AERMOD performance evaluation for three coal-fired electrical generating units in Southwest Indiana

An evaluation of the steady-state dispersion model AERMOD was conducted to determine its accuracy at predicting hourly ground-level concentrations of sulfur dioxide (SO₂) by comparing model-predicted concentrations to a full year of monitored SO₂ data. The two study sites are comprised of three coal-fired electrical generating units (EGUs) located in southwest Indiana. The sites are characterized by tall, buoyant stacks, flat terrain, multiple SO₂ monitors, and relatively isolated locations. AERMOD v12060 and AERMOD v12345 with BETA options were evaluated at each study site. For the six monitor–receptor pairs evaluated, AERMOD showed generally good agreement with monitor values for the hourly 99th percentile SO₂ design value, with design value ratios that ranged from 0.92 to 1.99. AERMOD was within acceptable performance limits for the Robust Highest Concentration (RHC) statistic (RHC ratios ranged from 0.54 to 1.71) at all six monitors. Analysis of the top 5% of hourly concentrations at the six monitor–receptor sites, paired in time and space, indicated poor model performance in the upper concentration range. The amount of hourly model predicted data that was within a factor of 2 of observations at these higher concentrations ranged from 14 to 43% over the six sites. Analysis of subsets of data showed consistent overprediction during low wind speed and unstable meteorological conditions, and underprediction during stable, low wind conditions. Hourly paired comparisons represent a stringent measure of model performance; however, given the potential for application of hourly model predictions to the SO₂ NAAQS design value, this may be appropriate. At these two sites, AERMOD v12345 BETA options do not improve model performance.

Implications:

A regulatory evaluation of AERMOD utilizing quantile-quantile (Q–Q) plots, the RHC statistic, and 99th percentile design value concentrations indicates that model performance is acceptable according to widely accepted regulatory performance limits. However, a scientific evaluation examining hourly paired monitor and model values at concentrations of interest indicates overprediction and underprediction bias that is outside of acceptable model performance measures. Overprediction of 1-hr SO₂ concentrations by AERMOD presents major ramifications for state and local permitting authorities when establishing emission limits.     

Emissions Variability Processor (EMVAP): Design,evaluation, and application

Emissions of pollutants such as SO₂ and NOx from external combustion sources can vary widely depending on fuel sulfur content, load, and transient conditions such as startup, shutdown, and maintenance/malfunction. While monitoring will automatically reflect variability from both emissions and meteorological influences, dispersion modeling has been typically conducted with a single constant peak emission rate. To respond to the need to account for emissions variability in addressing probabilistic 1-hr ambient air quality standards for SO₂ and NO₂, we have developed a statistical technique, the Emissions Variability Processor (EMVAP), which can account for emissions variability in dispersion modeling through Monte Carlo sampling from a specified frequency distribution of emission rates. Based upon initial AERMOD modeling of from 1 to 5 years of actual meteorological conditions, EMVAP is used as a postprocessor to AERMOD to simulate hundreds or even thousands of years of concentration predictions. This procedure uses emissions varied hourly with a Monte Carlo sampling process that is based upon the user-specified emissions distribution, from which a probabilistic estimate can be obtained of the controlling concentration. EMVAP can also accommodate an advanced Tier 2 NO₂ modeling technique that uses a varying ambient ratio method approach to determine the fraction of total oxides of nitrogen that are in the form of nitrogen dioxide. For the case of the 1-hr National Ambient Air Quality Standards (NAAQS, established for SO₂ and NO₂), a “critical value” can be defined as the highest hourly emission rate that would be simulated to satisfy the standard using air dispersion models assuming constant emissions throughout the simulation. The critical value can be used as the starting point for a procedure like EMVAP that evaluates the impact of emissions variability and uses this information to determine an appropriate value to use for a longer term (e.g., 30-day) average emission rate that would still provide protection for the NAAQS under consideration. This paper reports on the design of EMVAP and its evaluation on several field databases that demonstrate that EMVAP produces a suitably modest overestimation of design concentrations. We also provide an example of an EMVAP application that involves a case in which a new emission limitation needs to be considered for a hypothetical emission unit that has infrequent higher-than-normal SO₂ emissions.

