Innovative Approach for Estimating Fugitive Gaseous Fluxes Using Computed Tomography and Remote Optical Sensing Techniques

ABSTRACT

This paper presents a new approach to quantify emissions from fugitive gaseous air pollution sources. The authors combine Computed Tomography (CT) with Path-Integrated Optical Remote Sensing (PI-ORS) concentration data in a new field beam geometry. Path-integrated concentrations are sampled in a vertical plane downwind from the source along several radial beam paths. An innovative CT technique, which applies the Smooth Basis Function Minimization method to the beam data in conjunction with measured wind data, is used to estimate the total flux from the fugitive source. The authors conducted a synthetic data study to evaluate the proposed methodology under different meteorological conditions, beam geometry configurations, and simulated measurement errors. The measurement errors were simulated based on data collected with an Open-Path Fourier Transform Infra-Red system. This approach was found to be robust for the simulated errors and for a wide range of fluctuating wind directions. In the very sparse beam geometry examined (eight beam paths), successful emission rates were retrieved over a 70° range of wind directions under extremely large measurement error conditions.     

Localizing Gaseous Fugitive Emission Sources by Combining Real-Time Optical Remote Sensing and Wind Data

ABSTRACT

This paper presents a new approach to localize point emissions from ground-level fugitive gaseous air pollution sources. We estimate the crosswind plume's ground-level peak location downwind from the source by combining smooth basis functions minimization (SBFM) with path-integrated optical remote sensing concentration data acquired along the crosswind direction in alternating beam path lengths. Peak location estimates, in conjunction with real-time measured wind direction data, are used to reconstruct the fugitive source location. We conducted a synthetic data study to evaluate the proposed peak location SBFM reconstruction. Furthermore, the methodology was validated with open-path Fourier transform infrared concentration data collected with wind direction data downwind from a controlled point source. This approach was found to provide reasonable estimates of point source location. The field study reconstructed source location was within several meters of the real source location.     

Localizing gaseous fugitive emission sources by combining real-time optical remote sensing and wind data

This paper presents a new approach to localize point emissions from ground-level fugitive gaseous air pollution sources. We estimate the crosswind plume's ground-level peak location downwind from the source by combining smooth basis functions minimization (SBFM) with pathintegrated optical remote sensing concentration data acquired along the crosswind direction in alternating beam path lengths. Peak location estimates, in conjunction with real-time measured wind direction data, are used to reconstruct the fugitive source location. We conducted a synthetic data study to evaluate the proposed peak location SBFM reconstruction. Furthermore, the methodology was validated with open-path Fourier transform infrared concentration data collected with wind direction data downwind from a controlled point source. This approach was found to provide reasonable estimates of point source location. The field study reconstructed source location was within several meters of the real source location.     

Evaluation of Virtual Source Beam Configurations for Rapid Tomographic Reconstruction of Gas and Vapor Concentrations in Workplaces

Abstract

Beam path average data from an Open Path Fourier Transform Infrared (OP-FTIR) spectrometer can be used to reconstruct two-dimensional concentration maps of the gas and vapor contaminants in workplaces and the environment using computed tomographic (CT) techniques. However, a practical limitation arises because in the past, multiple-source and detector units were required to produce a sufficient number of intersecting beam paths in order to reconstruct concentration maps. Such a system can be applied to actual field monitoring situations only with great expense and difficulty. A single monostatic OP-FTIR system capable of rapid beam movement can eliminate this deficiency. Instead of many source and detector units, a virtual source arrangement has been proposed using a number of flat mirrors and retroreflectors to obtain intersecting folded beam paths.

Three virtual source beam configurations generated for a single-beam steerable FTIR system were tested using 54 flat mirrors and four retroreflectors or 54 flat mirrors and 56 retroreflectors mounted along the perimeter walls of a typical 24- x 21-ft test room. The virtual source CT configurations were numerically evaluated using concentration maps created from tracer gas concentration distributions measured experimentally in a test chamber. Synthetic beam path integral data were calculated from the test maps and beam configurations. Computer simulations of different beam configurations were used to determine the effects of beam geometry. The effects of noise and peak-reducing artifacts were evaluated. The performance of the tomographic reconstruction strategy was tested as a function of concentration and concentration gradients.     

