Numerical simulation of transport from a point source: error analysis

The techniques used to represent point sources in numerical air pollution models have received little attention.However, an inadequate representation of these sources can lead to significant loss of solution accuracy. Kasibhatla et al. (1988, Atmospheric Environment22, 75–82) have performed a parametric error analysis for the two-dimensional transport of an inert species from an infinite line source. This paper extends the analysis to three-dimensional problems.Numerical results for an inert plume emanating from a single point source shown that the radio of the advection time scale to the turbulent time scale in the vertical direction, K_zΔx/uΔy², as well as the ratio of the advection time scale to the turbulent diffusion time scale in the cross-wind direction, K_yΔx/uδy², have an effect on solution accuracy. In addition, comparisons between the volume-averaged representation of a point source and the use of an irregular grid for point source representation demonstrate that, near the source, improved results can be obtained by placing a node at the source location. Numerical results for the case in which the wind velocity vector is not aligned with tghe grid lines indicate that the cross-derivative diffusion term can be negleted without loss of accuracy.     

Large-eddy simulation of a turbulent reacting plume

The results of large-eddy simulations (LES) of a chemically reacting, dispersing plume in a turbulent boundary layer are presented. The detailed simulations of the dispersion mechanisms are used to investigate the effects of turbulent fluctuations on nonlinear chemical reactions. The idealized single reaction between ozone and nitrogen oxides, NO+O₃→NO₂+O₂, is used as a representative simple, irreversible binary reaction. Effects of different reaction rates are investigated by varying the source NO concentration, while maintaining a constant ambient ozone level. The simulations demonstrate that the rate of production of NO₂ is significantly affected by the turbulent nature of the dispersing plume. The effect of incomplete turbulent mixing of the two reactants on the reaction rate can persist for long distances downstream, particularly for the high NO levels typical of power plant stacks. The LES results also show that the important measure of the turbulent fluctuations, the turbulence segregation coefficient, may be reasonably approximated by a constant value over most of the plume cross-section. This result may prove useful for simplified plume modeling, but will depend on whether the range of constant segregation coefficient covers the whole reaction region since this takes place predominantly in the plumeedges.     

Building wake dispersion at an Arctic industrial site: Field tracer observations and plume model evaluations

Ten multi-hour atmospheric dispersion SF₆ tracer experiments were conducted during October and November of 1987 near a large oil gathering facility in the Prudhoe Bay, Alaska, oilfield reservation. The purpose of this study was to investigate dispersion under arctic conditions and in situations where building-generated airflow disturbances dominate downwind distributions of ground level pollutant concentrations. This was accomplished with a network of micrometeorological instruments, portable syringe tracer samplers, continuous tracer analyzers, and infrared visualization of near source plume behavior.Atmospheric stability and wind speed profiles at this arctic site are influenced by the smooth (surface roughness = 0.03 cm), snow covered tundra surface which receives negligible levels of solar isolation in winter. The dispersion of pollutants emitted from sources within the oil gathering facility, however, is dominated by the influence of nearby buildings when high winds generate elevated ground level concentrations. An order of magnitude increase in maximum ground level concentration was observed as wind speeds increased from 5 to 8 m s⁻¹ and another order of magnitude increase was observed as winds increased from 8 to 16 m s⁻¹. Variation in maximum concentrations was also observed with changes in wind direction. Vertical plume diffusion (σ_z) near the buildings was a factor of 2–3 greater than that observed in open terrain and was dependent on both wind speed and the projected building width and location of nearby buildings. Wind tunnel tracer distributions for east winds agree with field observations but also indicate that a significant increase in plume downwash occurs with other wind directions. Concentration distributions were calculated using several versions of the Industrial Source Complex (ISC) model. Model estimates of ground level concentrations were within a factor of three depending on wind direction. The model predictions are extremely sensitive to the ratio of plume height to vertical plume diffusion which is significantly influenced by a complex aerodynamic wake in the field.     

