Projected changes in particulate matter concentrations in the South Coast Air Basin due to basin-wide reductions in nitrogen oxides,volatile organic compounds,and ammonia emissions

An ozone abatement strategy for the South Coast Air Basin (SoCAB) has been proposed by the South Coast Air Quality Management District (SCAQMD) and the California Air Resources Board (ARB). The proposed emissions reduction strategy is focused on the reduction of nitrogen oxide (NO_x) emissions by the year 2030. Two high PM_2.5 concentration episodes with high ammonium nitrate compositions occurring during September and November 2008 were simulated with the Community Multi-scale Air Quality model (CMAQ). All simulations were made with same meteorological files provided by the SCAQMD to allow them to be more directly compared with their previous modeling studies. Although there was an overall under-prediction bias, the CMAQ simulations were within an overall normalized mean error of 50%; a range that is considered acceptable performance for PM modeling. A range of simulations of these episodes were made to evaluate sensitivity to NO_x and ammonia emissions inputs for the future year 2030. It was found that the current ozone control strategy will reduce daily average PM_2.5 concentrations. However, the targeted NO_x reductions for ozone were not found to be optimal for reducing PM_2.5 concentrations. Ammonia emission reductions reduced PM_2.5 and this might be considered as part of a PM_2.5 control strategy.

Implications: The SCAQMD and the ARB have proposed an ozone abatement strategy for the SoCAB that focuses on NO_x emission reductions. Their strategy will affect both ozone and PM_2.5. Two episodes that occurred during September and November 2008 with high PM_2.5 concentrations and high ammonium nitrate composition were selected for simulation with different levels of nitrogen oxide and ammonia emissions for the future year 2030. It was found that the ozone control strategy will reduce maximum daily average PM_2.5 concentrations but its effect on PM_2.5 concentrations is not optimal.     

Particulate matter emissions associated with marcellus shale drilling waste disposal and transport

ABSTRACT

This study models emissions quantities and neighboring exposure concentrations of six airborne pollutants, including PM₁₀, PM_2.5, crystalline silica, arsenic, uranium, and barium, which resulted from the disposal of Marcellus shale drill cuttings waste during the 2011–2017 period. Using these predicted exposures, this study evaluates current setback distances required in Pennsylvania from waste facilities. For potential residents living at the perimeter of the current setback distance, 274 m (900 ft), a waste disposal rate of 612.4 metric tons per day at landfills (the 99th percentile in record) does not result in exceedances of the exposure limits for any of the six investigated pollutants. However, the current setback distance can result in exceedance with respect to the 24-hr daily concentration standards for PM₁₀ and PM_2.5 established in the National Air Ambient Quality Standards (NAAQS), if daily waste disposal rate surpasses 900 metric tons per day. Dry depositions of barium-containing and uranium-containing particulate matter should not be a danger to public health based on these results. To investigate the air quality impacts of waste transportation and the potential for reductions, this article describes an optimization of landfill locations in Pennsylvania indicating the potential benefits in reduced environmental health hazard level possible by decreasing the distance traveled by waste disposal trucks. This strategy could reduce annual emissions of PM₁₀ and PM_2.5 by a mean of 64% and reduce the expected number of annual fatal accidents by nearly half, and should be considered a potential risk management goal in the long run. Therefore, policy to limit or encourage reduction of distances traveled by waste removal trucks and manage setback distances as a function of delivered waste quantities is merited.     

Analysis of PM10 Trends in the United States from 1988 through 1995

ABSTRACT

Because the U. S. Environmental Protection Agency (EPA) has changed the National Ambient Air Quality Standards (NAAQS) for ambient particulate matter (PM), there is a great deal of interest in determining recent PM trends. This paper examines trends in PM₁₀ (i.e., particulate matter less than 10 micrometers in diameter) for areas of the United States based on their attainment status—for PM₁₀ and ozone nonattainment and attainment areas. The analysis also focuses on urban, suburban, and rural areas, and eastern and western areas. The time period of evaluation is from 1988 through 1995. To shed further light on the ambient PM₁₀ trends, trends in ambient SO₂, NO₂, and volatile organic compounds (VOCs) are also analyzed. Finally, trends in emission inventories of SO₂, NO_x, VOCs, and PM₁₀ are evaluated. Results of the analysis show that widespread and similar reductions in PM₁₀ levels have occurred over the last seven years. Annual reductions range from 3.0% to 3.8%, with the greatest reductions coming in PM₁₀ nonattainment areas, but with very significant reductions also in PM₁₀ attainment areas, ozone attainment areas, and rural areas. The widespread reductions appear to be due to a set of controls or common factors that are having a fairly uniform effect in all of the areas. The consistency of the reductions in different areas suggests that the reductions may also be primarily in the fine particles (i.e., those less than 2.5 micrometers in diameter, or PM_2.5), which are more readily transported than coarse particles.     

