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1.
Lee  D. S.  Dollard  G. J.  Derwent  R. G.  Pepler  S. 《Water, air, and soil pollution》1999,113(1-4):175-202
Measurements of sulphur dioxide, ozone, ammonia, and soluble inorganic components of the atmospheric aerosol were made at a site in central southern England. Ammonia, ozone, and nitrate aerosol in winter were shown to exhibit significant diurnal variation. Ozone showed a typical diurnal variability, the magnitude of which was dependent upon wind speed. The lower night-time ozone concentrations at lower wind speeds were attributed to depletion inside nocturnal boundary layers by dry deposition. Ammonia, in contrast, showed a different behaviour, whereby the diurnal cycle was more pronounced at higher wind speeds, indicating that the cycle was unlikely to be the result of dry deposition at night. Ammonia concentrations showed a temperature dependence and the diurnal cycle of ammonia at this site appears to be the result of a temperature-driven emission signal. Of the total reduced nitrogen, NHx (NHx = NH3 + NH4 + aerosol), the phase was dominant and it is likely that more than 60% of the boundary layer NHx is in this phase. The loss term of ammonia by reaction with acid sulphate aerosol is likely to be greater than that by dry deposition on a UK scale. Nitrate aerosol showed a positive correlation with sodium aerosol, once the effect of mutual correlations with sulphate and ammonium were removed. This correlation effect, in combination with evidence of a marine-oriented directional dependence of nitrate aerosol, and negative non sea-salt chloride aerosol from the same ‘marine’ sector, shows the potential importance of the formation of sodium nitrate aerosol from reaction of dinitrogen pentoxide, or possibly nitric acid or nitrogen dioxide with sodium chloride aerosol. It is likely that this provides the major route of nitrate into rain, not the scavenging of nitric acid vapour. Aerosol sulphate, nitrate, and ammonium have been measured at Harwell since 1954. Sulphate aerosol increased up until 1976 and has declined subsequently. Nitrate aerosol has increased over the whole period, whereas ammonium aerosol follows a similar pattern to that of sulphate, but with an equivocal direction of trend after 1976. Sulphate, nitrate and ammonium aerosol all show a similar statistically significant seasonality. A historical inventory of ammonia emissions shows a clear correlation with ammonium aerosol.  相似文献   

2.
The representative mass ratio of the reactive airborne sulphur-to-nitrogen, S/N in the gas and aerosol phases, and in wet and dry deposition over the territory of Hong Kong, SAR,was determined, utilizing available data for the 12 yr period, 1986–1997. Using this information, the representative stoichiometric ratio values for sulphate-to-nitrate in aerosoland in wet and dry depositions were estimated. A limited supplementary data set on various canopy depositions was alsoutilized. This information collectively suggests several basicdifferences in photochemical processes between the urbanatmospheres in and around Hong Kong and the classical, smoggyLos Angeles. This is also supported by the typical diurnal variation of nitrogen oxides in Hong Kong, which suggests a moreefficient photo-oxidation of NO to NO2 within the territoryand in nearby areas upwind, as compared to further oxidation tothe NO3 (or nitrate) stage. On the other hand, the relatively low gas-to-particle ratio value estimated for S (~3) relative to N (~26) suggests that the advectedfraction of non-sea salt aerosol sulphate in the territory couldbe considerably greater than the corresponding fraction for nitrate. Finally, significant losses (probably related to sampling) of NH4-NH3 in dry deposition could be inferred, while for SO4 in wet deposition, a moderate enrichment factor of ~2 is observed in relation to SO4 in aerosol.  相似文献   

3.
Aerosol samples and meteorological data were collected at a mid-southern Lake Michigan site (87° 00′ W, 42° 00′ N) from May through September 1977. Hi-volume samplers with cellulose fiber filters and a digital meteorological data recording system were operated on board the U.S. EPA's R/VRoger R. Simons during four intensive sampling periods. Aerosol samples were analyzed by atomic absorption spectroscopy for seventeen trace elements. A diabatic drag coefficient method was used to determine aerosol deposition velocity (v d ) overlake. A meanv d of 0.5 cm s?1 was found for the 0.1v d to a long-term climatological record, annual dry deposition loadings to the southern basin for nine elements were estimated. For four elements, Fe, Mn, Pb, and Zn, dry deposition loadings to the southern basin alone of at least 500, 30, 250, and 100 (×103 kg yr?1) were found. For Fe and Mn, these loadings represent about 15% of the total of all inputs to Lake Michigan. for Zn and Pb, about one-third to one-half of the annual loading from all sources is from dry deposition of atmospheric aerosol.  相似文献   