Comparison of three dry deposition models applied to field measurements in the Southern Bight of the North Sea

Dry deposition velocities have been calculated using three different approaches. Turbulent wind profile theory has been used to predict the drag coefficient, wind speed and friction velocity at 10 m height when the wind speed is measured at a higher altitude. The resulting parameters were introduced in a two-layer deposition model. The second approach was the well-known model of Slinn and Slinn (1980, Atmospheric Environment14, 1013–1016), whereas the third corresponded to the model published by Williams (1982, Atmospheric Environment16, 1933–1938). Results point to clear differences. However, in a field experiment carried out at the Southern Bight of the North Sea, all three approaches show relatively comparable results. The role played by the size distribution of atmospheric particulate matter is essential. In our case any of the three models could have given satisfactory outcomes taking into account the wide spread of the experimental results cited in the literature for the same airshed.     

Aerosol formation and growth in atmospheric organic/NOχ systems—II. Aerosol dynamics

Aerosol dynamics that were observed in the outdoor smog chamber experiments described in Wang et al. (1992, Atmospheric Environment, 26A, 403–420) aresimulated by numerical solution of the aerosol general dynamic equation. The vapor source generation rate was estimated directly from the experimental measurements assuming a single surrogate condensing species for each hydrocarbon studied. Sensitivity analysis of the simulated aerosol dynamics to various input parameters revealed that the physical properties of the condensing vapor are important in determining the interplay between nucleation and condensation while the vapor source generation rate is the only factor that determines the eventual total amount of vapor converted to aerosol. The simulations suggest that over 99% of the mass of condensible vapor is converted to aerosol by condensation even when a significant burst of nucleation occurs.     

Mathematical modeling of cloud chemistry in the Los Angeles basin

A mathematical model of cloud chemistry was evaluated with the cloud chemistry data collected by Richardset al. (1983,Atmospheric Environment17, 911–914) from 1981 to 1985 in stratus clouds in the Los Angeles Basin. The model simulates atmospheric chemistry including gas-phase chemistry, aqueous-phase chemistry and droplet mass transfer, vertical transport, rainfall and turbulent diffusion.Evaluation of the model entailed two major part. First, the equilibrium chemistry is evaluated with a total of 52 case studies. Then, the model with treatment of cloud chemistry, vertical transport and diffusion is evaluated with two case studies. The results of the model simulations show the importance of vertical transport in determining the chemical composition of stratiform clouds.The sensitivity of sulfate, nitrate, ammonium and hydrogen ion concentrations to precursor levels, various chemical kinetic and cloud microphysical parameters and various environmental conditions is discussed.     

The removal of sulphur dioxide in a long-lived line echo system: A numerical study

The removal of SO₂ in precipitation systems is not only a major sink of SO₂ but is also directly related to the acidity of precipitation. However the physical and chemical processes are not well understood due to their complicated characteristics. The lack of measurements also hinders us from studying those processes. In order to investigate what mechanisms are important about the removal of SO₂ in precipitation systems, an alternative approach is to examine the simulation result from a numerical cloud model.A two-dimensional version of the Klemp-Wilhelmson numerical model (1978, J. atmos. Sci.35, 1070–1096) is used to simulate a fast-moving long-lived line echo precipitation system that occurred in the Taiwan area during Mei-Yu season. The simulation model was assumed to be perpendicular to the north-south orientated line echo. In this simulation an artificial source of SO₂ is placed in front of the line echo system in the low level. As the line echo system approaches the region of SO₂, some SO₂ is brought into the line echo system through advection and diffusion effects. A simple parameterization scheme similar to Fisher's (1982, Atmospheric Environment16, 775–783) is used to represent the removal of SO₂ by cloud and rain. The model results show that the major sink of SO₂ is removed by rain below the cloud base although some is removed by cloud and rain inside the precipitation system itself.     

Diurnal variation of OH radical and hydrocarbons in a polluted air mass during long-range transport in central Japan

Long-range transport (LRT) of photochemical air pollution from the coastal area, with large emission sources to the inland mountainous region, occurs frequently in central Japan on clear summer days. Hydrocarbons and other pollutants were measured together with meteorological parameters along this route, and the diurnal variations of OH radical and hydrocarbons in the polluted air mass were investigated in relation with these photochemical reactions.At inland sampling sites, hydrocarbon concentrations in a polluted air mass decreased during LRT in the daytime. In particular, olefins were destroyed significantly because of more active photochemical reactions. From these destruction rates and/or O₃ formation rates the OH radical concentration was estimated and found to increase from 0.5 × 10⁻⁷ in the morning to a maximum of 8.0 × 10⁻⁷ ppm at midday. These values, as well as the diurnal variation, compared well with the numerical result of the comprehensive transport/reaction/removal model (Chang et al., 1989, Atmospheric Environment23, 363–393, 1749–1773). The contribution of each hydrocarbon component to the total hydrocarbon destruction was also discussed.     