ImplicationsEmissions of pollutants from combustion sources can vary widely depending on fuel sulfur content, load, and transient conditions such as startup and shutdown. While monitoring will automatically reflect this variability on measured concentrations, dispersion modeling is typically conducted with a single peak emission rate assumed to occur continuously. To realistically account for emissions variability in addressing probabilistic 1-hr ambient air quality standards for SO₂ and NO₂, the authors have developed a statistical technique, the Emissions Variability Processor (EMVAP), which can account for emissions variability in dispersion modeling through Monte Carlo sampling from a specified frequency distribution of emission rates.     

Near-roadway monitoring of vehicle emissions as a function of mode of operation for light-duty vehicles

Determination of the effect of vehicle emissions on air quality near roadways is important because vehicles are a major source of air pollution. A near-roadway monitoring program was undertaken in Chicago between August 4 and October 30, 2014, to measure ultrafine particles, carbon dioxide, carbon monoxide, traffic volume and speed, and wind direction and speed. The objective of this study was to develop a method to relate short-term changes in traffic mode of operation to air quality near roadways using data averaged over 5-min intervals to provide a better understanding of the processes controlling air pollution concentrations near roadways. Three different types of data analysis are provided to demonstrate the type of results that can be obtained from a near-roadway sampling program based on 5-min measurements: (1) development of vehicle emission factors (EFs) for ultrafine particles as a function of vehicle mode of operation, (2) comparison of measured and modeled CO₂ concentrations, and (3) application of dispersion models to determine concentrations near roadways. EFs for ultrafine particles are developed that are a function of traffic volume and mode of operation (free flow and congestion) for light-duty vehicles (LDVs) under real-world conditions. Two air quality models—CALINE4 (California Line Source Dispersion Model, version 4) and AERMOD (American Meteorological Society/U.S. Environmental Protection Agency Regulatory Model)—are used to predict the ultrafine particulate concentrations near roadways for comparison with measured concentrations. When using CALINE4 to predict air quality levels in the mixing cell, changes in surface roughness and stability class have no effect on the predicted concentrations. However, when using AERMOD to predict air quality in the mixing cell, changes in surface roughness have a significant impact on the predicted concentrations.

Implications: The paper provides emission factors (EFs) that are a function of traffic volume and mode of operation (free flow and congestion) for LDVs under real-world conditions. The good agreement between monitoring and modeling results indicates that high-resolution, simultaneous measurements of air quality and meteorological and traffic conditions can be used to determine real-world, fleet-wide vehicle EFs as a function of vehicle mode of operation under actual driving conditions.     

Evaluation of an explicit NOx chemistry method in AERMOD

An explicit NO_x chemistry method has been implemented in AERMOD version 15181, ADMSM. The scheme has been evaluated by comparison with the methodologies currently recommended by the U.S. EPA for Tier 3 NO₂ calculations, that is, OLM and PVMRM2. Four data sets have been used for NO₂ chemistry method evaluation. Overall, ADMSM-modeled NO₂ concentrations show the most consistency with the AERMOD calculations of NO_x and the highest Index of Agreement; they are also on average lower than those of both OLM and PVMRM2. OLM shows little consistency with modeled NO_x concentrations and markedly overpredicts NO₂. PVMRM2 shows performance closer to that of ADMSM than OLM; however, its behavior is inconsistent with modeled NO_x in some cases and it has less good statistics for NO₂. The trend in model performance can be explained by examining the features particular to each chemistry method: OLM can be considered as a screening model as it calculates the upper bound of conversion from NO to NO₂ possible with the background O₃ concentration; PVMRM2 includes a much-improved estimate of in-plume O₃ but is otherwise similar to OLM, assuming instantaneous reaction of NO with O₃; and ADMSM allows for the rate of this reaction and also the photolysis of NO₂. Evaluation with additional data sets is needed to further clarify the relative performance of ADMSM and PVMRM2.

Implications: Extensive evaluation of the current AERMOD Tier 3 chemistry methods OLM and PVMRM2, alongside a new scheme that explicitly calculates the oxidation of NO by O₃ and the reverse photolytic reaction, shows that OLM consistently overpredicts NO₂ concentrations. PVMRM2 performs well in general, but there are some cases where this method overpredicts NO₂. The new explicit NO_x chemistry scheme, ADMSM, predicts NO₂ concentrations that are more consistent with both the modeled NO_x concentrations and the observations.     

