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1.
ABSTRACT

Land use data are among the inputs used to determine dry deposition velocities for photochemical grid models such as the Comprehensive Air Quality Model with extensions (CAMx) that is currently used for attainment demonstrations and air quality planning by the state of Texas. The sensitivity of dry deposition and O3 mixing ratios to land use classification was investigated by comparing predictions based on default U.S. Geological Survey (USGS) land use data to predictions based on recently compiled land use data that were collected to improve biogenic emissions estimates. Dry deposition of O3 decreased throughout much of eastern Texas, especially in urban areas, with the new land use data. Predicted 1-hr averaged O3 mixing ratios with the new land use data were as much as 11 ppbv greater and 6 ppbv less than predictions based on USGS land use data during the late afternoon. In addition, the area with peak O3 mixing ratios in excess of 100 ppbv increased significantly in urban areas when deposition velocities were calculated based on the new land use data. Finally, more detailed data on land use within urban areas resulted in peak changes in O3 mixing ratios of ~2 ppbv. These results indicate the importance of establishing accurate, internally consistent land use data for photochemical modeling in urban areas in Texas. They also indicate the need for field validation of deposition rates in areas experiencing changing land use patterns, such as during urban reforestation programs or residential and commercial development.  相似文献   

2.
Measurements of the dry deposition velocity of O3 to material samples of calcareous stone, concrete and wood at varying humidity of the air, were performed in a deposition chamber. Equilibrium surface deposition velocities were found for various humidity values by fitting a model to the time-dependent deposition data. A deposition velocity-humidity model was derived giving three separate rate constants for the surface deposition velocities, i.e. on the dry surface, on the first mono-layer of adsorbed water and on additional surface water. The variation in the dry air equilibrium surface deposition velocities among the samples correlated with variations in effective areas, with larger effective areas giving higher measured deposition velocities. A minimum for the equilibrium surface deposition velocity was generally measured at an intermediate humidity close to the humidity found to correspond to one mono-layer of water molecules on the surfaces. At low air humidity the equilibrium surface deposition velocity of O3 was found to decrease as more adsorbed water prevented direct contact of the O3 molecules with the surface. This was partly compensated by an increase as more adsorbed water became available for reaction with O3. At high air humidity the equilibrium surface deposition velocity was found to increase as the mass of water on the surface increased. The deposition velocity on bulk de-ionised water at RH=90% was an order of magnitude lower than on the sample surfaces.  相似文献   

3.
A numerical model of atmospheric pollutant dispersion was developed in order to analyse the effects of a plant canopy on air concentrations. The increase in surface roughness is shown to significantly influence the concentration distributions. Moreover the integrated velocities of deposition and the plume depletion are evaluated for particles and SO2 passing over wooded strips. The model is particularly useful to learn how and where dry deposition occurs in high canopies such as forests.  相似文献   

4.
Determining the destructions of both ozone and odd oxygen, Ox, in the nocturnal boundary layer (NBL) is important to evaluate the regional ozone budget and overnight ozone accumulation. This work develops a simple method to determine the dry deposition velocity of ozone and its destruction at a polluted nocturnal boundary layer. The destruction of Ox can also be determined simultaneously. The method is based on O3 and NO2 profiles and their surface measurements. Linkages between the dry deposition velocities of O3 and NO2 and between the dry deposition loss of Ox and its chemical loss are constructed and used. Field measurements are made at an agricultural site to demonstrate the application of the model. The model estimated nocturnal O3 dry deposition velocities from 0.13 to 0.19 cm s?1, very close to those previously obtained for similar land types. Additionally, dry deposition and chemical reactions account for 60 and 40% of the overall nocturnal ozone loss, respectively; ozone dry deposition accounts for 50% of the overall nocturnal loss of Ox, dry deposition of NO2 accounts for another 20%, and chemical reactions account for the remaining 30%. The proposed method enables the use of measurements made in typical ozone field studies to evaluate various nocturnal destructions of O3 and Ox in a polluted environment.  相似文献   