4.
The distribution of acidic andalkaline constituents (SO4 2-,NO3 -, Cl-, NH4 +, Na+,K+, Ca2+) between the fine and coarseparticle range has been examined in an urban locationin Thessaloniki, N. Greece over an 8-month period. The chemistry of wet and dry deposition collected overthe same period was also examined. Statisticalassociations between species within each environmentalphase were investigated using correlation analysis.Use of principal component analysis was made toinvestigate compositional similarities betweenaerosol, deposited dust and rain. It was found thatSO4 followed by NO3, NH4 and Caprevailed in fine aerosol. Sulphates and Ca were alsothe prevailing ions in the coarse particle fraction.Wet deposition was found to be the dominant depositionmechanism for all species. The high dry depositionrates observed for Ca and SO4 suggest that mostof the dry deposited sulphate is in the form ofCaSO4. Scavenging ratios of ionic speciesassociated with coarse aerosol were higher than thecorresponding ratios for fine particles. Principalcomponent analysis suggested that variations in ioniccomposition of fine aerosol could be interpretedprimarily by gas-to-particle neutralization reactionsinvolving atmospheric ammonia. In contrast, theinteraction between SO2 and HNO3 with Cacompounds seems to be the most likely factor that canexplain variations in wet and dry deposition ioniccontents.  相似文献   

5.
The deposition of ozone onto hypostomatous red maple and amphistomatous hybrid poplar leaves was studied under controlled environments. Under similar environmental conditions, the ozone deposition was substantially greater onto poplar than onto maple leaves. Two kinds of surface wetness (simulating dew and raindrops) were artificially created on leaves to determine how deposition was affected. The ozone deposition onto wet maple leaves markedly increased almost immediately after water spraying. The increases were measured during both daytime and nighttime conditions. Nighttime measurements revealed that the enhanced ozone deposition onto wet maple leaves was largely controlled by the chemistry of the solution which eventually developed while leaves remained wet. Unlike maple leaves, small ozone deposition reductions were measured after poplar leaves became wet during daytime conditions. In addition, little ozone deposition was detected onto wet poplar leaves during the night, indicating that leaf water chemistry was less important for poplar than for maple leaves.  相似文献   

6.
We measured atmospheric nutrient deposition as wet deposition and dry deposition to dry and wet surfaces. Our analyses offer estimates of atmospheric transport of nitrogen (N), phosphorus (P) and silicon (Si) in an agricultural region. Annual dry and wet deposition (ha?1 year?1) was 0.3 kg of P, 7.7 kg of N, and 6.1 kg of Si; lower than or similar to values seen in other landscapes. N:P and Si:N imply that atmospheric deposition enhances P and Si limitation. Most P and soluble reactive P (SRP) deposition occurred as dryfall and most dry-deposited P was SRP so would be more readily assimilable by plant life than rainfall P. Dry deposition of N to wet surfaces was several times greater than to dry surfaces, suggesting that ammonia (NH x ) gas absorbtion by water associated with wet surfaces is an important N transport mechanism. Deposition of all nutrients peaked when agricultural planting and fertilization were active; ratios of NH x :nitrate (NO x ) hbox{reflected} the predominant use of NH x fertilizer. Wet deposition estimates were consistent over hundreds of km, but dry deposition estimates were influenced by animal confinements and construction. Precipitation wash-out of atmospheric nutrients was substantial but larger rain events yielded higher rates of wet deposition. Methodological results showed that local dust contaminated wet deposition more than dry; insects, bird droppings and leaves may have biased past deposition estimates; and estimating dry deposition to dry plastic buckets may underestimate annual deposition of N, especially NH x .  相似文献   