Development of a PM2 5 Emissions Inventory for the South Coast Air Basin

ABSTRACT

With the promulgation of a national PM_2.5 ambient air quality standard, it is important that PM_2.5 emissions inventories be developed as a tool for understanding the magnitude of potential PM2.5 violations. Current PM₁₀ inventories include only emissions of primary particulate matter (1 ^ï PM), whereas, based on ambient measurements, both PM₁₀ and PM2.5 emissions inventories will need to include sources of both 1^ï PM and secondary particulate matter (2^ï PM). Furthermore, the U. S. Environmental Protection Agency’s (EPA) current edition of AP-42 includes size distribution data for 1o PM that overestimate the PM_2.5 fraction of fugitive dust sources by at least a factor of 2 based on recent studies.

This paper presents a PM_2.5 emissions inventory developed for the South Coast Air Basin (SCAB) that for the first time includes both 1^ï PM and 2^ï PM. The former is calculated by multiplying PM₁₀ emissions estimates by the PM_2.5/PM₁₀ ratios for different sources. The latter is calculated from estimated emission rates of gas-phase aerosol precursor and gas to aerosol conversion rates consistent with the measured chemical composition of ambient PM_2.5 concentrations observed in the SCAB. The major finding of this PM_2.5 emissions inventory is that the ^2ï aerosol component is more than twice the ^1ï aerosol component, which may result in widely different control strategies being required for fine PM and coarse PM.     

Response of Fine Particulate Matter to Emission Changes of Oxides of Nitrogen and Anthropogenic Volatile Organic Compounds in the Eastern United States

Abstract

A three-dimensional chemical transport model (Particulate Matter Comprehensive Air Quality Model with Extensions [PMCAMx]) is used to investigate changes in fine particle (PM_2.5) concentrations in response to 50% emissions changes of oxides of nitrogen (NO_x) and anthropogenic volatile organic compounds (VOCs) during July 2001 and January 2002 in the eastern United States. The reduction of NO_x emissions by 50% during the summer results in lower average oxidant levels and lowers PM_2.5 (8% on average), mainly because of reductions of sulfate (9–11%), nitrate (45–58%), and ammonium (7–11%). The organic particulate matter (PM) slightly decreases in rural areas, whereas it increases in cities by a few percent when NO_x is reduced. Reduction of NO_x during winter causes an increase of the oxidant levels and a rather complicated response of the PM components, leading to small net changes. Sulfate increases (8–17%), nitrate decreases (18– 42%), organic PM slightly increases, and ammonium either increases or decreases a little. The reduction of VOC emissions during the summer causes on average a small increase of the oxidant levels and a marginal increase in PM_2.5. This small net change is due to increases in the inorganic components and decreases of the organic ones. Reduction of VOC emissions during winter results in a decrease of the oxidant levels and a 5–10% reduction of PM_2.5 because of reductions in nitrate (4–19%), ammonium (4–10%), organic PM (12–14%), and small reductions in sulfate. Although sulfur dioxide (SO₂) reduction is the single most effective approach for sulfate control, the coupled decrease of SO₂ and NO_x emissions in both seasons is more effective in reducing total PM_2.5 mass than the SO₂ reduction alone.     

Modeling an air pollution episode in northwestern United States: Identifying the effect of nitrogen oxide and volatile organic compound emission changes on air pollutants formation using direct sensitivity analysis