5.
Numerical sensitivity tests and four months of complete model runs have been conducted for the Routine Deposition Model (RDM). The influence of individual model inputs on dry deposition velocity as a function of land-use category (LUC) and pollutant (SO2, O3, SO2−4 and HNO3) were examined over a realistic range of values for solar radiation, stability and wind speed. Spatial and temporal variations in RDM deposition velocity (Vd) during June – September 1996 time period generated using meteorological input from a mesoscale model run at 35 km resolution over north-eastern North America were also examined. Comparison of RDM Vd values to a variety of measurements of dry deposition velocities of SO2, O3, SO2−4 and NHO3 that have been reported in the literature demonstrated that RDM produces realistic results. Over northeastern NA RDM monthly averaged dry deposition velocities for SO2 vary from 0.2 to 3.0 cm s−1 with the highest deposition velocities over water surfaces. For O3, the monthly averaged dry deposition velocities are from 0.05 to 1.0 cm s−1 with the lowest values over water surfaces and the highest over forested areas. For HNO3, the monthly averaged dry deposition velocities have the range of 0.5 to 6 cm s−1, with the highest values for forested areas. For SO2−4, they range from 0.05–1.5 cm s−1, with the lowest values over water and the highest over forest. The monthly averaged dry deposition velocities for SO2 and O3 are higher in the growing season compared to the fall, but this behaviour is not apparent for HNO3 and sulphate. In the daytime, the hourly averaged dry deposition velocities for SO2, O3, SO2−4 and HNO3 are higher than that in the nighttime over most of the vegetated area. The diurnal variation is most evident for surfaces with large values for leaf area index (LAI), such as forests. Based on the results presented in this paper, it is concluded that RDM Vd values can be combined with measured air concentrations over hourly, daily or weekly periods to determine dry deposition amounts and with wet deposition measurements to provide seasonal estimates of total deposition and estimates of the relative importance of dry deposition.  相似文献   

6.
The distribution of aerosol particles in the troposphere is described. Starting with long term mean seasonal flow and diffusivities as well as temperature, cloud distribution (six cloud classes), relative humidity and OH radical concentration, the steady state concentration of aerosol particles and SO2 are calculated in a two-dimensional global (height and latitude) model. The following sources and sinks for particles are handled: direct emission, gas-to-particle conversion from SO2, coagulation, rainout, washout, gravitational settling, and dry deposition. The sinks considered for sulphur emissions are dry deposition, washout, rainout, gasphase oxidation, and aqueous phase oxidation. Model tests with the water vapour cycle show a good agreement between measured and calculated zonal mean precipitation distribution.The steady state concentration distribution for natural emissions reached after 10 weeks model time, may be described by a mean exponent α = 3.2 near the surface assuming a modified Junge distribution and an increased value, α = 3.7, for the combined natural and man-made emission. The maximum ground level concentrations are 2000 and 10,000 particles cm−3 for natural and natural plus man-made emissions, respectively. The resulting distribution of sulphur dioxide agrees satisfactorily with measurements given by several authors.  相似文献   

7.
This paper reports on progress to date of an ongoing effort to develop, evaluate and apply a European Regional Model of Air Pollution (EURMAP). This model is capable of calculating longterm (monthly, seasonal and/or annual) averages of the contributions from SO2 in individual emittor countries to SO2 and SO42− concentrations, dry deposition and wet deposition in receptor countries. The model covers all of western and central Europe, a geographical area 2100 km × 2250 km in size. A trajectory-type approach is used, which involves the tracking of pollutant ‘puffs’ released from each emissions cell in an extensive 32 × 36 grid. Meteorological data in the form of wind and precipitation values from some 45 upper-air and 535 surface stations are input at 6-hourly intervals for use in the calculations of puff transport and wet deposition. A wet deposition coefficient is used that depends upon precipitation rate.The preliminary model has been used to calculate annualized as well as monthly mean maps for January, April, July and October 1973 of SO2 and SO42− concentration, dry deposition and wet deposition patterns resulting from SO2 emissions in 13 countries in western and central Europe. The dry and wet deposition patterns are presented, along with values of calculated international exchanges of SO2 and SO42− wet and dry deposition among these various countries. The EURMAP results are compared with those from Fisher's (1975) model and the LRTAP model (Ottar, 1978; OECD, 1977). In many (but not all) respects the results from the three models are similar. The possible reasons for the differences revealed by this comparison are examined.  相似文献   