Evaluation of low wind modeling approaches for two tall-stack databases

The performance of the AERMOD air dispersion model under low wind speed conditions, especially for applications with only one level of meteorological data and no direct turbulence measurements or vertical temperature gradient observations, is the focus of this study. The analysis documented in this paper addresses evaluations for low wind conditions involving tall stack releases for which multiple years of concurrent emissions, meteorological data, and monitoring data are available. AERMOD was tested on two field-study databases involving several SO₂ monitors and hourly emissions data that had sub-hourly meteorological data (e.g., 10-min averages) available using several technical options: default mode, with various low wind speed beta options, and using the available sub-hourly meteorological data. These field study databases included (1) Mercer County, a North Dakota database featuring five SO₂ monitors within 10 km of the Dakota Gasification Company’s plant and the Antelope Valley Station power plant in an area of both flat and elevated terrain, and (2) a flat-terrain setting database with four SO₂ monitors within 6 km of the Gibson Generating Station in southwest Indiana. Both sites featured regionally representative 10-m meteorological databases, with no significant terrain obstacles between the meteorological site and the emission sources. The low wind beta options show improvement in model performance helping to reduce some of the overprediction biases currently present in AERMOD when run with regulatory default options. The overall findings with the low wind speed testing on these tall stack field-study databases indicate that AERMOD low wind speed options have a minor effect for flat terrain locations, but can have a significant effect for elevated terrain locations. The performance of AERMOD using low wind speed options leads to improved consistency of meteorological conditions associated with the highest observed and predicted concentration events. The available sub-hourly modeling results using the Sub-Hourly AERMOD Run Procedure (SHARP) are relatively unbiased and show that this alternative approach should be seriously considered to address situations dominated by low-wind meander conditions.

Implications: AERMOD was evaluated with two tall stack databases (in North Dakota and Indiana) in areas of both flat and elevated terrain. AERMOD cases included the regulatory default mode, low wind speed beta options, and use of the Sub-Hourly AERMOD Run Procedure (SHARP). The low wind beta options show improvement in model performance (especially in higher terrain areas), helping to reduce some of the overprediction biases currently present in regulatory default AERMOD. The SHARP results are relatively unbiased and show that this approach should be seriously considered to address situations dominated by low-wind meander conditions.     

Evaluation of the SO2 and NOX offset ratio method to account for secondary PM2.5 formation

The U.S. Environmental Protection Agency (EPA), state and local agencies have focused their efforts in assessing secondary fine particulate matter (aerodynamic diameter ≤2.5 µm; PM_2.5) formation in prevention of significant deterioration (PSD) air dispersion modeling. The National Association of Clean Air Agencies (NACAA) developed a method to account for secondary PM_2.5 formation by using sulfur dioxide (SO₂) and nitrogen oxides (NO_x) offset ratios. These ratios are used to estimate the secondary formation of sulfate and nitrate PM_2.5. These ratios were first introduced by the EPA for nonattainment areas in the Implementation of the New Source Review (NSR) Program for Particulate Matter Less than 2.5 Micrometers (PM_2.5), 73 FR 28321, to offset emission increases of direct PM_2.5 emissions with reductions of PM_2.5 precursors and vice versa. Some regulatory agencies such as the Minnesota Pollution Control Agency (MPCA) have developed area-specific offset ratios for SO₂ and NO_x based on Comprehensive Air Quality Model with Extensions (CAMx) evaluations for air dispersion modeling analyses. The current study evaluates the effect on American Meteorological Society/Environmental Protection Agency Regulatory Model (AERMOD) predicted concentrations from the use of EPA and MPCA developed ratios. The study assesses the effect of these ratios on an electric generating utility (EGU), taconite mine, food processing plant, and a pulp and paper mill. The inputs used for these four scenarios are based on common stack parameters and emissions based on available data. The effect of background concentrations also evaluates these scenarios by presenting results based on uniform annual PM_2.5 background values. This evaluation study helps assess the viability of the offset ratio method developed by NACAA in estimating primary and secondary PM_2.5 concentrations. An alternative Tier 2 approach to combine modeled and monitored concentrations is also presented.

Implications:

On January 4, 2012, the EPA committed to engage in rulemaking to evaluate updates to the Guideline on Air Quality Models (Appendix W of 40 CFR 51) and, as appropriate, incorporate new analytical techniques or models for secondary PM_2.5. As a result, the National Association of Clean Air Agencies (NACAA) developed a screening method involving offset ratios to account for secondary PM_2.5 formation. The use of this method is promising to evaluate total (direct and indirect) PM_2.5 impacts for permitting purposes. Therefore, the evaluation of this method is important to determine its viability for widespread use.     