A computational study of particulate emissions from an open pit quarry under neutral atmospheric conditions

The extraction of minerals from surface mines and quarries can produce significant fugitive dust emissions as a result of site activities such as blasting, road haulage, loading, crushing and stockpiling. If uncontrolled, these emissions can present serious environmental, health, safety and operational issues impacting both site personnel and the wider community.The dispersion of pollutant emissions within the atmosphere is principally determined by the background wind systems characterized by the atmospheric boundary layer (ABL). This paper presents an overview of the construction and solution of a computational fluid dynamics (CFD) model to replicate the development of the internal ventilation regime within a surface quarry excavation due to the presence of a neutral ABL above this excavation. This model was then used to study the dispersion and deposition of fugitive mineral dust particles generated during rock blasting operations. The paths of the mineral particles were modelled using Lagrangian particle tracking. Particles of four size fractions were released from five blast locations for eight different wind directions.The study concluded that dependent on the location of the bench blast within the quarry and the direction of the wind, a mass fraction of between 0.3 and 0.6 of the emitted mineral particles was retained within the quarry. The retention was largest when the distance from the blast location to the downwind pit boundary was greatest.     

Comparison of a two-dimensional numerical dust transport model with experimental dust emissions from soil surfaces in a wind tunnel

Near-surface wind-tunnel fugitive dust concentration profiles arising from soil surfaces beds were compared to a finite difference numerical dust transport model. Comparisons of the type shown in this study were previously non-existent in the literature due to the lack of experimental wind-tunnel data for near-surface concentrations over a soil bed. However, in a previous study by the authors, near-surface steady-state concentration profiles were measured in order to obtain fugitive dust emission rates, thus allowing the comparison to models shown in this paper. The novel aspects of the current study include: comparison of concentration profiles of dust obtained experimentally in the wind tunnel with those calculated numerically; comparison of the calculated numerical fetch effect on dust emissions with that obtained in the wind tunnel; and comparison of the emission rates calculated numerically with those obtained experimentally in the wind tunnel. Initial comparisons with the model indicate good agreement implying that the physical mechanism of advection–diffusion is reasonably modeled with the choice of equations for the simple “steady-state” process near the surface. Furthermore, the numerical solutions presented in this paper provide a means to systematically explore the relative impact of varied surface boundary conditions upon the emission process and provide a potential link between wind-tunnel simulations and field scale models.     

The absorption of Hydrogen chloride by aqueous aerosols

A general gas/droplet interaction model has been used to examine the absorption of gaseous hydrogen chloride in aqueous aerosols formed in the presence of typical ambient concentrations of soluble and insoluble particulate over the relative humidity range 60–99 % and temperature range 273–283 K. Absorption of hydrogen chloride in aqueous aerosols formed on inert fugitive ash from a point source has also been simulated using simple puff and constant angle dispersion models. For ambient atmospheres it is predicted that appreciable uptake of hydrogen chloride occurs only for relative humidities approaching 99%. Equilibration times increase with particle size and gas concentration and lie in the range < 1–600 s. For diluting point source emissions, it is predicted that conditions close to equilibrium exist throughout most of the dispersion period. Hydrogen chloride absorption increases with initial plume water content and ambient relative humidity and decreases with ambient temperature. Substantial temporary removal of gaseous hydrogen chloride is predicted under most conditions simulated but the period of uptake is significant only for slowly diluting plumes at ambient relative humidities > 95%. Initial plume particulate diameters > 5 μm are required for enhanced deposition and substantial permanent removal of gaseous HCl. Absorption in aqueous ambient and plume aerosols is thus unlikely to constitute a general highly efficient process for the removal of hydrogen chloride from the atmosphere.     

Experimental evaluation of a radial beam geometry for mapping air pollutants using optical remote sensing and computed tomography

We describe the first experimental evaluation of a non-overlapping radial beam geometry to map air pollutants using computed tomography (CT) and optical remote sensing (ORS) instruments. Nitrous oxide was released from a point source inside a 11 m long×5.4 m wide ventilation chamber. An open path Fourier transform infrared (OP-FTIR) spectrometer gathered path integrated concentration data. The smooth basis function minimization (SBMF) CT algorithm was applied to a radial geometry with 19 rays. Two-dimensional maps were reconstructed from the OP-FTIR measurements and compared with kriged maps calculated from 13-point samples collected simultaneously during the experiments. The CT reconstructions showed good agreement compared to the kriged maps obtained from point samples (concordance correlation factor >0.55). The CT reconstructions also located the peak concentration within 1.2 m compared to the point samplers. In contrast to the complex CT beam geometries proposed in the past, the development of this radial scanning configuration could broaden the application of CT to many optical remote sensing instruments.     