Air quality impacts of volatile organic compound (VOC) and nitrogen oxide (NO_x) emissions from major sources over the northwestern United States are simulated. The comprehensive nested modeling system comprises three models: Community Multiscale Air Quality (CMAQ), Weather Research and Forecasting (WRF), and Sparse Matrix Operator Kernel Emissions (SMOKE). In addition, the decoupled direct method in three dimensions (DDM-3D) is used to determine the sensitivities of pollutant concentrations to changes in precursor emissions during a severe smog episode in July of 2006. The average simulated 8-hr daily maximum O₃ concentration is 48.9 ppb, with 1-hr O₃ maxima up to 106 ppb (40 km southeast of Seattle). The average simulated PM_2.5 (particulate matter with an aerodynamic diameter <2.5 μm) concentration at the measurement sites is 9.06 μg m^?3, which is in good agreement with the observed concentration (8.06 μg m^?3). In urban areas (i.e., Seattle, Vancouver, etc.), the model predicts that, on average, a reduction of NO_x emissions is simulated to lead to an increase in average 8-hr daily maximum O₃ concentrations, and will be most prominent in Seattle (where the greatest sensitivity is??0.2 ppb per % change of mobile sources). On the other hand, decreasing NO_x emissions is simulated to decrease the 8-hr maximum O₃ concentrations in remote and forested areas. Decreased NO_x emissions are simulated to slightly increase PM_2.5 in major urban areas. In urban areas, a decrease in VOC emissions will result in a decrease of 8-hr maximum O₃ concentrations. The impact of decreased VOC emissions from biogenic, mobile, nonroad, and area sources on average 8-hr daily maximum O₃ concentrations is up to 0.05 ppb decrease per % of emission change, each. Decreased emissions of VOCs decrease average PM_2.5 concentrations in the entire modeling domain. In major cities, PM_2.5 concentrations are more sensitive to emissions of VOCs from biogenic sources than other sources of VOCs. These results can be used to interpret the effectiveness of VOC or NO_x controls over pollutant concentrations, especially for localities that may exceed National Ambient Air Quality Standards (NAAQS).

Implications: The effect of NO_x and VOC controls on ozone and PM_2.5 concentrations in the northwestern United States is examined using the decoupled direct method in three dimensions (DDM-3D) in a state-of-the-art three-dimensional chemical transport model (CMAQ). NO_x controls are predicted to increase PM_2.5 and ozone in major urban areas and decrease ozone in more remote and forested areas. VOC reductions are helpful in reducing ozone and PM_2.5 concentrations in urban areas. Biogenic VOC sources have the largest impact on O₃ and PM_2.5 concentrations.     

Comparative Study of Spray Booth Filter System Efficiency

ABSTRACT

During recent years, greater emphasis has been placed on the control of particulate emissions from painting operations. This has gained more importance as more is learned about the potential release of toxic metals to the atmosphere from painting operations. This has led to queries about the efficiency of various painting arrestor systems to reduce particulate discharges to the atmosphere. Even more important is the capability of the arrestor systems to control PM₁₀ emissions.

In 1995, the U.S. Environmental Protection Agency initiated a study to evaluate various dry paint overspray arrestor systems. This study was designed to evaluate not only the total emissions control capability of the arrestor but also the PM₁₀ control capability of the various system designs. Paint overspray arrestor systems using five different filtration concepts or materials were selected. They include systems constructed of fiberglass, paper, Styrofoam, and cardboard materials. These systems used filtration techniques incorporating the following filtration phenomena and designs: cyclone, baffle, bag systems, and mesh systems.

The testing used an optical particle counting procedure to determine the concentration of particles of a given size fraction to penetrate a test arrestor system. The results of the testing indicated that there are significant differences in the efficiency of the tested system designs to capture and retain PM₁₀.

This paper summarizes the results of the research conducted to determine the capability of the arrestor systems to capture particulate of sizes down to approximately 1 μm in surface diameter.     

Air Quality Modeling of Interpollutant Trading for Ozone Precursors in an Urban Area

Abstract

Emission trading is a market‐based approach designed to improve the efficiency and economic viability of emission control programs; emission trading has typically been confined to trades among single pollutants. Interpollutant trading (IPT), as described in this work, allows for trades among emissions of different compounds that affect the same air quality end point, in this work, ambient ozone (O₃) concentrations. Because emissions of different compounds impact air quality end points differently, weighting factors or trading ratios (tons of emissions of nitrogen oxides (NO_x) equivalent to a ton of emissions of volatile organic compounds [VOCs]) must be developed to allow for IPT. In this work, IPT indices based on reductions in O₃ concentrations and based on reductions in population exposures to O₃ were developed and evaluated using a three‐dimensional gridded photochemical model for Austin, TX, a city currently on the cusp of nonattainment with the National Ambient Air Quality Standards for O₃ concentrations averaged over 8 hr. Emissions of VOC and NO_x from area and mobile sources in Austin are larger than emissions from point sources. The analysis indicated that mobile and area sources exhibited similar impacts. Trading ratios based on maximum O₃ concentration or population exposure were similar. In contrast, the trading ratios did exhibit significant (more than a factor of two) day‐to‐day variability. Analysis of the air quality modeling indicated that the daily variability in trading ratios could be attributed to daily variations in both emissions and meteorology.     