The role of a steel plant in north-west Italy to the local air concentrations of PCDD/Fs

Polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) are ubiquitous contaminants, mainly released into the environment during combustion processes (point sources), but also from other sources (traffic, uncontrolled combustion).This study aims at investigating the contribution of a steel plant in NW Italy (700 000 tons of steel year⁻¹) to the air concentrations of PCDDs/PCDFs at local level, through the analysis of measured, modelled and literature data. The study was carried out in an area of 600 km², using air quality data measured by the institutional monitoring network, data obtained from AERMOD simulations and literature data.The measured air concentrations were consistent with literature values for similar areas, and both the homologue profiles and PCA analyses showed a clear distinction between the monitoring stations and the source profiles.All the previous results were confirmed by the air dispersion model (AERMOD), that predicted PCDD/F air concentrations due to the steel plant from four to two orders of magnitude lower than those measured in the monitoring stations, highlighting the presence of other sources.This study outlines the limited influence of the source in the local PCDD/F air concentrations and at the same time the usefulness of a joint analysis of measured, literature and calculated data to correctly evaluate the role of a source to the local pollution. The study also highlights the usefulness of AERMOD as a complementary tool to define the correct placement of monitoring stations and to locate those areas expected to have the highest air concentrations deriving from a source.     

Source Identification of Atlanta Aerosol by Positive Matrix Factorization

Abstract

Data characterizing daily integrated particulate matter (PM) samples collected at the Jefferson Street monitoring site in Atlanta, GA, were analyzed through the application of a bilinear positive matrix factorization (PMF) model. A total of 662 samples and 26 variables were used for fine particle (particles ≤2.5 µm in aerodynamic diameter) samples (PM_2.5 ), and 685 samples and 15 variables were used for coarse particle (particles between 2.5 and 10 µm in aerodynamic diameter) samples (PM_10–2.5 ). Measured PM mass concentrations and compositional data were used as independent variables. To obtain the quantitative contributions for each source, the factors were normalized using PMF-apportioned mass concentrations. For fine particle data, eight sources were identified: SO₄ ^2?-rich secondary aerosol (56%), motor vehicle (22%), wood smoke (11%), NO₃ ^?-rich secondary aerosol (7%), mixed source of cement kiln and organic carbon (OC) (2%), airborne soil (1%), metal recycling facility (0.5%), and mixed source of bus station and metal processing (0.3%). The SO₄ ^2?-rich and NO₃ ^?-rich secondary aerosols were associated with NH₄ ⁺. The SO₄ ^2?-rich secondary aerosols also included OC. For the coarse particle data, five sources contributed to the observed mass: airborne soil (60%), NO₃ ^?-rich secondary aerosol (16%), SO₄ ^2?-rich secondary aerosol (12%), cement kiln (11%), and metal recycling facility (1%). Conditional probability functions were computed using surface wind data and identified mass contributions from each source. The results of this analysis agreed well with the locations of known local point sources.     

Long-term trends in airborne SO2 in an air quality monitoring station in Seoul,Korea, from 1987 to 2013

Atmospheric concentration of sulfur dioxide (SO₂) was intermittently measured at an air quality monitoring (AQM) station in the Yong-san district of Seoul, Korea, between 1987 and 2013. The SO₂ level was compared with other important pollutants concurrently measured, including methane (CH₄), carbon monoxide (CO), nitric oxide (NO), nitrogen dioxide (NO₂), ozone (O₃), and particulate matter (PM₁₀). If split into three different periods (period 1, 1987–1988, period 2, 1999–2000, and period 3, 2004–2013), the respective mean [SO₂] values (6.57 ± 4.29, 6.30 ± 2.44, and 5.29 ± 0.63 ppb) showed a slight reduction across the entire study period. The concentrations of SO₂ are found to be strongly correlated with other pollutants such as CO (r = 0.614, p = 0.02), which tracked reductions in reported emissions due to tighter emissions standards enacted by the South Korean government. There was also a clear seasonal trend in the SO₂ level, especially in periods 2 and 3, reflecting the combined effects of domestic heating by coal briquettes and meteorological conditions. Although only a 16% concentration reduction was achieved during the 27-year study duration, this is significant if one considers rapid urbanization, an 83.2% increase in population, and rapid industrialization that took place during that period.