Mapping Odor Sources from Complaint Statistics I: Identifying the Major Source

Odor is acknowledged as a major community air pollution nuisance, but the problems of analysis, particularly in Identifying the origin of odor, are also well recognised. One approach to the problem has been the development of computational schemes which use wind directions at the times of odor observations to locate the likely source of odor. An earlier technique, PONG, has now been superseded by a more sophisticated version, PONG2, which incorporates Gaussian plume modeling techniques. This paper describes the operation of PONG2 in the odor source mapping mode and provides an analysis of the Insensitivity of the technique to errors in input. Then, using specific Australian examples of community odor nuisance emanating from a large sewage treatment complex near Melbourne, and an irrigated golf course within metropolitan Darwin, the paper outlines the utility of PONG2 in resolving problem odor sources at a range of scales and levels of complexity.     

Characterization of near-road pollutant gradients using path-integrated optical remote sensing

Understanding motor vehicle emissions, near-roadway pollutant dispersion, and their potential impact to near-roadway populations is an area of growing environmental interest. As part of ongoing U.S. Environmental Protection Agency research in this area, a field study was conducted near Interstate 440 (I-440) in Raleigh, NC, in July and August of 2006. This paper presents a subset of measurements from the study focusing on nitric oxide (NO) concentrations near the roadway. Measurements of NO in this study were facilitated by the use of a novel path-integrated optical remote sensing technique called deep ultraviolet differential optical absorption spectroscopy (DUV-DOAS). This paper reviews the development and application of this measurement system. Time-resolved near-road NO concentrations are analyzed in conjunction with wind and traffic data to provide a picture of emissions and near-road dispersion for the study. Results show peak NO concentrations in the 150 ppb range during weekday morning rush hours with winds from the road accompanied by significantly lower afternoon and weekend concentrations. Traffic volume and wind direction are shown to be primary determinants of NO concentrations with turbulent diffusion and meandering accounting for significant near-road concentrations in off-wind conditions. The enhanced source capture performance of the open-path configuration allowed for robust comparisons of measured concentrations with a composite variable of traffic intensity coupled with wind transport (R2 = 0.84) as well as investigations on the influence of wind direction on NO dilution near the roadway. The benefits of path-integrated measurements for assessing line source impacts and evaluating models is presented. The advantages of NO as a tracer compound, compared with nitrogen dioxide, for investigations of mobile source emissions and initial dispersion under crosswind conditions are also discussed.     

Measurement of total site mercury emissions from a chlor-alkali plant using ultraviolet differential optical absorption spectroscopy and cell room roof-vent monitoring

This technical note describes a United States Environmental Protection Agency (U.S. EPA) measurement project to determine elemental mercury (Hg⁰) emissions from a mercury cell chlor-alkali (MCCA) facility in the southeastern U.S. during a 53-day monitoring campaign in the fall of 2006. The optical remote sensing (ORS) area source measurement method EPA OTM 10 was used to provide Hg⁰ flux data for the site. These results are reported and compared with cell room roof-vent monitoring data acquired by the facility for similar time periods. The 24-h extrapolated mercury emission rate estimates determined by the two monitoring approaches are shown to be similar with overall averages in the 400 g day^?1 range with maximum values around 1200 g day^?1. Results from the OTM 10 measurements, which include both cell room emissions and potential fugitive sources outside the cell room, are shown to be approximately 10% higher than cell room monitoring results indicating that fugitive emissions from outside the cell room produce a small but measurable effect for this site.     