Air pollutant emissions from the development,production, and processing of Marcellus Shale natural gas

The Marcellus Shale is one of the largest natural gas reserves in the United States; it has recently been the focus of intense drilling and leasing activity. This paper describes an air emissions inventory for the development, production, and processing of natural gas in the Marcellus Shale region for 2009 and 2020. It includes estimates of the emissions of oxides of nitrogen (NO_x), volatile organic compounds (VOCs), and primary fine particulate matter (≤2.5 µm aerodynamic diameter; PM_2.5) from major activities such as drilling, hydraulic fracturing, compressor stations, and completion venting. The inventory is constructed using a process-level approach; a Monte Carlo analysis is used to explicitly account for the uncertainty. Emissions were estimated for 2009 and projected to 2020, accounting for the effects of existing and potential additional regulations. In 2020, Marcellus activities are predicted to contribute 6–18% (95% confidence interval) of the NO_x emissions in the Marcellus region, with an average contribution of 12% (129 tons/day). In 2020, the predicted contribution of Marcellus activities to the regional anthropogenic VOC emissions ranged between 7% and 28% (95% confidence interval), with an average contribution of 12% (100 tons/day). These estimates account for the implementation of recently promulgated regulations such as the Tier 4 off-road diesel engine regulation and the U.S. Environmental Protection Agency's (EPA) Oil and Gas Rule. These regulations significantly reduce the Marcellus VOC and NO_x emissions, but there are significant opportunities for further reduction in these emissions using existing technologies.

Implications: The Marcellus Shale is one of the largest natural gas reserves in United States. The development and production of this gas may emit substantial amounts of oxides of nitrogen and volatile organic compounds. These emissions may have special significance because Marcellus development is occurring close to areas that have been designated nonattainment for the ozone standard. Control technologies exist to substantially reduce these impacts. PM_2.5 emissions are predicted to be negligible in a regional context, but elemental carbon emissions from diesel powered equipment may be important.     

Resolving the interactions between population density and air pollution emissions controls in the San Joaquin Valley,USA

The effectiveness of emissions control programs designed to reduce concentrations of airborne particulate matter with an aerodynamic diameter <2.5 μm (PM_2.5) in California's San Joaquin Valley was studied in the year 2030 under three growth scenarios: low, medium, and high population density. Base-case inventories for each choice of population density were created using a coupled emissions modeling system that simultaneously considered interactions between land use and transportation, area source, and point source emissions. The ambient PM_2.5 response to each combination of population density and emissions control was evaluated using a regional chemical transport model over a 3-week winter stagnation episode. Comparisons between scenarios were based on regional average and population-weighted PM_2.5 concentrations. In the absence of any emissions control program, population-weighted concentrations of PM_2.5 in the future San Joaquin Valley are lowest under growth scenarios that emphasize low population density. A complete ban on wood burning and a 90% reduction in emissions from food cooking operations and diesel engines must occur before medium- to high-density growth scenarios result in lower population-weighted concentrations of PM_2.5. These trends partly reflect the fact that existing downtown urban cores that naturally act as anchor points for new high-density growth in the San Joaquin Valley are located close to major transportation corridors for goods movement. Adding growth buffers around transportation corridors had little impact in the current analysis, since the 8-km resolution of the chemical transport model already provided an artificial buffer around major emissions sources.

Assuming that future emissions controls will greatly reduce or eliminate emissions from residential wood burning, food cooking, and diesel engines, the 2030 growth scenario using “as-planned” (medium) population density achieves the lowest population-weighted average PM_2.5 concentration in the future San Joaquin Valley during a severe winter stagnation event.

Implications: The San Joaquin Valley is one of the most heavily polluted air basins in the United States that are projected to experience strong population growth in the coming decades. The best plan to improve air quality in the region combines medium- or high-density population growth with rigorous emissions controls. In the absences of controls, high-density growth leads to increased population exposure to PM_2.5 compared with low-density growth scenarios (urban sprawl).     