8.
Estimates of short-term, regional-scale spatial distributions of ozone (O3) and hydrogen peroxide (H2O2) dry deposition over the northeast U.S. are presented. Dry deposition fluxes to surfaces are computed using a regional tropospheric chemistry model with deposition velocities which vary with local meteorology, land type, insolation, seasonal factors and surface wetness. A compilation of O3 surface resistances is presented based on a survey of O3 dry deposition measurements. The surface resistance for H2O2 is assumed to be small under most conditions, causing H2O2 to dry deposit at a rate which is frequently limited by surface-layer turbulence. Regional patterns of dry deposition velocities for these oxidants over the northeast U.S. are computed using landuse data and meteorological information predicted using a mesoscale meteorology model. Domain-averaged O3 deposition velocities during a spring period reach a mid-day peak of 0.7–0.8 cm s−1 and drop to 0.1–0.2 cm s−1 at night. Domain-averaged H2O2 deposition velocities at a height of approximately 80 m are predicted to reach a mid-day peak of 1.6–2.0cm s−1, and fall to 0.6–0.9 cm s−1 at night. Time-averaged surface-layer H2O2 concentrations show a latitude dependence, with higher concentrations in the south. H2O2 concentrations are significantly reduced due to efficient wet removal and chemical destruction during the passage of a cyclonic frontal system. In contrast, O3 concentrations are predicted to rise during the passage of a frontal system due to efficient vertical exchange of midtropospheric air into the boundary layer during convective conditions, followed by synoptic-scale subsidence occurring in the high pressure airmass following a cyclone. Maximum O3 deposition during this 3-day springtime period occurs in polluted agricultural areas. In contrast, H2O2 dry deposition exhibits a latitude dependence with maximum 3-day accumulations occurring in the south. Domain-averaged mid-day deposition rates for O3 and H2O2 were 45–50 μmol m−2 h−1 and 4–5 μmol m−2 h−1. At night, deposition rates were approximately 5–10 μmol m−2 h−1 and 1.5–2.5 μmol m−2 h−1 for O3 and H2O2. These model results show that regional patterns of oxidant dry deposition are strongly influenced by oxidant concentrations, atmospheric stability, surface roughness and numerous other surface and meteorological factors. Each of these factors must be well-characterized before regional patterns of biological damage associated with oxidant dry deposition can be quantified.  相似文献   

9.
A mathematical dry deposition model was developed and an experiment performed to verify that the interfacial transfer velocity (V(S)) of ozone dry deposition includes the interfacial reactive velocity (V(Sr)) and interfacial kinetic velocity (V(Sk)), as determined by measuring the ozone depletion over agricultural field soils in a dry deposition chamber. Experimental results indicate that the chemical reaction (O3 + NO --> NO2 + O2) produces the reactive velocity. Observed interfacial transfer velocities depend on nitrogen oxide emission (NO) and soil temperature (T(S)). Additionally, observed kinetic velocities of conditioned field soils increased linearly with soil temperature. Moreover, observed reactive velocities of field soils increased exponentially with soil temperature, and depend on the emission rate of nitrogen oxide. Results in this study demonstrate that interfacial transfer velocities are variable velocities for long-term transportation, that influenced factors are chemical kinetics, thermodynamics and biochemical mechanisms.  相似文献   