Implications: Since 1970, a network of air quality monitoring (AQM) stations has been operated by the Korean Ministry of Environment (KMOE) for routine nationwide monitoring of air pollutant concentrations in urban/suburban areas. To date, the information obtained from these stations has provided a platform for analyzing long-term trends of major pollutant species. In this study, we examined the long-term trends of SO₂ levels and relevant environmental parameters monitored continuously in the Yong-san district of Seoul between 1987 and 2013. The data were analyzed over various time scales (i.e., monthly, seasonal, and annual intervals). The results obtained from this study will allow us to assess the effectiveness of abatement strategy and to predict future concentrations trends in association with future abatement strategies and technologies.     

Use of AERMOD to Determine a Hydrogen Sulfide Emission Factor for Swine Operations by Inverse Modeling

This study was conducted to determine both optimal settings applied to the plume dispersion model, AERMOD, and a scalable emission factor for accurately determining the spatial distribution of hydrogen sulfide concentrations in the vicinity of swine concentrated animal feeding operations (CAFOs). These operations emit hydrogen sulfide from both housing structures and waste lagoons. With ambient measurements made at 4 stations within 1 km of large swine CAFOs in Iowa, an inverse-modeling approach applied to AERMOD was used to determine hydrogen sulfide emission rates. CAFO buildings were treated as volume sources whereas nearby lagoons were modeled as area sources. The robust highest concentration (RHC), calculated for both measured and modeled concentrations, was used as the metric for adjusting the emission rate until the ratio of the two RHC levels was unity. Utilizing this approach, an average emission flux rate of 0.57 μg/m(2)-s was determined for swine CAFO lagoons. Using the average total animal weight (kg) of each CAFO, an average emission factor of 6.06 × 10(-7) μg/yr-m(2)-kg was calculated. From studies that measured either building or lagoon emission flux rates, building fluxes, on a floor area basis, were considered equal to lagoon flux rates. The emission factor was applied to all CAFOs surrounding the original 4 sites and surrounding an additional 6 sites in Iowa, producing an average modeled-to-measured RHC ratio of 1.24. When the emission factor was applied to AERMOD to simulate the spatial distribution of hydrogen sulfide around a hypothetical large swine CAFO (1M kg), concentrations 0.5 km from the CAFO were 35 ppb and dropped to 2 ppb within 6 km of the CAFO. These values compare to a level of 30 ppb that has been determined by the State of Iowa as a threshold level for ambient hydrogen sulfide levels.     

Influence of sulfur dioxide-related interactions on PM2.5 formation in iron ore sintering

The formation of PM_2.5 (aerosol particulate matter less than 2.5 µm in aerodynamic diameter) in association with SO₂ emission during sintering process has been studied by dividing the whole sintering process into six typical sampling stages. A low-pressure cascade impactor was used to collect PM_2.5 by automatically segregating particulates into six sizes. It was found that strong correlation existed between the emission properties of PM_2.5 and SO₂. Wet mixture layer (overwetted layer and raw mixture layer) had the function to simultaneously capture SO₂ and PM_2.5 during the early sintering stages, and released them back into flue gas mainly in the flue gas temperature-rising period. CaSO₄ crystals constituted the main SO₂-related PM_2.5 during the disappearing process of overwetted layer, which was able to form perfect individual crystals or to form particles with complex chemical compositions. Besides the existence of individual CaSO₄ crystals, mixed crystals of K₂SO₄-CaSO₄ in PM_2.5 were also found during the first half of the temperature-rising period of flue gas. The interaction between fine-grained Ca-based fluxes, potassium vapors, and SO₂ was the potential source of SO₂-related PM_2.5.

Implications: The emission property of PM_2.5 and SO₂ throughout the sintering process exhibited well similarity. This phenomenon tightened the relationship between the formation of PM_2.5 and the emission of SO₂. Through revealing the properties of SO₂-related PM_2.5 during sintering process, the potential interaction between fine-grained Ca-based fluxes, potassium vapors, and SO₂ was found to be the source of SO₂-related PM_2.5. This information can serve as the guidance to develop efficient techniques to control the formation and emission of PM_2.5 in practical sintering plants.     