7.
The exchange process known as dry deposition encompasses the dynamic exchange of trace gases and aerosol particles, and the gravitational settling of large particles. Except for particles large enough that their sedimentation velocity exceeds turbulent velocities, the rate of deposition is mostly determined by surface properties, such as roughness, stickiness, and wetness, and by atmospheric stability. Thus, it is difficult to interpret results obtained using collection devices having surfaces different from those of nature. Other methods for measuring dry deposition exist, mostly micrometeorological, but these are sufficiently complicated that routine application as in a monitoring network is not yet feasible. For some chemical species and in some locations, inferential methods offer considerable promise. These methods measure atmospheric concentrations (C) of the relevant chemical species, and derive relevant deposition velocities (vd) on a site-specific, species-dependent, and time-evolving basis. The dry deposition rates of interest are then evaluated as the product vd.C. A major goal of current research programs is to provide the knowledge necessary to evaluate vd. Experimental methods are reviewed, and potential sources of error are examined, for both the research methods and the “concentration monitoring” methodologies presently being advocated for use in numerical models as well as for routine monitoring.  相似文献   

8.
Various species including nitrate, HN03 and Pb were sampled in Antigonish, Nova Scotia and their fluctuations were compared to those of simultaneously sampled acid and sulphate (reported previously). The 24 hr average aerosol nitrate, ~0.3 μg m?3, was similar in the summer and winter. Nitric acid made up ~42 % of the total (aerosol and gaseous) nitrate in the summer and winter, but nitrate and HN03 were correlated only in the summer. Windroses are used to show the dependence of sulphate, nitrate and aerosol acid on wind direction. Lead had a 24 hr average concentration of 71 ng m?3, was of mainly local origin and was not able to be correlated with other parameters.  相似文献   

9.
The importance of dry deposition was assessed to oak and pine trees, in a hardwood and coniferous canopy, respectively. In both canopies, ambient particle and gas concentrations on the interior were decreased relative to perimeter concentrations due to dry deposition scavenging by the canopy. Deposition of all species was higher to perimeter leaves than to interior leaves, due both to the lower concentrations and the lower wind speeds in the sheltered interior. The deposition velocities measured to the pine needles were similar to the values measured to the oak leaves.  相似文献   

10.
Precipitation composition has been measured daily at five UK EMEP sites since 1987. Sulphur dioxide and sulphate aerosol concentrations are also measured daily at the sites. Back trajectories and wind sectors calculated by the Norwegian Meteorological Institute have been used to characterise the variation in wet deposition in terms of air mass source. Contributions to wet deposition from various source regions have been estimated for Eskdalemuir. Observations from the EMEP sites have been compared with output from the Hull Acid Rain Model (HARM). HARM is a Lagrangian model using simplified meteorology but straight-line trajectories. Results are compared on a site-by-site and sector-by-sector basis and the model reproduces the general features of pollutant concentration and wet deposition indicated by the measurements. The possible effects of future reductions in emissions of SO2 and NOx on precipitation concentrations by wind sector are described.  相似文献   

11.
Wet and dry deposition of atmospheric nitrogen (N) compounds into forest ecosystems and their effect on physical, chemical and microbial processes in the soil has attracted considerable attention for many years. Still the consequences of atmospheric N deposition on N metabolism of trees and its interaction with soil microbial processes has only recently been studied. Atmospheric N deposited to the leaves is thought to enter the general N metabolism of the leaves, but the processes involved, the interaction with different metabolic pathways, and the connection between injury by atmospheric N and its metabolic conversion are largely unknown. Laboratory and field experiments have shown that N of atmospheric NO2 and NH3, deposited to the leaves of trees, is subject to long-distance transport in the phloem to the roots. This allocation can result in considerable decline of N uptake by the roots. Apparently, the flux of N from the soil into the roots can be down-regulated to an extent that equals N influx into the leaves. This down-regulation is not mediated by generally enhanced amino-N contents, but by elevated levels of particular amino acids. Field experiments confirm these results from laboratory studies: Nitrate (NO3) uptake by the roots of trees at a field sites exposed to high loads of atmospheric N is negligible, provided concentrations of Gln in the roots are high. At the ecosystem level, consequences of reduced N uptake by the roots of trees exposed to high loads of atmospheric N are (1) an increased availability of N for soil microbial processes, (2) enhanced emission of gaseous N-oxides from the soil, and (3) elevated leaching of NO3 into the ground water. How recent forest management practices aimed at transforming uniform monocultures to more structured species-rich forests will interact with these processes remains to be seen. Possible implications of these forest management practices on N metabolism in trees and N conversion in the soil are discussed particularly in relation to atmospheric N deposition.  相似文献   