10.
This paper describes the development of a detailed dry deposition model for routine computation of dry deposition velocities of SO2, O3, HNO3 and fine particle SO42− across much of North America. Four different dry deposition/surface exchange sub-models have been combined with the current Canadian weather forecast model (Global Environmental Multiscale model) with a 3 h time resolution and a horizontal spatial resolution of 35 km. The present model uses the US Geological Survey North American Land Cover Characteristics data to obtain fourteen different land use and five seasonal categories. The four sub-models used are a multi-layer model for gaseous species over taller canopy land-use types, a big-leaf model for gaseous species over lower canopies (including bare soil and water) and for HNO3 under all surface types and, two different models for SO42−, one for tall canopies and the other for short canopies. All necessary parameters for each sub-model, chemical species, land-use and seasonal categories have been selected from available data libraries or from the values reported in the literature. The purpose for developing this model (referred to as the Routine Deposition Model (RDM)), when coupled with air concentration data, is to provide estimates of seasonal dry deposition, which can be combined with wet deposition to produce total deposition estimates. Model theory is discussed in this paper and model sensitivity tests and results will be presented in a companion paper.  相似文献   

11.
The dry deposition velocities and fluxes of ammonia have been estimated from measurements of the vertical gradient of ammonia and micrometeorology above a spruce forest in western Jutland, Denmark. Measurements have been made in seven periods, each lasting about one week and covering all seasons and different meteorological situations. Different deposition characteristics were observed, depending on the ammonia concentration and the relative humidity. At conditions with westerly winds, the wind brings air masses from the North Sea with low concentration levels of ammonia to the site, while at conditions with easterly winds, the air have passed central Jutland with large emission areas. Some of the relatively low deposition velocities or emissions were observed during conditions with low ammonia concentration and westerly winds. These observations might relate to a compensation point of the forest, i.e. an ammonia concentration below which the trees and/or the surface emit ammonia due to an equilibrium with the ammonia inside the needles or on the surface. Emission of ammonia was also observed at relatively high ammonia concentration levels (above 2 μg NH3–N m-3), mainly during one measuring period characterized by easterly winds with dry conditions and high ammonia concentrations, and the emissions might relate to evaporation from ammonia saturated surfaces or emission from mineralization in the forest soil. In general, relatively high net deposition velocities were observed during conditions with relative humidity above 80% or at ammonia concentrations moderate higher than a given (temperature dependent) compensation point. During stable conditions some observations revealed that the gradient above the canopy not necessarily represents the exchange with the canopy.  相似文献   

12.
In a land- and sea-breeze situation, effects of dry deposition on the dynamics of the concentrations of chemically reacting air pollutants are investigated using a transport/transformation/removal model with diurnally varying deposition velocities modeled in terms of the aerodynamic, surface, and residual resistances. The results show that the diurnally varying flows and eddy diffusivities, which are characteristic of the landand sea-breeze system, transfer the effects of dry deposition on the concentrations quickly to the upper layer over the land and sea surfaces. The dry deposition effect on one species can be transmitted to others through the network of chemical reactions, e.g. inclusion of dry deposition into the simulation resulted in the increase of hydrocarbon concentrations. It is also predicted that the dry deposition processes could remove a considerable part of emitted NOx, and SO2 from the local circulations, e.g. for 2 days about 40% of the emitted NOx was removed by the dry deposition of NO, NO2, HNO3 and PAN and in the case of SO2, 25 % by that of SO2 and SO42−.  相似文献   