Minimum turbulence assumptions and u* and L estimation for dispersion models during low-wind stable conditions

The U.S. Environmental Protection Agency (EPA) short-distance dispersion model, AERMOD, has been shown to overpredict by a factor of as much as 10 when compared with observed concentrations from continuous releases at the Oak Ridge, TN (OR), and Idaho Falls, ID (IF), field experiments during stable periods when wind speeds often dropped below 1 m/sec. Some of this overprediction tendency can be reduced by revising AERMOD's meteorological preprocessor's parameterizations of the friction velocity, u _* , during low-wind stable conditions, thus increasing the calculated σ _v and σ _w and hence the lateral and vertical dispersion rates. Observations show that as the mean wind speed approaches zero at night, there is always significant σ _v and σ _w over time periods of 15 to 60 min, while standard Monin–Obukhov Similarity Theory (MOST) predicts that σ _v and σ _w will approach zero. This paper focuses on the u _* estimation methods and the minimum turbulence (σ _v and σ _w ) assumptions in AERMOD (beta option 4) and two widely used U.S. operational dispersion models, AERMOD (v12345) and SCICHEM. The U.S. EPA has provided results of its tests with the OR and IF data, with its base AERMOD version and its December 2012 modified versions, which assume adjustments to the low-wind u _* and increases in the minimum σ _v parameterization. SCICHEM has relatively small mean bias for both data sets. The revised AERMOD shows much less mean bias, agreeing more with SCICHEM.

Implications:

Suggestions are made for improvements to dispersion models such as AERMOD to correct overpredictions during light-wind stable conditions. Methods for estimating u_*, L, and the minimum turbulence parameters (σ_v and σ_w) are reviewed and compared. SCICHEM and the current operational version and an optional beta version (December 2012) of AERMOD are evaluated with tracer data from low-wind stable field experiments in Idaho Falls and Oak Ridge. It is seen that the operational version of AERMOD overpredicts by a factor of 2 to 10, while the optional beta version of AERMOD and SCICHEM have much less bias.     

NO2 and SO2dispersion modeling and relative roles of emission sources over Map Ta Phut industrial area,Thailand

Map Ta Phut industrial area (MA) is the largest industrial complex in Thailand. There has been concern about many air pollutants over this area. Air quality management for the area is known to be difficult, due to lack of understanding of how emissions from different sources or sectors (e.g., industrial, power plant, transportation, and residential) contribute to air quality degradation in the area. In this study, a dispersion study of NO₂ and SO₂ was conducted using the AERMOD model. The area-specific emission inventories of NO_x and SO₂ were prepared, including both stack and nonstack sources, and divided into 11 emission groups. Annual simulations were performed for the year 2006. Modeled concentrations were evaluated with observations. Underestimation of both pollutants was found, and stack emission estimates were scaled to improve the modeled results before quantifying relative roles of individual emission groups to ambient concentration over four selected impacted areas (two are residential and the others are highly industrialized). Two concentration measures (i.e., annual average area-wide concentration or AC, and area-wide robust highest concentration or AR) were used to aggregately represent mean and high-end concentrations for each individual area, respectively. For AC-NO₂, on-road mobile emissions were found to be the largest contributor in the two residential areas (36–38% of total AC-NO₂), while petrochemical-industry emissions play the most important role in the two industrialized areas (34–51%). For AR-NO₂, biomass burning has the most influence in all impacted areas (>90%) except for one residential area where on-road mobile is the largest (75%). For AC-SO₂, the petrochemical industry contributes most in all impacted areas (38–56%). For AR-SO₂, the results vary. Since the petrochemical industry was often identified as the major contributor despite not being the largest emitter, air quality workers should pay special attention to this emission group when managing air quality for the MA.

Implications: Effective air quality management in Map Ta Phut Industrial Area, Thailand requires better understanding of how emissions from various sources contribute to the degradation of ambient air quality. Based on the dispersion study here, petrochemical industry was generally identified as the major contributor to ambient NO₂ and SO₂. By accounting for all stack and non-stack sources, on-road mobile emissions were found to be important in some particular areas.     

A comparison of hourly with annual air pollutant emissions: Implications for estimating acute exposure and public health risk