12.
As a new approach, urban air pollution was characterised by the variation of columnar content of the pollutants. Columnar content (CC) was estimated as the product of the pollutant??s mixing ratio and the mixing height. Mixing ratio data of the Metropolitan Air Quality Monitoring Network of Budapest were used, whilst mixing height was calculated by the meteorological AERMET model code. Time variation of CC refers to the real pollution exchange in the atmosphere that allows direct investigation of the emissions as well as post-emission modifications of the pollutants (such as chemical degradation or production). The diurnal urban CO cycle was found to be determined by two or three main influx peaks according to the traffic pattern of the site. The diurnal variation of NO x level was found to be driven by traffic emission as well. Variant ratios of NO x to CO influxes obtained for the different locations of the city range from 0.12 to 0.23, probably according to the vehicle composition of the traffic. The daily balance of photochemical production, chemical degradation and deposition of ozone yielded negative or positive depending on the location. Negative balances imply that the polluted urban atmosphere is a net ozone neutraliser source. Entrainment from the free troposphere yielded the major contributor to the diurnal ozone level at each site. The diurnal urban PM10 cycle was found to be determined by traffic emission during the morning and evening rush hours whilst secondary aerosol formation around noon. In the evening, high PM10 level rise was observed due to direct traffic emission as well as rapid conversion of the fine aerosol fraction to the coarse fraction.  相似文献   

13.
Wet-only rainwater composition on a daily basis, and atmospheric SO2 and NO2 concentrations on a monthly basis have been measured over a two year period at four sites ~100 km to the west of Sydney. Bulk aerosol composition on a monthly basis was also measured at one site. The study region is predominantly rural in character, but contains two coal-fired thermal power stations with a total installed capacity of 2320 MW, as well as several min or population centres, including a small city, with a total population of about 21,000. The measurement sites were located roughly on the perimeter of a circle of about 20 km radius having the power stations at its centre. Three of the sites were situated in rural settings, while the fourth was located on the outskirts of the small city of Lithgow. Atmospheric acid loadings at all sites were low by the standards usually associated with industrialised regions of Europe and North America, with about one third of rainwater total acidity provided by organic acids (formic, acetic and oxalic). At the three rural sites, total inorganic acid deposition, comprising measured wet deposition plus inferred dry deposition of acidic S and N species, averaged about 30 meq m?2 y?1, a low figure by most standards. At the site located near the city of Lithgow total deposition of acidic S and N species averaged about 80 meq m?2 y?1.  相似文献   

14.
The atmospheric chemistry, deposition and transport of mercury (Hg) in the Upper Great Lakes region is being investigated at a near-remote sampling location in northern Wisconsin. Intensive sampling over two years and various seasons has been completed. A multi-phase collection strategy (gas-, particle- and precipitation-phases) was employed to gain insight into the processes controlling concentrations and chemical/physical speciation of atmospheric Hg. Additional chemical and physical atmospheric determinations (e.g. ozone, particulate constituents, meteorology) were also made during these periods to aid in the interpretation of the Hg determinations. For example, correlations of Hg with ozone, sulfur dioxide and synopticscale meteorological features suggest a regionally discernible signal in Hg. Comparison to isosigma backward air parcel trajectories confirms this regionality and implicates the areas south, southeast and northwest of the site to be sources for Hg. Particle-phase Hg (Hgp) was found to be approximately 40% in an oxidized form, or operationally defined as “reactive”. However, this was quite variable from year-to-year. Hgp and other particle constituents (esp. sulfate) show significant correlation and similarity in behavior (concentration ratios in precipitation and in particles). These observations are part of the growing evidence to support the hypothesis that precipitation-phase Hg arises in large part from the scavenging of atmospheric particulates bearing Hg. Observed concentrations of rain and particle-Hg fit broadly the theoretical expectations for nucleation and below-cloud scavenging. Significant increases in the Hg/aerosol mass ratio appear to take place during transport. Enrichment of aerosols is taken as evidence of gas/particle conversion which could represent the step linking gas-phase Hg with rain. The refined budget indicates ca. 24% of total deposition is from summer particle dry deposition, and that this deposition also contributes ca. 24% of all reactive Hg deposition. Additionally, almost all (86%) deposition (wet and dry) occurs during the summer months.  相似文献   

