 18 sets of 48–96 h size distribution data on dicarboxylic acids, sulfate, nitrate and sodium at an urban site and a rural site from June 2000 to May 2001 were obtained using a Micro-Orifice Uniform Deposit Impactor. Data from both sites show similar size distribution characteristics of the dicarboxylic acids. The condensation mode of oxalate was usually observed at 0.177–0.32 μm. The location of the peak of the droplet mode of oxalate was associated with that of sulfate. When the peak of sulfate in the droplet mode appeared at 0.32–0.54 μm, the peak of oxalate sometimes appeared at 0.32–0.54 μm and sometimes shifted to 0.54–1.0 μm. When the peak of sulfate in the droplet mode appeared at 0.54–1.0 μm, the peak of oxalate sometimes appeared at 0.54–1.0 μm and sometimes shifted to 1.0–1.8 μm. Oxalate, succinate and sulfate found in the droplet mode were attributed to in-cloud formation. The slight shift of the oxalate peak from 0.32–0.54 to 0.54–1.0 μm or from 0.54–1.0 to 1.0–1.8 μm was ascribed to minor oxalate evaporation after in-cloud formation. The maximum peak of malonate sometimes appeared in the droplet mode and sometimes appeared at 3.1–6.2 μm. The formation of malonate is associated to the reactions between sea salt and malonic acid.  相似文献   

16.
Concentrations of size fractionated particulate sodium and potassium were measured in both marine and urban air. Marine air sampling was conducted during a cruise on R/V Hakuho-maru in the northwestern North Pacific in the summer of 1998. Urban air sampling was performed in the central part of Tokyo in 1997 and 1998. The fine sodium concentration (D<1.1 μm) in “Urban” air (180 ng m−3) was 3 times higher than that in “Marine” air (56 ng m−3). In the urban air samples, the size distributions of sodium and potassium showed bimodal peaks in the fine particle range (D<1.1 μm) and in the coarse particle range (D>1.1 μm). The existence of anthropogenic sodium in the fine particle range was detected in the urban air. The K/Na weight ratios in the fine particle range of the urban air (1.8–2.7) was 50–75 times higher than that in seawater (0.036). Potassium in the urban air is thought to be derived largely from anthropogenic sources. In the urban air samples, a high correlation between fine sodium and fine potassium concentrations suggests that they have the same anthropogenic source. Reevaluating the K/Na ratios in marine air to be relatively higher than that in seawater, we can estimate that several percents of anthropogenic sodium can be transported from land to remote marine air.  相似文献   

17.
Deposition processes of particles with dry diameter larger than about 10 μm are dominated by gravitational settling, while molecular diffusion and Brownian motion predominate the deposition processes of particles smaller than 0.1 μm in dry diameter. Many air pollution derived elements exhibit characteristics common to sub-micron particles. The objective of the present study is to examine the effects of meteorological conditions within the turbulent transfer layer on the deposition velocity of particles with dry diameter between 0.1 and 1 μm. It is for these sub-micron particles that particle growth by condensation in the deposition layer, the broken water surface effect and the enhanced transfer process due to atmospheric turbulence in the turbulent transfer layer play important roles in controlling the particle deposition velocity. Results of the present study show that the `dry air’ assumption of Williams’ model is unrealistic. Effects of ambient air relative humidity and water surface temperature cannot be ignored in determining the deposition velocity over a water surface. Neglecting effects of ambient air relative humidity and water surface temperature will result in defining atmospheric stability incorrectly. It is found that the largest effect of air relative humidity on deposition velocity occurs at an air–water temperature difference corresponding to the point of `displaced neutral stability'. For a given wind speed of U=5 m s−1 the additive effects of water surface temperature, Tw, changes from 5 to 25°C and ambient air relative humidity variations from 85 to 60%, respectively, lead to a maximum difference in vd of about 20%. For a higher wind speed of 10 m s−1, however, the corresponding change in vd reduces to less than 5%. This is further confirmation that wind speed is one of the strongest variables that governs the magnitude of vd. The present study also found that the broken surface transfer coefficient, kbs, given as a multiple of the smooth surface transfer coefficient, kss, is physically more meaningful than assigning it a constant value independent of particle size. The method used in this study requires only a single level of atmospheric data coupled with the surface temperature measurement. The present method is applicable for determining deposition velocity not only at the conventional measurement height of 10 m but also at any other heights that are different from the measurement height.  相似文献   