Health risks from air pollutants are evaluated by comparing chronic (i.e., an average over 1 yr or greater) or acute (typically 1-hr) exposure estimates with chemical- and duration-specific reference values or standards. When estimating long-term pollutant concentrations via exposure modeling, facility-level annual average emission rates are readily available as model inputs for most air pollutants. In contrast, there are far fewer facility-level hour-by-hour emission rates available for many of these same pollutants. In this report, we first analyze hour-by-hour emission rates for total reduced sulfur (TRS) compounds from eight kraft pulp mill operations. This data set is used to demonstrate discrepancies between estimating exposure based on a single TRS emission rate that has been calculated as the mean of all operating hours of the year, as opposed to reported hourly emission rates. A similar analysis is then performed using reported hourly emission rates for sulfur dioxide (SO₂) and oxides of nitrogen (NO_x) from three power generating units from a U.S. power plant. Results demonstrate greater variability at kraft pulp mill operations, with ratios of reported hourly to average hourly TRS emissions ranging from less than 1 to greater than 160 during routine facility operations. Thus, if fluctuations in hourly emission rates are not accounted for, over- or underestimates of hourly exposure, and thus acute health risk, may occur. In addition to this analysis, we also demonstrate an additional challenge when assessing health risk based on hourly exposures: the lack of human health reference values based on 1-hr exposures.

Implications: Largely due to the lack of reported hourly emission rate data for many air pollutants, an hourly average emission rate (calculated from an annual emission rate) is often used when modeling the potential for acute health risk. We calculated ratios between reported hourly and hourly average emission rates from pulp and paper mills and a U.S. power plant to demonstrate that if not considered, hourly fluctuations in emissions could result in an over- or underestimation of exposure and risk. We also demonstrate the lack of 1-hr human health reference values meant to be protective of the general population, including children.     

Photochemical oxidation and dispersion of gaseous sulfur compounds from natural and anthropogenic sources around a coastal location

The photochemical oxidation and dispersion of reduced sulfur compounds (RSCs: H₂S, CH₃SH, DMS, CS₂, and DMDS) emitted from anthropogenic (A) and natural (N) sources were evaluated based on a numerical modeling approach. The anthropogenic emission concentrations of RSCs were measured from several sampling sites at the Donghae landfill (D-LF) (i.e., source type A) in South Korea during a series of field campaigns (May through December 2004). The emissions of natural RSCs in a coastal study area near the D-LF (i.e., source type N) were estimated from sea surface DMS concentrations and transfer velocity during the same study period. These emission data were then used as input to the CALPUFF dispersion model, revised with 34 chemical reactions for RSCs. A significant fraction of sulfur dioxide (SO₂) was produced photochemically during the summer (about 34% of total SO₂ concentrations) followed by fall (21%), spring (15%), and winter (5%). Photochemical production of SO₂ was dominated by H₂S (about 55% of total contributions) and DMS (24%). The largest impact of RSCs from source type A on SO₂ concentrations occurred around the D-LF during summer. The total SO₂ concentrations produced from source type N around the D-LF during the summer (a mean SO₂ concentration of 7.4 ppbv) were significantly higher than those (≤0.3 ppbv) during the other seasons. This may be because of the high RSC and SO₂ emissions and their photochemistry along with the wind convergence.     

Assimilative capacity–based emission load management in a critically polluted industrial cluster

In the present study, a modified approach was adopted to quantify the assimilative capacity (i.e., the maximum emission an area can take without violating the permissible pollutant standards) of a major industrial cluster (Manali, India) and to assess the effectiveness of adopted air pollution control measures at the region. Seasonal analysis of assimilative capacity was carried out corresponding to critical, high, medium, and low pollution levels to know the best and worst conditions for industrial operations. Bottom-up approach was employed to quantify sulfur dioxide (SO₂), nitrogen dioxide (NO₂), and particulate matter (aerodynamic diameter <10 μm; PM₁₀) emissions at a fine spatial resolution of 500 × 500 m² in Manali industrial cluster. AERMOD (American Meteorological Society/U.S. Environmental Protection Agency Regulatory Model), an U.S. Environmental Protection Agency (EPA) regulatory model, was used for estimating assimilative capacity. Results indicated that 22.8 tonnes/day of SO₂, 7.8 tonnes/day of NO₂, and 7.1 tonnes/day of PM₁₀ were emitted from the industries of Manali. The estimated assimilative capacities for SO₂, NO₂, and PM₁₀ were found to be 16.05, 17.36, and 19.78 tonnes/day, respectively. It was observed that the current SO₂ emissions were exceeding the estimated safe load by 6.7 tonnes/day, whereas PM₁₀ and NO₂ were within the safe limits. Seasonal analysis of assimilative capacity showed that post-monsoon had the lowest load-carrying capacity, followed by winter, summer, and monsoon seasons, and the allowable SO₂ emissions during post-monsoon and winter seasons were found to be 35% and 26% lower, respectively, when compared with monsoon season.