15.
In this study, we evaluated the relative contribution of atmospheric particulate mercury (Hg(p)) and divalent reactive gaseous mercury (RGM) to mercury dry deposition in Japan. The dry deposition fluxes (on a water surface sampler) and atmospheric PM concentrations of Hg, Cd, Cu, Mn, Ni, Pb and V, which were measured concurrently from April 2004 to March 2006 at 10 sites across the nation, were used in this evaluation. We considered that Hg(p) and RGM, but not Hg0, are deposited on the water surface, and that our method of sampling Hg(p) without the use of KCl-coated annular denuders enables the exclusion of a significant amount of RGM artifact. The monthly average dry deposition velocities (= deposition flux/atmospheric PM concentration) of Cd and Pb were found to be similar to each other (Cd/Pb deposition velocities?=?1.06?±?0.58). It was assumed that the deposition velocity of Hg(p) is identical to the mean deposition velocity of Cd and Pb, because the particle size distribution of Hg(p) is likely similar to those of both elements. Using this deposition velocity, the monthly dry deposition flux of Hg(p) was calculated. The average contribution (±1σ) of Hg(p) to the annual deposition flux at ten sites was 26?±?15%. The mercury dry deposition flux increased generally from spring to early summer, which was attributed mostly to the deposition of RGM. This seasonal change correlated to that in photochemical oxidant (primarily O3) concentration in air at most sites. These suggest that mercury dry deposition in Japan is predominantly deposition of RGM, which was formed via oxidation of Hg0 by O3 in the atmosphere.  相似文献   

16.
Rainwater has been sampled weekly from five sites (nos. 1–5) in northeastern Vietnam in the period of May 1997 to Apr. 2000 (except Hoabinh site, from Aug. 1999 to Apr. 2000). Since Aug. 1999, weekly dry deposition samples including acidic gas and aerosol have been additionally collected at Hanoi (no. 4) and Hoabinh (no. 5) using filter pack system. In general, the pH in rainwater was frequently higher than 5.0. However, the trend of lower pH was observed during the winter and the beginning of autumn (from Nov. to Apr.). Interestingly, the highest frequency of the acidifying rainwater (32 %) and the lowest pH value (min. pH = 4.0) were observed in Hoabinh site. Acidic pH of rain water was also observed in Viettri (no. 3) and Hanoi (no. 4), indicating the local effects of human and industrial activities. Ca2+ and SO4 2? were generally found as predominant in both rainwater and aerosol. SO2 and NH3 in Hanoi and Hoabinh were monitored out of corresponding environmental features.  相似文献   

17.
This paper outlines the results to date of the continuing acidic deposition study from 1997 in three teak plantations at the Na Pralan, Klangdong, and Donglan villages of Thailand. The aim of this study was to examine the impact on teak plantations of acid deposition — the increasing flow of chemical compounds including CO2, SO2, NO2, and NOx into the atmosphere. The 1997–1999 results showed no symptoms of acidity of the precipitation in the teak plantations at the treated sites (Na Pralan and Klangdong). During this period, the pHs of stemflow and throughfall were still over 7; and the pHs of the rainfall were around 7, except at Klandong where it dropped to around 5 in 1999. The pH and EC values were higher at the polluted sites than at the control site; this may be attributed to contamination with lime dust from nearby industrial plants, including cement factories and quarrying mills. Fresh leaves were contaminated with Sulphur to quite high levels at the Na Pralan site. This contamination seems to have affected the physiology, biomass and chemical content of the leaves. It might be due to pollution gases (SO2 and NOx) from the heavy trucks on the nearby Phaholyothin road. However, these gases could not be detected by a gas detector even though pollution seemed quite heavy. This study did not detect acid rain damage to the teak plantations.  相似文献   