18.
《Chemosphere》2012,86(11):1664-1671
The Connecticut Department of Environmental Protection (CTDEP) commenced monitoring for PCDDs/PCDFs (polychlorinated dibenzodioxins and polychlorinated dibenzofurans) in ambient air in 1987 and adopted the long term (30 d) sampling approach in 1993. The CTDEP method represents the first use of isotopically labeled PCDDs/PCDFs as field surrogates to monitor the behavior of native PCDDs/PCDFs present in actual ambient air samples. This feature first introduced in 1987 was later adopted by US EPA in revisions to sampling methods for PCDDs/PCDFs in ambient air (EPA Method TO9A) as well as development of EPA Reference Method 23 for measurement of PCDDs/PCFDs in stationary source emissions. Results are provided here for a total of twenty-three (23) samples (reported as pairs) representing twelve (12) 30 d sampling events conducted at a site located in metropolitan Hartford CT. Samples were collected in winter months during calendar years 2002–2008. PCDDs/PCDFs concentration data (pg m−3) are reported as both congener sums (Cl4–Cl8) and 2378-substitued congeners. Total PCDDs/PCDFs concentrations for these twelve (12) sampling events ranged from 0.68 pg m−3 (2003) to 4.18 pg m−3 (2004) with a mean concentration of 2.04 pg m−3.Method performance was monitored through use of collocated samples, in field isotopically labeled compounds, isotopically labeled laboratory applied internal standards and field blank samples. Method performance consistently exceeded goals established in USEPA Method TO9A for these same parameters. Average recoveries of in field labeled PCDDs/PCDFs ranged from 97.5% to 104.2%. Average (mean) recoveries for each of the ten (10) isotopically labeled internal standards ranged from 77.0% (13C-OCDF) to 95.5% (13C-2,3,7,8-TCDF). Method precision defined as % RPD data for collocated sampler pairs ranged from 8% to 14% for PCDDs and from 5% to 12% for PCDFs. The mean RPD for all PCDDs/PCDFs combined is 9.6%. Field monitoring results demonstrate method sensitivity for all PCDDs/PCDFs congeners and 2378-substituted congeners to be well below concentrations typically found for these compounds in ambient air (all reported data represent measured concentrations). Quantities (pg) found in field blanks represent the major determinant to achieving further enhancements in method sensitivity for selected congeners (OCDD < 42 fg m−3; 1,2,3,4,6,7,8-HpCDD < 5.7 fg m−3; and 1,2,3,4,6,7,8-HpCDF < 2.1 fg m−3). The CTDEP method represents a highly sensitive and reliable technique for monitoring of PCDDs/PCDFs congeners and other persistent organic pollutants (POPs) at ultra trace levels in ambient air (fg m−3).  相似文献   

19.
Even though dry deposition and air–water exchange of semivolatile organic compounds (SOCs) are important for surfaces in and around the urban areas, there is still no generally accepted direct measurement technique for dry deposition. In this study, a modified water surface sampler (WSS) configuration, including a filter holder and an XAD-2 resin column, was employed to investigate the polycyclic aromatic hydrocarbon (PAH) dry deposition in an urban area. The measured total (particle+dissolved) PAH fluxes to the WSS averaged to be 34 960±16 540 ng m−2 d−1. Average particulate PAH flux, determined by analyzing the filter in the WSS, was about 8% of the total PAH flux. Temporal flux variations indicated that colder months (October–April) had the highest PAH fluxes. This increase could be attributed to the residential heating as well as meteorological effects including lower mixing height. A high volume air sampler was concurrently employed to collect ambient air concentrations. The average total (gas+particle) atmospheric PAH concentration (456±524 ng m−3) was within the range of previously measured values at different urban locations. PAH concentrations in urban areas are more than two orders of magnitude higher than those measured in pristine areas and this result may indicate that urban areas have major source sectors and greater deposition rates are expected near to these areas. The average contribution of particle phase was about 10% in total concentration. Simultaneous particulate phase dry deposition and ambient air samples were collected in this study. Then, particulate phase apparent dry deposition velocities were calculated using the fluxes and concentrations for each PAH compound and they ranged from 0.1 to 1.2 cm s−1. These values are in good agreement with previously reported values.  相似文献   

20.
A high volume electrostatic field-sampler was developed for collection of fine particles, which easily can be recovered for subsequent sample characterisation and bioassays. The sampler was based on a commercial office air cleaner and consisted of a prefilter followed by electrostatic collection plates operating at 2.7 kV. The sampler performance was characterised for 26 nm to 5.4 μm-size particles in urban street air. The collection efficiency reached a maximum (60–70%) between 0.2 and 0.8 μm and dropped to ∼25% at 30 nm and 2.5 μm, respectively. After extraction in water, the particle loss was<2%. The extraction efficiency for dry lyophilised particulate matter was above 80%, allowing retrievement of ∼12 mg day−1 in urban street air at PM10 levels of ∼24 μg m−3. The ozone generating capacity of the corona discharge during operation was on the order of 10 ppb. A polycyclic aromatic hydrocarbons (PAH) degradation test using benzo[a]pyrene as a model showed that ∼85% was degraded after 24 h. However, similar results were observed when the corona discharge was switched off. Hence, the ozone and other corona discharge reactants do not appear to contribute considerably to PAH-degradation. The overall results show that the sampler type is a promising alternative to traditional sampling of fine particles for bulk analysis and bioassays. The main advantages are simple operation, high stability, high quantifiable particle recovery rates and low cost.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号