13.
Wet and dry deposition as collected by a bucket were measured at two sites in southeastern Michigan for two years. The precipitation had an average pH of 4.27 and a SO2−4 to NO3 ratio of 2.0. Particulate dry deposition velocities of 0.6 cm s−1 for SO2−4 and NO3 and > 2 cm s−1 for Cl, Ca2+, Mg2+,Na+ and K+ were calculated. The ambient particle composition, dry bucket collection and wet deposition were compared at two sites, one urban and the other rural. Higher ambient particle concentrations and dry deposition rates were measured at the urban site than the rural site, indicating the influence of local emissions. However, local emissions had no effect on the wet deposition concentrations. The influence of more distant source regions was examined by separating the precipitation events by wind direction. The events from the south and east had the highest SO2−4 to NO3 ratios, which corresponded to the areas with the highest sulfur emissions. NO3 showed no directional dependence.Wet deposition was examined for the effect of storm type and seasonal trends. Contrary to a recent study on Long Island, we found higher concentrations of H+, SO2−4 and NH+4 in winter rain compared to snow. The wet deposition concentrations of H+, SO2−4, and NH+4 were highest in the summer, while only Na+ and Cl concentrations were highest in the winter, presumably due to winter road salting. The total deposition of acidic ions was highest in the summer and lowest in the winter, due both to lower concentrations and lower precipitation volumes in the winter. The dry deposition as collected by a bucket accounted for 1 % of total H+ deposition, 21 % of SO2−4 deposition, 27% of NO3 deposition, 50% of Cl deposition and 61 % of Ca2+ deposition.  相似文献   

14.
A general relationship between roadway tunnel air quality and vehicle emissions has been derived. The model includes the effect of pollutant deposition on the tunnel surfaces and dilution from ventilation. The model is applied to air quality measurements of SO2 and particulates obtained at the Tuscarora Mountain Tunnel. It is found that, if deposition is neglected, SO2 and sulfate emission factors for both gasoline and Diesel vehicles may be underestimated by ~ 10%. The derived deposition velocities are 0.07cms−1 for SO2, 0.03cms−1 for sulfate, and ~ 0.001 cms−1 for total suspended particulates and paniculate components (except sulfate). The last value is lower than smooth-surface values quoted for aerosol deposition, and the difference between the last two values presumably reflects the approximations in the model and/or the uncertainty in its input data.  相似文献   

15.
Land use data are among the inputs used to determine dry deposition velocities for photochemical grid models such as the Comprehensive Air Quality Model with extensions (CAMx) that is currently used for attainment demonstrations and air quality planning by the state of Texas. The sensitivity of dry deposition and O3 mixing ratios to land use classification was investigated by comparing predictions based on default U.S. Geological Survey (USGS) land use data to predictions based on recently compiled land use data that were collected to improve biogenic emissions estimates. Dry deposition of O3 decreased throughout much of eastern Texas, especially in urban areas, with the new land use data. Predicted 1-hr averaged O3 mixing ratios with the new land use data were as much as 11 ppbv greater and 6 ppbv less than predictions based on USGS land use data during the late afternoon. In addition, the area with peak O3 mixing ratios in excess of 100 ppbv increased significantly in urban areas when deposition velocities were calculated based on the new land use data. Finally, more detailed data on land use within urban areas resulted in peak changes in O3 mixing ratios of approximately 2 ppbv. These results indicate the importance of establishing accurate, internally consistent land use data for photochemical modeling in urban areas in Texas. They also indicate the need for field validation of deposition rates in areas experiencing changing land use patterns, such as during urban reforestation programs or residential and commercial development.  相似文献   

16.
A modeling study was conducted on dispersion and dry deposition of ammonia taking one hog farm as a unit. The ammonia emissions used in this study were measured under our OPEN (Odor, Pathogens, and Emissions of Nitrogen) project over a waste lagoon and from hog barns. Meteorological data were also collected at the farm site. The actual layout of barns and lagoons on the farms was used to simulate dry deposition downwind of the farm. Dry deposition velocity, dispersion, and dry deposition of ammonia were studied over different seasons and under different stability conditions using the short-range dispersion/air quality model, AERMOD. Dry deposition velocities were highest under near-neutral conditions and lowest under stable conditions. The highest deposition at short range occurred under nighttime stable conditions and the lowest occurred during daytime unstable conditions. Significant differences in deposition over crop and grass surfaces were observed under stable conditions.  相似文献   

17.
This paper describes a methodology for estimating the effect of local source emissions on dry deposition of sulfur dioxide in regions of complex terrain. Airflow in complex terrain is simulated by a time-dependent dynamical model for the meteorological fields. The results of the dynamical model are used to drive a semi-stochastic Lagrangian dispersion model in order to evaluate concentrations resulting from local source emissions. The Lagrangian dispersion model is coupled with a dry deposition treatment which includes the effects of both surface properties and micrometeoroiogical factors on deposition.