Trends in primary particulate matter emissions from Canadian agriculture

Particulate matter (PM) has long been recognized as an air pollutant due to its adverse health and environmental impacts. As emission of PM from agricultural operations is an emerging air quality issue, the Agricultural Particulate Matter Emissions Indicator (APMEI) has been developed to estimate the primary PM contribution to the atmosphere from agricultural operations on Census years and to assess the impact of practices adopted to mitigate these emissions at the soil landscape polygon scale as part of the agri-environmental indicator report series produced by Agriculture and Agri-Food Canada. In the APMEI, PM emissions from animal feeding operations, wind erosion, land preparation, crop harvest, fertilizer and chemical application, grain handling, and pollen were calculated and compared for the Census years of 1981–2006. In this study, we present the results for PM₁₀ and PM_2.5, which exclude chemical application and pollen sources as they only contribute to total suspended particles. In 2006, PM emissions from agricultural operations were estimated to be 652.6 kt for PM₁₀ and 158.1 kt for PM_2.5. PM emissions from wind erosion and land preparation account for most of PM emissions from agricultural operations in Canada, contributing 82% of PM₁₀ and 76% of PM_2.5 in 2006. Results from the APMEI show a strong reduction in PM emissions from agricultural operations between 1981 and 2006, with a decrease of 40% (442.8 kt) for PM₁₀ and 47% (137.7 kt) for PM_2.5. This emission reduction is mainly attributed to the adoption of conservation tillage and no-till practices and the reduction in the area of summerfallow land.

Implications: Increasing sustainability in agriculture often means adapting management practices to have a beneficial impact on the environment while maintaining or increasing production and economic benefits. We developed an inventory of primary PM emissions from agriculture in Canada to better quantify the apportionment, spatial distribution, and trends for Census years 1981–2006. We found major reductions of 40% in PM₁₀ and 47% in PM_2.5 emissions over the 25-yr period as a co-benefit of increasing carbon sequestration in agricultural soils. Indeed, farmers adopted conservation tillage/no-till practices, increased usage of cover crops, and reduced summerfallow, in order to increase soil organic matter and reduce carbon dioxide emissions, which also reduced primary PM emissions, although the agricultural production increased over the period.     

Particulate Emissions from Construction Activities

Abstract

Although it has long been recognized that road and building construction activity constitutes an important source of particulate matter (PM) emissions throughout the United States, until recently only limited research has been directed to its characterization. This paper presents the results of PM₁₀ and PM_2.5 (particles ≤10 μm and ≤2.5 μm in aerodynamic diameter, respectively) emission factor development from the onsite testing of component operations at actual construction sites during the period 1998 –2001. Much of the testing effort was directed at earthmoving operations with scrapers, because earthmoving is the most important contributor of PM emissions across the construction industry. Other sources tested were truck loading and dumping of crushed rock and mud and dirt carryout from construction site access points onto adjacent public paved roads. Also tested were the effects of watering for control of scraper travel routes and the use of paved and graveled aprons at construction site access points for reducing mud and dirt carryout. The PM₁₀ emissions from earthmoving were found to be up to an order of magnitude greater than predicted by AP-42 emission factors drawn from other industries. As expected, the observed PM_2.5:PM₁₀ emission factor ratios reflected the relative importance of the vehicle exhaust and the resuspended dust components of each type of construction activity. An unexpected finding was that PM_2.5 emissions from mud and dirt carryout were much less than anticipated. Finally, the control efficiency of watering of scraper travel routes was found to closely follow a bilinear moisture model.     

Day-of-Week Patterns of Particulate Matter and Its Chemical Components at Selected Sites in California

Abstract

This paper analyzes day-of-week variations in concentrations of particulate matter (PM) in California. Because volatile organic compounds (VOCs) and oxides of nitrogen (NO_x) are not only precursors of ozone (O₃) but also of secondary PM, it is useful to know whether the variations by day of week in these precursors are also evident in PM data. Concentrations of PM ≤10 μm (PM₁₀) and ≤2.5[H9262]m in aerodynamic diameter (PM_2.5) were analyzed. PM concentrations exhibit a general weekly pattern, with the maximum occurring late in the workweek and the minimum occurring on weekends (especially Sunday); however, this pattern does not prevail at all sites and areas. PM nitrate (NO₃ ^-) data from Size Selective Inlet (SSI) samplers in the South Coast Air Basin (SoCAB) tend to be somewhat lower on weekends compared with weekdays. During 1988–1991, the weekend average was lower than the weekday average at 8 of 13 locations, with an average decrease of 1%. During 1997–2000, the weekend average was lower than the weekday average at 10 of 13 locations, with an average decrease of 6%. The weekend averages are generally lower than weekday averages for sulfates, organic carbon, and elemental carbon. Because heavy-duty trucks typically represent a major source of elemental carbon, the weekend decrease in heavy-duty truck traffic may also result in a decrease in ambient elemental carbon concentrations.     