Minimizing the effect of automotive pollution in urban geometry using mathematical optimization

One of the factors that needs to be considered during the layout of new urban geometry (e.g. street direction, spacing and width, building height restrictions) is the effect of the air pollution associated with the automotive transport that would use routes in this urban area. Although the pollution is generated at street level, its effect can be widespread due to interaction of the pollutant dispersion and diffusion with the wind speed and direction. In order to study the effect of a new urban geometry on the pollutant levels and dispersion, a very time-consuming experimental or parametric numerical study would have to be performed. This paper proposes an alternative approach, that of combining mathematical optimization with the techniques of computational fluid dynamics (CFD). In essence, the meteorological information as represented by a wind rose (wind speed and direction), is used to calculate pollutant levels as a function of urban geometry variables: street canyon depth and street canyon width. The pollutant source specified in conjunction with a traffic scenario with CO is used as pollutant. The main aim of the study is to be able to suggest the most beneficial configuration of an idealized urban geometry that minimizes the peak pollutant levels due to assumed traffic distributions. This study uses two mathematical optimization methods. The first method is implemented through a successive maximization–minimization approach, while the second method determines the location of saddle points of the pollutant level, considered as a function of urban geometry and wind rose. Locally, a saddle point gives the best urban geometry for the worst meteorological scenario. The commercial CFD code, STAR-CD, is coupled with a version of the DYNAMIC-Q optimization algorithm of Snyman, first to successively locate maxima and minima in a min–max approach; and then to locate saddle points. It is shown that the saddle-point method is more cost-effective. The methodology presented in this paper can readily be extended to optimize traffic patterns for existing geometry or in the development of geometry modification for pollution control or toxic releases.     

Simulating sulfur dioxide plume dispersion and subsequent deposition downwind from a stationary point source: a model

Dispersion and subsequent deposition of SO(2) downwind from a stationary point source are affected by several transport processes: buoyancy at the source, advection, and air turbulence en route from the source to the area of impact. In this paper, SO(2) transport processes are simulated by way of Lagrangian air parcel trajectory simulations. In these simulations, the source releases air parcels in puffs. The calculations cover both daytime and night-time conditions and take into account: (i) solar geometry, (ii) diurnal variations of wind speed and air turbulence, (iii) resistance to the transfer of SO(2) from the air to the land, and (iv) flat terrain. Deposition to the forest is determined by calculating the rate of SO(2) flux from individual air parcels to the land according to the parcel's velocity and an assumed air-to-surface SO(2) transfer coefficient. Daily cumulative SO(2) deposition rates are calculated by summing the simulated diffusional fluxes of SO(2) from air to land over each simulated time step. Daily cumulative SO(2) amounts are calculated for downwind distances from 0 to 42 km, for smokestack heights from 30 to 200 m, and for each day of the year according to historical year-round and local weather patterns representative of days with neutral conditions and days with transitions from stable to unstable conditions. Annual per hectare rates of SO(2) deposition are calculated by way of Monte Carlo simulations, according to historical patterns for daily wind, atmospheric stability, and precipitation. These simulations are calibrated for the area surrounding a coal-burning power generator at Grand Lake in south-central New Brunswick, Canada. Calculated concentrations for SO(2) were similar to those obtained with a mobile SO(2) detection unit and a SO(2)-monitoring unit 42 km NE from the emission source. Cumulative SO(2) deposition rates were reasonably similar to those obtained with PbO(2) sulfation plates. A detailed comparison revealed topography was an important factor in modifying actual cumulative SO(2) deposition rates.     

Characterization of Near-Road Pollutant Gradients Using Path-Integrated Optical Remote Sensing

Abstract

Understanding motor vehicle emissions, near-roadway pollutant dispersion, and their potential impact to near-roadway populations is an area of growing environmental interest. As part of ongoing U.S. Environmental Protection Agency research in this area, a field study was conducted near Interstate 440 (I-440) in Raleigh, NC, in July and August of 2006. This paper presents a subset of measurements from the study focusing on nitric oxide (NO) concentrations near the roadway. Measurements of NO in this study were facilitated by the use of a novel path-integrated optical remote sensing technique called deep ultraviolet differential optical absorption spectroscopy (DUV-DOAS). This paper reviews the development and application of this measurement system. Time-resolved near-road NO concentrations are analyzed in conjunction with wind and traffic data to provide a picture of emissions and near-road dispersion for the study. Results show peak NO concentrations in the 150 ppb range during weekday morning rush hours with winds from the road accompanied by significantly lower afternoon and weekend concentrations. Traffic volume and wind direction are shown to be primary determinants of NO concentrations with turbulent diffusion and meandering accounting for significant near-road concentrations in off-wind conditions. The enhanced source capture performance of the open-path configuration allowed for robust comparisons of measured concentrations with a composite variable of traffic intensity coupled with wind transport (R² = 0.84) as well as investigations on the influence of wind direction on NO dilution near the roadway. The benefits of path-integrated measurements for assessing line source impacts and evaluating models is presented. The advantages of NO as a tracer compound, compared with nitrogen dioxide, for investigations of mobile source emissions and initial dispersion under crosswind conditions are also discussed.     