Implications: The authors present a modified approach for quantitative estimation of assimilative capacity of a critically polluted Indian industrial cluster. The authors developed a geo-coded fine-resolution PM₁₀, NO₂, and SO₂ emission inventory for Manali industrial area and further quantitatively estimated its season-wise assimilative capacities corresponding to various pollution levels. This quantitative representation of assimilative capacity (in terms of emissions), when compared with routine qualitative representation, provides better data for quantifying carrying capacity of an area. This information helps policy makers and regulatory authorities to develop an effective mitigation plan for air pollution abatement.     

Alternate approaches for assessing impacts of oil sands development on air quality: A case study using the First Nation Community of Fort McKay

Previous analyses of continuously measured compounds in Fort McKay, an indigenous community in the Athabasca Oil Sands, have detected increasing concentrations of nitrogen dioxide (NO₂) and total hydrocarbons (THC), but not of sulfur dioxide (SO₂), ozone (O₃), total reduced sulfur compounds (TRS), or particulate matter (aerodynamic diameter <2.5 μm; PM_2.5). Yet the community frequently experiences odors, dust, and reduced air quality. The authors used Fort McKay’s continuously monitored air quality data (1998–2014) as a case study to assess techniques for air quality analysis that make no assumptions regarding type of change. Linear trend analysis detected increasing concentrations of higher percentiles of NO₂, nitric oxide (NO), and nitrogen oxides (NO_x), and THC. However, comparisons of all compounds between an early industrial expansion period (1998–2001) and current day (2011–2014) show that concentrations of NO₂, SO₂, THC, TRS, and PM_2.5 have significantly increased, whereas concentrations of O₃ are significantly lower. An assessment of the frequency and duration of periods when concentrations of each compound were above a variety of thresholds indicated that the frequency of air quality events is increasing for NO₂ and THC. Assessment of change over time with odds ratios of the 25th, 50th, 75th, and 90th percentile concentrations for each compound compared with an estimate of natural background variability showed that concentrations of TRS, SO₂, and THC are dynamic, higher than background, and changes are nonlinear and nonmonotonic. An assessment of concentrations as a function of wind direction showed a clear and generally increasing influence of industry on air quality. This work shows that evaluating air quality without assumptions of linearity reveals dynamic changes in air quality in Fort McKay, and that it is increasingly being affected by oil sands operations.

Implications: Understanding the nature and types of air quality changes occurring in a community or region is essential for the development of appropriate air quality management policies. Time-series trending of air quality data is a common tool for assessing air quality changes and is often used to assess the effectiveness of current emission management programs. The use of this tool, in the context of oil sands development, has significant limitations, and alternate air quality change analysis approaches need to be applied to ensure that the impact of this development on air quality is fully understood so that appropriate emission management actions can be taken.     

Which meteorological conditions produce worst-case odors from area sources?

Two competing meteorological factors influence atmospheric concentrations of pollutants from open liquid area sources such as wastewater treatment plant units: temperature and stability. High temperatures in summer produce greater emissions from liquid area sources because of increased compound volatility; however, these emissions tend to disperse more readily because of frequent occurrence of unstable conditions. An opposite scenario occurs in winter, with lesser emissions due to lower temperatures, but also frequently less dispersion, due to stable atmospheric conditions. The primary objective of this modeling study was thus to determine whether higher atmospheric concentrations from open liquid area sources occur more frequently in summer, when emissions are greater but so is dispersion, or in winter, when emissions are lesser but so is dispersion. The study utilized a rectangular clarifier emitting hydrogen sulfide as a sample open liquid area source. Dispersion modeling runs were conducted using ISCST3 and AERMOD, encompassing 5 yr of hourly meteorological data divided by season. Emission rates were varied hourly on the basis of a curve-fit developed from previously collected field data. Model output for each season was used to determine (1) maximum 2-min average concentrations, (2) the number of odor events (2-min average concentrations greater than odor detection thresholds), and (3) areas of impact. On the basis of these 3 types of output, it was found that the worst-case odors were associated with summer, considering impacts of meteorology upon both emissions and dispersion. Not accounting for the impact of meteorology on emissions (using a constant worst-case emission rate) caused concentrations to be overpredicted compared with a variable emission rate case. The highest concentrations occurred during stability classes D, E, and F, as anticipated. A comparison of ISCST3 and AERMOD found that for the area source modeled, ISCST3 predicted higher concentrations and more odor events for all seasons.