Air Quality Management in Los Angeles: Perspectives on Past and Future Emission Control Strategies

The 1988 Air Quality Management Plan was approved by the Board of the California South Coast Air Quality Management District in March 1989. The District comprises the counties of Los Angeles, Orange, and Riverside, and the non-desert portion of San Bernardino county. Emissions reductions in the past have lead to significant improvement in air quality despite large increases in growth. However, the District, largely because of continuous growth, currently violates the air quality standards for ozone, carbon monoxide, nitrogen dioxide, and respirable particulate matter (PM₁₀). Based upon the AQMP, reduction of approximately 80 percent in emissions of oxides of nitrogen and volatile organic compounds is required to bring the District into compliance with all air quality standards in the next twenty years.

Achieving compliance will necessitate the use of advanced technologies, as well as some changes in lifestyle and management practices. Advanced technologies, including the use of electric vehicles powered by batteries or fuel cells, the use of cleaner burning fuels and advanced combustion modifications, and treatment of surface coatings and solvents are included in the AQMP. The Technology Advancement Office in the District was created to work with industry, universities, research institutes, and other local, state and federal agencies to identify, evaluate, and promote low emitting fuels and technologies. In addition to electricity, fuels burning cleaner than conventional gasoline or diesel are being tested to obtain emissions and durability data so that rational choices can be made for the future. Compressed natural gas, methanol and liquefied petroleum gas are considered to be cleaner burning fuels for current applications. Ethanol, butane, and various oxygenated blends are being evaluated, and the broader application of solar energy and hydrogen are being investigated.

The impact of various cleaner burning fuels on air quality is being addressed. To date, methanol is the only fuel for which results are available. These results indicate that methanol use in vehicles—with control of formaldehyde emissions below 15 mg/mile for light-duty vehicles—can provide air quality benefits for all criteria pollutants and certain air toxics. These benefits are greater for M₁₀₀ than M₈₅.

Several District advanced technology programs are described, including a reduction in emissions from paints and coatings, and the demonstration of electric vehicles.     

Modelling long-range transport of primary particulate material over Europe

This paper uses a simple model of atmospheric transport and an emissions inventory prepared by TNO to estimate the contribution of primary particulate material to PM₁₀ and PM_2.5 concentration across Europe. The resulting population exposure is compared with that of secondary particulates, and it is noted that both primary and secondary contributions will be significantly reduced with the implementation of new protocols under the Convention on Long-Range Transboundary Air Pollution (CLRTAP). Since concentrations of primary PM₁₀ can become elevated in episodic situations, when long-range transport of particulate could, on its own, exceed 24 h average targets of 50 μg m⁻³ over large areas of Europe, such reduction is important for achievement of current air quality standards to control exposure to atmospheric particulate PM₁₀.     

Marginal PM25: Nonlinear Aerosol Mass Response to Sulfate Reductions in the Eastern United States

ABSTRACT

Reductions in airborne sulfate concentration may cause inorganic fine particulate matter (PM₂₅) to respond nonlinearly, as nitric acid gas may transfer to the aerosol phase. Where this occurs, reductions in sulfur dioxide (SO₂) emissions will be much less effective than expected at reducing PM_2.5. As a measure of the efficacy of reductions in sulfate concentration on PM , we define marginal PM_2.5 as the local change in PM_2.5 resulting from a small change in sulfate concentration. Using seasonal-average conditions and assuming thermodynamic equilibrium, we find that the conditions for PM_2.5 to respond nonlinearly to sulfate reductions are common in the eastern United States in winter, occurring at half of the sites considered, and uncommon in summer, due primarily to the influence of temperature. Accounting for diurnal and intraseasonal variability, we find that seasonal-average conditions provide a reasonable indicator of the time-averaged PM_2.5 response. These results indicate that reductions in sulfate concentration may be up to 50% less effective at reducing the annual-average PM_2.5 than if the role of nitric acid is neglected. Further, large reductions in sulfate will also cause an increase in aerosol nitrate in many regions that are the most acidic.     