18.
The size- and time-resolved indoor/outdoor aerosol concentration relationships were studied experimentally in an empty office without internal particle sources. Two Scanning Mobility Particle Sizers (SMPS) and an Aerodynamic Particle Sizer (APS) sampled alternately from indoor and outdoor, together covering the size range 3–10,000 nm. The results showed that the indoor aerosol concentration depends mainly on the air exchange and deposition rates, and the outdoor concentration. At higher air exchange rates the indoor aerosol concentration approaches the outdoor one. This was observed for the accumulation mode particles. The size-dependent deposition rates were estimated using a simple aerosol dynamics experiment. It was based on equilibration of the indoor/outdoor concentrations by opening windows and analyzing the concentration decay curves after the windows were closed. For this purpose a simple mass balance model was used. The overall loss rate and the asymptotic value of indoor concentration were found by applying a non-linear least squares method on the time dependence of the indoor concentrations. The air exchange rate was estimated from the overall loss rate and the steady state values of the indoor/outdoor concentration of the accumulation mode particles.  相似文献   

19.
Dry deposition velocity estimates of SO, HNO3 and SO4 2? were computed for six locations in eastern North America using two different inferential models; a Big-Leaf model utilized by the U. S. National Dry Deposition Network (NDDN) and, a land-use based model (LUM) that has been used in the past to estimate the relative importance of dry versus wet deposition over selected Canadian regions. There were consistent differences between models that were related to the surface type, chemical species and time of year. Mean monthly dry deposition velocities based upon the 1990–91 time period were compared at two locations. The seasonal cycles in deposition velocity were similar between models, but there were considerable differences in the amplitude of the cycles. The LUM predicted about a 400% increase in S042- deposition velocity from the winter to the summer months, while there was a 50 to 100% increase in the NDDN model estimates, depending upon location. According to the LUM, HN03 deposition to crop land increased by about a factor of 6 from winter to summer, while the big leaf model predicted a 50% increase. Overall, there was better agreement for SO2. Averaged over 12 months, the differences in deposition velocity between models were smaller and generally within the range of uncertainty associated with inferential models. For all six sites, the mean percent difference between models in deposition velocity for SO2, HNO3 and SO4 2? were 13, 35 and 79, respectively. These differences highlight the effect of using different methods for estimating dry deposition and the importance of applying the same model when examining regional patterns in dry/total deposition rates.  相似文献   

20.
Lycopodium spores were released steadily into the air during 20–30 min from a line source positioned within a wheat crop. The spores were trapped on sticky strips held at angles, π, of 0, 30, 60 and 90° with respect to the horizontal and oriented to face the mean wind direction and on sticky, vertical glass rods. The aerial spore concentration, C, was measured by small suction traps. Deposits of the spores on wheat leaves were obtained from sections of leaves whose posture in the canopy was nearly horizontal, nearly vertical, or at angles between 30 and 60°. Number of spores per m2 for all trapping surfaces were obtained by counting under a microscope. Experiments were conducted on seven different days, encompassing friction velocities, u*, of 0.27–0.50 m s−1. The rate of deposition on angled surfaces, D(π), was given approximately by D(θ) = D(0) cos (θ) + D(90) sin (θ), where D(0) and D(90) were the observed rate of deposit on horizontal and on vertical surfaces, respectively. Below mid-canopy height, inertial impaction of spores was negligible, so that D(90) = 0 for all the trap surfaces. There, D(0) was mainly due to sedimentation and was very nearly equal to vs·C, where vs is the settling speed of the spore in still air. Near the top of the canopy, deposition on sticky surfaces was enhanced by inertial impaction and turbulent deposition, so that D(0) was about twice that expected from sedimentation and D(90) was about five times larger than expected from inertial impaction at the mean wind speed. Nevertheless, considering the vertical distribution of leaf area and the angles of leaves in a wheat canopy, the rate of deposition of spores for the entire depth of a wheat canopy can be calculated with a probable underestimation of only 20% by simply assuming sedimentation on horizontally projected area and impaction on vertically projected area.  相似文献   

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