Parallel processing of a random-walk model of atmospheric dispersion

Algorithms for random-walk models of atmospheric dispersion take considerable processing time on sequential computers. Such algorithms are, however, more suited to parallel computers as they contain a high degree of parallelism. In this paper, to show this suitability and to investigate the improvement in the processing time with the use of a parallel computer, the model algorithm developed and applied in Luhar and Britter (1989, Atmospheric Environment23, 1911–1924) has been implemented on a Distributed Array of Processors (DAP). The results show a 14-fold improvement in the processing time over a sequential machine.     

The use of Procrustes Target Analysis to discriminate dominant source regions of fine sulfur in the western U.S.A.

Receptor modeling, using Procrustes Target Analysis (PTA), was applied to a fine sulfur data set to discriminate dominant sources and areas of influence in the western U.S.A. The work presented in this note is closely linked to a paper published by Malm et al. (Atmospheric Environment24, 3047–3060, 1990), which used two different analyses, area of influence analysis (AIA) and rotated principal component analysis (RPCA), to show similar areas of influence for most source regions in the western U.S.A. A critical examination of RPCA revealed that two issues might confound interpretations. These are (i) eigenvalue degeneracy combined with trying to fit nine orthogonal dimensions pairwise in the PC space and (ii) statistical issues related to missing data and eigenvector truncation. In determining how much of the AIA results are present in the data spanned by the PC space, our findings indicated a 164% improvement in the variance overlap when PTA was substituted for RPCA.     

Indoor air pollution by organic emissions from textile floor coverings. Climate chamber studies under dynamic conditions

The time dependence of the emission of organic compounds from a polyamide floor covering with styrene-butadiene-rubber (SBR) backing was studied in three climate chambers (0.03, 1.0 and 38 m³) at 23°C 5nd 45% RH. While volatile compounds such as toluene reach a maximum concentration in the gas phase within 1 h and decrease in concentration to less than 2% within 60 h, the concentration of less volatile compounds, such as 4-phenylcyclohexene, decreases slowly over a period of months.If the chamber is well mixed and a defined chamber loading is maintained the observed concentrations do not depend on the chamber size, the wall material and air velocity. The concentration of the observed emissions is roughly proportional to the chamber loading. Surprisingly it is not inversely proportional to the air exchange rate. Rather, at high air exchange rates mass transfer from the carpet to the gas phase is enhanced.The “decreasing source models” of Dunn and Tichenor (Atmospheric Environment22, 885–894, 1988) have been applied to the data. They allow the extrapolation of experimental data beyond the time available for measurement.The model calculations reveal the presence of sink effects. The role of the chamber walls as sinks can be determined more reliably if constant sources of an organic compound are placed into the chamber and their increase in concentration with time is compared with the theoretical predictions neglecting sink effects.     

Proportionality between SO2 emissions and wet SO42− concentrations: The effect of area of averaging

An earlier analysis of empirical associations between SO₂ emissions and wet SO₄²⁻ concentrations in central North America (Hilst and Chapman, 1990, Atmospheric Environment 24A, 1889–1901) showed that local wet SO₄²⁻ concentrations were not proportional to SO₂ emissions averaged over areas up to ∼10⁶ km². Because it is axiomatic that at a global level of averaging a proportionality between total S emissions and S deposition should exist, we have extended these analyses in an attempt to determine whether there is proportionality between S emissions and wet SO₄²⁻ deposition. We have found that for the eastern half of central North America (an area of about 4.3 × 10⁶ km²), the annual average wet SO₄²⁻ concentration exhibits a linear-proportional dependence on anthropogenic SO₂ emissions. However, the internal structure of this association for subareas of the eastern half of central North America suggests the “global” proportionality is achieved by a combination of imported SO₂ from major source areas and an oxidant-limited conversion of SO₂ to SO₄²⁻ within the major source areas. If this inference is even approximately correct, a rollback SO₂ control strategy for the eastern United States and southeast Canada should result in an immediate proportional decrease in wet SO₄²⁻ concentrations in minor SO₂ source areas, but no appreciable reduction of wet SO₄²⁻ concentrations in major SO₂ source areas until the oxidant limitation has been overcome.     