Sulfur Dioxide and Nitrogen Oxides Emissions from U.S. Pulp and Paper Mills, 1980–2005

Abstract

Comprehensive surveys conducted at 5-yr intervals were used to estimate sulfur dioxide (SO₂) and nitrogen oxides (NO_x) emissions from U.S. pulp and paper mills for 1980, 1985, 1990, 1995, 2000, and 2005. Over the 25-yr period, paper production increased by 50%, whereas total SO₂ emissions declined by 60% to 340,000 short tons (t) and total NO_x emissions decreased approximately 15% to 230,000 t. The downward emission trends resulted from a combination of factors, including reductions in oil and coal use, steadily declining fuel sulfur content, lower pulp and paper production in recent years, increased use of flue gas desulfurization systems on boilers, growing use of combustion modifications and add-on control systems to reduce boiler and gas turbine NO_x emissions, and improvements in kraft recovery furnace operations.     

Particulate Matter in California: Part 2—Spatial,Temporal, and Compositional Patterns of PM2.5, PM10–2.5, and PM10

Abstract

Geographic and temporal variations in the concentration and composition of particulate matter (PM) provide important insights into particle sources, atmospheric processes that influence particle formation, and PM management strategies. In the nonurban areas of California, annual-average PM_2.5 and PM₁₀ concentrations range from 3 to 10 [H9262]g/m³ and from 5 to 18 µg/m³, respectively. In the urban areas of California, annual-averages for PM_2.5 range from 7 to 30 [H9262]g/m³, with observed 24-hr peaks reaching levels as high as 160 [H9262]g/m³. Within each air basin, exceedances are a mixture of isolated events as well as periods of elevated PM_2.5 concentrations that are more prolonged and regional in nature. PM_2.5 concentrations are generally highest during the winter months. The exception is the South Coast Air Basin, where fairly high values occur throughout the year. Annual-average PM_2.5 mass, as well as the concentrations of major components, declined from 1988 to 2000. The declines are especially pronounced for the sulfate (SO₄ ^2?) and nitrate (NO₃ ^?) components of PM_2.5 and PM₁₀ and correlate with reductions in ambient levels of oxides of sulfur (SO_x) and oxides of nitrogen (NO_x). Annual averages for PM_10–2.5 and PM₁₀ exhibited similar downwind trends from 1994 to 1999, with a slightly less pronounced decrease in the coarse fraction.     

Nitrate Artifacts during PM25 Sampling in the South Coast Air Basin of California

ABSTRACT

In February 1993, the South Coast Air Basin (SCAB) was redesignated as a “serious” nonattainment area for PM10. To improve the understanding and characterization of fine particulate matter in the SCAB, the South Coast Air Quality Management District (SCAQMD) initiated a comprehensive PM₁₀ Technical Enhancement Program (PTEP). Using enhanced PTEP monitors (specially designed multichannel/multifilter samplers), a one-year fine particulate matter (PM) monitoring program was initiated in January 1995. As part of the special monitoring program, nitric acid, ammonia, and speciated PM₁₀ and PM_2.5 concentrations were measured at five locations in the SCAB (downtown Los Angeles, Anaheim, Diamond Bar, Fontana, and Rubidoux) and at one background station (San Nicolas Island). The PM2.5 data are the first spatially resolved speciated data collected in the SCAB on an annual basis. Within the SCAB, where nitrate is a major component of PM_2.5, nitrate losses have been documented. The spatial and temporal variations of the nitrate losses during PM_2.5 sampling and the uncertainties of the nitrate losses are discussed. Significant losses occur at a low mass range, between 10 and 50 ìg/m³. Significant gains occur at an even lower mass range of less than 30 ìg/m³. On an annual average basis, nitrate losses vary between 1.25 and 2.32 ìg/m³ and the SCAB-wide average value of nitrate loss is 1.8 ìg/m³ based on five PTEP stations in the SCAB. The maximum nitrate losses for each station vary from 6.4 ìg/m³ to 22.5 ìg/m ³. Theoretical prediction of the sampling efficiency of the nitrate during PM_2.5 sam - pling was compared with the PTEP data. In general, theoretical prediction was in good agreement with measured values.     

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.