A sample application is discussed for a source in the Shenandoah Valley. The largest concentrations and deposition rates were obtained shortly after sunrise, during the transition from the nocturnal to the daytime flow regime. These results suggest that dry deposition may be episodic.  相似文献   

18.
A combined transport/chemistry model which simulates the regional distribution of SO2 and sulfate within the lower troposphere is described. The mathematical analysis is based on the coupled three-dimensional advection-diffusion equations for SO2 and sulfate, and incorporates chemical transformations as well as the physical phenomena of dry deposition at the surface. The analysis also considers spatial variations in topography and spatial and temporal variations in both the mixing layer heights and the wind field. Based on the results from a series of numerical experiments, the dynamic model employs a Galerkin method for the numerical solution of the partial differential equations.A SO2 photochemical oxidation mechanism is incorporated into the transport model. The SO2 photochemical oxidation rate is based on a set of 27 reactions used to estimate the hydroxyl and peroxyl radical concentrations. The kinetic mechanism has been tested in simulations of smog chamber studies and yields realistic concentrations and conversion rates in model simulations of both urban and natural tropospheres.Other major facets treated in the formulation of the model include the interpretation and use of data available on dry deposition and the development of procedures to calculate meteorological model inputs (e.g., eddy diffusivities, dry deposition velocities, the three components of wind velocity, etc.) from routinely measured meteorological data. Simulations using the analysis are presented in a companion paper.  相似文献   

19.
Region-to-grid source–receptor (S/R) relationships are established for sulfur and reactive nitrogen deposition in East Asia, using the Eulerian-type Community Multiscale Air Quality (CMAQ) model with emission and meteorology data for 2001. We proposed a source region attribution methodology by analyzing the non-linear responses of the CMAQ model to emission changes. Sensitivity simulations were conducted where emissions of SO2, NOx, and primary particles from a source region were reduced by 25%. The difference between the base and sensitivity simulations was multiplied by a factor of four, and then defined as the contribution from that source region. The transboundary influence exhibits strong seasonal variation and generally peaks during the dry seasons. Long-range transport from eastern China contributes a significant percentage (>20%) of anthropogenic reactive nitrogen as well as sulfur deposition in East Asia. At the same time, northwestern China receives approximately 35% of its sulfur load and 45% of its nitrogen load from foreign emissions. Sulfur emissions from Miyakejima and other volcanoes contribute approximately 50% of the sulfur load in Japan in 2001. Sulfur inflows from regions outside the study domain, which is attributed by using boundary conditions derived from the MOZART global atmospheric chemistry model, are pronounced (10–40%) over most parts of Asia. Compared with previous studies using simple Lagrangian models, our results indicate higher influence from long-range transport. The estimated S/R relationships are believed to be more realistic since they include global influence as well as internal interactions among different parts of China.  相似文献   

20.
Dry deposition and removal in precipitation of SO2 and of paniculate sulphate are considered in turn. Many assessments of the dry deposition of SO2 to various surfaces give deposition velocities of about 0.8cm s−1, although variations with season and weather conditions are important. The deposition velocity of the sulphate aerosol is probably about 0.l cm s−1. Removal of SO2 in rain is also a rather inefficient process and theoretical and experimental results suggest that the sulphur in precipitation results chiefly from the rainout of cloud condensation nuclei. The removal time constants for SO2 and sulphate by moderate rain are probably of order 10−5 and 10−4s−1 respectively. A much simplified model suggests that about a half of the SO2 emitted to the atmosphere is removed by dry deposition, the remainder is oxidised to sulphate and removed in precipitation and the atmospheric residence time is about 5 days for sulphur. The method and climatological statistics for a more realistic treatment do not yet appear to be available.  相似文献   

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