An intercomparison of semiempirical diffusion models under low wind speed,stable conditions

The performances of some diffusion models are analysed using concentration data measured at ground level up to 400 m from the emission point, in a series of diffusion tests conducted by U.S. National Oceanic and Atmospheric Administration (NOAA) under inversion conditions with light winds. All tested models are simple semiempirical formulae based on the Gaussian formulation, with different assumptions concerning dispersion parameters; each model utilizes a minimum set of information, i.e. vertical stability category, mean wind speed and standard deviation of the horizontal wind direction over the considered averaging time, σ_θ.Results show that for cases with very low wind speed and large plume spread, explicit consideration of diffusion along the mean wind direction, which is neglected in the standard plume model, significantly improves model results; moreover, when σ_θ is very large (greater than 50–60°), the analysis suggests that standard deviations of the horizontal wind speed may significantly differ from the estimates commonly found in the literature.     

A comparison of measurements of atmospheric ammonia by filter packs,transition-flow reactors,simple and annular denuders and fourier transform infrared spectroscopy

Using data obtained during the 1985 Nitrogen Species Methods Comparison Study (1988,Atmospheric Environment22, 1517), several measurement methods for sampling ambient NH₃ are compared. Eight days of continuous measurements at Pomona College, a smog receptor site in Los Angeles, provided an extensive data base for comparing the following methods: Fourier transform i.r. spectroscopy (FTIR), three filter pack configurations, a simple and an annular denuder, and the transition flow reactor. FTIR was defined as the reference method and it reported hourly NH₃ concentrations ranging from > 60 to 2280 nmol m⁻³ (1.5−57ppb) during the course of the study, the highest values coming from the influence of nearby livestock operations.Although only limited quality assurance procedures were carried out, the following conclusions can, nevertheless, be drawn: most of the methods correlated highly with the FTIR method (correlation coefficientr > 0.96); generally, the linear regression slopes were close to unity and the intercepts were insignificantly different from zero at the 95% confidence level); relative to the FTIR average values, (1) for 4–6 h sampling periods, the averages of the three filter packs from three research groups were 83–130% and the annular denuder average was 87%, and (2) for 10–12 h sampling periods, the simple denuder averaged 90% and the two transition flow reactors were 77–98%. Possible reasons for the reported systematic biases are presented, but these are not able to fully explain the large range of differences reported by the various methods.     

A micro-scale dispersion model for motor vehicle exhaust gas in urban areas—OMG volume-source model

A micro-scale dispersion model is presented for estimating the concentration of pollutants from motor vehicle exhaust gas within an area extending 200 m from the side of the road in an urban area. The initial mixing of pollutants in a street canyon is modeled as a volume source employing an analytical solution to the Fickian diffusion equation.Parameters for the model were determined based on data from experiments performed at five locations in Osaka. In the experiments, SF₆ was released as a tracer gas. The height for wind speed measurements for use as the advection speed of the plume was determined from an analysis of the flux of SF₆. The eddy diffusivities in the vertical and lateral directions were derived from statistics of the turbulent velocity fluctuations of the air. The sensitivity analysis of the model revealed that proper characterization of the thickness of the volume source is essential for proper estimation of the concentration of pollutants.     

A Lagrangian particle model of fumigation by breakdown of the nocturnal inversion

Several fumigation modelling studies are reviewed and an approach involving a coupled mesoscale grid point model and a Lagrangian particle dispersion model is chosen for further study. A number of particle model formulations are evaluated for their ability to maintain a well-mixed profile under steady-state convective conditions. The importance of using a formulation of the Langevin equation which is compatible with the specified turbulence parameterization is emphasised. Other considerations such as the form of the parameterizations and the magnitude of the timestep must also be taken into account.For prediction of hourly-averaged surface concentrations under fumigation conditions, it is found that a simple homogeneous turbulence formulation is equally effective as more sophisticated parameterizations involving inhomogeneity and skewness. Such a particle model, in conjunction with a mesoscale model for predicting the growth of the mixed layer, is able to reproduce well the results of the Deardorff and Willis (1982, Atmospheric Environment16, 1159–1170) laboratory experiments on fumigation.     