Validation of the lagrangian particle dispersion model FLEXPART against large-scale tracer experiment data

A comprehensive validation of FLEXPART, a recently developed Lagrangian particle dispersion model based on meteorological data from the European Centre for Medium-Range Weather Forecasts, is described in this paper. Measurement data from three large-scale tracer experiments, the Cross-Appalachian Tracer Experiment (CAPTEX), the Across North America Tracer Experiment (ANATEX) and the European Tracer Experiment (ETEX) are used for this purpose. The evaluation is based entirely on comparisons of model results and measurements paired in space and time. It is found that some of the statistical parameters often used for model validation are extremely sensitive to small measurement errors and should not be used in future studies. 40 cases of tracer dispersion are studied, allowing a validation of the model performance under a variety of different meteorological conditions. The model usually performs very well under undisturbed meteorological conditions, but it is less skilful in the presence of fronts. The two ETEX cases reveal the full range of the model’s skill, with the first one being among the best cases studied, and the second one being, by far, the worst. The model performance in terms of the statistical parameters used stays rather constant with time over the periods (up to 117 h) studied here. It is shown that the method used to estimate the concentrations at the receptor locations has a significant effect on the evaluation results. The vertical wind component sometimes has a large influence on the model results, but on the average only a slight improvement over simulations which neglect the vertical wind can be demonstrated. Subgrid variability of mixing heights is important and must be accounted for.     

Estimating fugitive dust emission rates using an environmental boundary layer wind tunnel

Emissions from fugitive dust due to erosion of “natural” wind-blown surfaces are an increasingly important part of PM₁₀ (particulate matter with sizes of 10 μm aerodynamic diameter) emission inventories. These inventories are particularly important to State Implementation Plans (SIP), the plan required for each state to file with the Federal government indicating how they will comply with the Federal Clean Air Act (FCAA). However, techniques for determining the fugitive dust contribution to over all PM₁₀ emissions are still in their developmental stages. In the past, the methods have included field monitoring stations, specialized field studies and field wind-tunnel studies. The measurements made in this paper allow for systematic determination of PM₁₀ emission rates through the use of an environmental boundary layer wind tunnel in the laboratory. Near surface steady-state concentration profiles and velocity profiles are obtained in order to use a control volume approach to estimate emission rates. This methodology is applied to soils retrieved from the nation's single largest PM₁₀ source, Owens (dry) Lake in California, to estimate emission rates during active storm periods. The estimated emission rates are comparable to those obtained from field studies and lend to the validity of this method for determining fugitive dust emission rates.     

Pollutant tomography using integrated concentration data from non-intersecting optical paths

We investigate the possibility of performing tomographic pollutant mapping using path-integral data from non-intersecting optical paths, and conclude that such a geometry does allow reconstruction of the pollutant distribution with the smooth basis function minimization method. The simulated optical data are derived from actual pollutant concentration distributions determined from previous experiments.     

Open-path tunable diode laser absorption spectroscopy for acquisition of fugitive emission flux data

Air pollutant emission from unconfined sources is an increasingly important environmental issue. The U.S. Environmental Protection Agency (EPA) has developed a ground-based optical remote-sensing method that enables direct measurement of fugitive emission flux from large area sources. Open-path Fourier transform infrared spectroscopy (OP-FTIR) has been the primary technique for acquisition of pollutant concentration data used in this emission measurement method. For a number of environmentally important compounds, such as ammonia and methane, open-path tunable diode laser absorption spectroscopy (OP-TDLAS) is shown to be a viable alternative to Fourier transform spectroscopy for pollutant concentration measurements. Near-IR diode laser spectroscopy systems offer significant operational and cost advantages over Fourier transform instruments enabling more efficient implementation of the measurement strategy. This article reviews the EPA's fugitive emission measurement method and describes its multipath tunable diode laser instrument. Validation testing of the system is discussed. OP-TDLAS versus OP-FTIR correlation testing results for ammonia (R2 = 0.980) and methane (R2 = 0.991) are reported. Two example applications of tunable diode laser-based fugitive emission measurements are presented.