Wind tunnel measurements of line integrated concentration

Visibility through aerosol plumes is related to the integral of the aerosols concentrations along the line of vision. A novel method for measuring the mean and fluctuating values of such integrals in wind tunnel simulated plumes is presented together with measurements of Vertical Integrated Concentrations (VIC) in a neutrally buoyant plume generated by a ground-level source in a simulated, neutrally stratified atmospheric boundary layer. The data depict the similar structure of the intermittent VIC fluctuations. The relative fluctuations of VIC are shown to be close to the relative fluctuations of the ground-level concentration fluctuations.     

Numerical analysis of the role of sea breeze fronts on air quality in coastal and inland polluted areas

The role of moving sea breeze fronts on air quality in coastal and inland polluted areas was investigated by the numerical simulation of the transport/chemistry of air pollutants, using detailed structures of eddy diffusivity, temperature and flow fields associated with the moving sea breeze fronts. The eddy diffusivity field used was the output of a two-equation turbulence model (i.e. the k-ϵ model) and reasonably well expressed dynamical nature of turbulence in sea breeze, at its front and in an inland mixed layer (Kitada et al., 1987, Proc. Envir. Sani. Eng. Res.23, 103–113). The transport/chemistry of pollutants was calculated using a comprehensive Eulerian model, which adopts more than twenty chemical species advected (Kitada et al., 1983, Proc. 3rd. Int. Symp. on Numer. Methods in Engng, pp. 223–233; Carmichael et al., 1986, Atmospheric Environment20, 173–188).Several cases of numerical simulations were performed, being characterized by the locations of emission sources (i.e. coastal or inland), and the temporal activities of those. Results showed the following. In the coastal-source cases, (1) a circulation behind the sea breeze front was responsible for maintaining high concentration zone of photochemical product, just behind the front; (2) the local maximum of the product's concentration appeared at the upper part of the circulation (i.e. around a height of 500 m), where the temperature profile was stably stratified; (3) the concentration profile was vertically-uniform in the lower part of the circulation, where the thermal internal boundary layer extended over; in the inland-source cases, (4) updraft at the front swept away pollutants into the upper layer. Thus the vertical profile of the pollutant, having a peak at a higher level of 900–1000 m above ground, was formed; (5) this polluted zone at the higher layer remained for several hours after the front passed over. Finally, these indicate that the passage of the sea breeze front can result in complex layering of pollutants.     

Time scales of physical and chemical processes in chemically reactive plumes

The rate of non-linear chemical reactions in a dispersing plume, such as the formation of NO₂, is discussed on the basis of various models and measurements of the oxidation rate of NO. Results of calculations with four different reactive plume models are compared with a set of plume measuremeent and discussed in terms of the ration of the time scales of physical (T_p) and chemical processes (T_c), the Damköhler number:T_p/T_c. In modelling a fast non-linear chemical reaction an interaction between physical processes of dispersion and mixing and chemical reactions can be expected. Models may differ in that they assume either chemical equilibrium (T_p/T_c⪢1) or no chemical equilibbrium (T_p/T_c⪡1).From our study it is concluded that for the first 5 km from a stack concentrations in the plume change more rapidly by dilution due to dispersion of the plume than by chemical reactions. Farther off it is the other way around and the chemistry is fast enough to achieve chemical equilibrum in the plume parcels.Conversion of NO is then inhibited by the mixing rate of the plume with its surrounding air. To incorporate the mixing rate of the plume correctly into a model, in principle the concentration distribution in a momentary plume has to be used. If a non-linear chemical reaction is modelled it is therefore important to establish the averaging times on which the dispersion parameters in the model are based. The contribution of plume meandering to dispersion, which is especially important in the daytime, can be eliminated by taking shorter averaging times. This leads to a marked improvement of modelling results. Further research is required to investigate how the contribution of fluctuations in the concentrations around the mean has to be incorporated into a model of a chemically reactive plume.