Size and Composition Distributions of Particulate Matter Emissions: Part 1—Light-Duty Gasoline Vehicles

Abstract

Size-resolved particulate matter (PM) emitted from light-duty gasoline vehicles (LDGVs) was characterized using filter-based samplers, cascade impactors, and scanning mobility particle size measurements in the summer 2002. Thirty LDGVs, with different engine and emissions control technologies (model years 1965–2003; odometer readings 1264–207,104 mi), were tested on a chassis dynamometer using the federal test procedure (FTP), the unified cycle (UC), and the correction cycle (CC). LDGV PM emissions were strongly correlated with vehicle age and emissions control technology. The oldest models had average ultrafine PM_0.1 (0.056- to 0.1-μm aerodynamic diameter) and fine PM_1.8 (≤1.8-μm aerodynamic diame ter) emission rates of 9.6 mg/km and 213 mg/km, respectively. The newest vehicles had PM_0.1 and PM_1.8 emis sions of 51 μg/km and 371 μg/km, respectively. Light duty trucks and sport utility vehicles had PM_0.1 and PM_1.8 emissions nearly double the corresponding emission rates from passenger cars. Higher PM emissions were associated with cold starts and hard accelerations. The FTP driving cycle produced the lowest emissions, followed by the UC and the CC. PM mass distributions peaked between 0.1-and 0.18-μm particle diameter for all vehicles except those emitting visible smoke, which peaked between 0.18 and 0.32 μm. The majority of the PM was composed of carbonaceous material, with only trace amounts of water-soluble ions. Elemental carbon (EC) and organic matter (OM) had similar size distributions, but the EC/OM ratio in LDGV exhaust particles was a strong function of the adopted emissions control technology and of vehicle maintenance. Exhaust from LDGV classes with lower PM emissions generally had higher EC/OM ratios. LDGVs adopting newer technologies were characterized by the highest EC/OM ratios, whereas OM dominated PM emissions from older vehicles. Driving cycles with cold starts and hard accelerations produced higher EC/OM ratios in ultrafine particles.     

Particulate Matter in California: Part 1—Intercomparison of Several PM2.5, PM10–2.5, and PM10 Monitoring Networks

Abstract

It will be many years before the recently deployed network of fine particulate matter with an aerodynamic diameter less than 2.5 [H9262]m (PM_2.5) Federal Reference Method (FRM) samplers produces information on nonattainment areas, trends, and source impacts. However, data on PM_2.5 and its major constituents have been routinely collected in California for the past 20 years. The California Air Resources Board operated as many as 20 dichotomous (dichot) samplers for PM_2.5 and coarse PM (PM_10–2.5). The California Acid Deposition Monitoring Program (CADMP) collected 12-h-average PM_2.5 and PM₁₀ from 1988 to 1995 at ten urban and rural sites and 24-h-average PM_2.5 at five urban sites since 1995. Beginning in 1994, the Children’s Health Study collected 2-week averages of PM_2.5 in 12 communities in southern California using the Two-Week Sampler (TWS). Comparisons of collocated samples establish relationships between the dichot, CADMP, and TWS samplers and the 82-site network of PM_2.5 FRM samplers deployed since 1999 in California. PM mass data from the different monitoring programs have modest to high correlation to FRM mass data, fairly small systematic biases and negative proportional biases ranging from 7 to 22%. If the biases are taken into account, all of the programs should be considered comparable with the FRM program. Thus, historical data can be used to develop long-term PM trends in California.     

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.     

On the Determination of Odor Thresholds in Air Pollution Control—An Experimental Field Study on Flue Gases from Sulfate Cellulose Plants

From the hygienic point of view, not only the health hazards caused by air pollutants but also the odor from emitted flue gases should be reduced to a minimum. An effective control of the risk of odor at ground level presupposes knowledge of the source concentration of the odoriferous gas as well as its odor threshold. This threshold has to be estimated empirically, as the flue gases often contain a complex mixture of different odoriferous substances, the odor thresholds of which are in most cases unknown. For this purpose a method has been developed for estimating the odor thresholds of flue gases emitted, from different industrial processes. The method, afield method, is based on an exposure procedure, a number of subjects compare different concentrations of the flue gas with samples of fresh air and decide at what concentration the flue gas is no longer noticeable. The gas samples used are neither compressed, nor absorbed or heated before the exposure test. The method has been used in two studies on gases from Swedish sulfate cellulose plants. In order to estimate the effect on the odor threshold of different deodorizing measures, gas samples were taken not only from the stack but also from different phases in the production process. The results and a brief discussion on the practical applications of the method are given.     

Determination of Atmospheric Nitrogen Input to Lake Greenwood,South Carolina: Part 2—Gaseous Measurements and Modeling

Abstract

The Reedy River branch of Lake Greenwood, SC, has repeatedly experienced summertime algal blooms, upsetting the natural system. A series of experiments were carried out to investigate atmospheric nitrogen (N) input into the lake. N was examined because of the insignificant phosphorus dry atmospheric flux and the unique nutrient demands of the dominant algae (Pithophora oedogonia) contributing to the blooms. Episodic atmospheric measurements during January and March 2001 have shown that the dry N flux onto the lake ranged from 0.9 to 17.4 kg N/ha-yr, and on average is caused by nitric acid (HNO₃; 31%), followed by nitrogen dioxide (NO₂; 23%), fine ammonium (NH₄ ⁺; 20%), coarse nitrate (NO₃ ^?; 16%), fine NO₃ ⁺ (5%), and coarse NH₄ ⁺ (5%). Similar measurements in Greenville, SC (the upper watershed of the Reedy River), showed that the dry N deposition flux there ranged from 1.4 to 9.7 kg N/ha-yr and was mostly caused by gaseous deposition (40% NO₂ and 40% HNO₃). The magnitude of this dry N deposition flux is comparable to wet N flux as well as other point sources in the area. Thermodynamic modeling showed low concentrations of ammonia, relative to the particulate NH₄ ⁺ concentrations.     

Atmospheric dispersion and transport within coastal regions—Part II. Tracer study of industrial emissions in the California Delta Region

Eight large-scale atmospheric tracer tests, utilizing CBrF₃ and/or SF₆, were conducted during September, 1976, within the California Delta Region. The purpose of this study was to demonstrate the large-scale application of single and double tracer techniques to the study of pollutant transport and dispersion under complex, coastal meteorological conditions.The resulting tracer data base was comprehensive enough to permit accurate mass balances of the tracer; essentially all of the tracer was accounted for by this analysis. On the average, plumes emitted from the Montezuma Hills during the test periods were transported southeast over Stockton into the San Joaquin Valley. As a result of the steady nature of the winds, the commonly used Hino correction was found to grossly underestimate the hourly averaged tracer concentrations computed from 10-s averaged concentrations.Experimentally determined rates of dispersion were greater than those associated with Pasquill-Gifford dispersion curves. In spite of the complex meteorology and terrain, estimates of tracer concentrations based upon the Gaussian plume model were found to be reasonably accurate.The relationship between the horizontal standard deviation of the wind, σ_θ, and the horizontal dispersion parameter of the plume, σ_y, was found to follow σ_y∼-0.85 xσ_θ, where x is the downwind distance of the plume center. Calculated trajectories and arrival times of air parcels based upon a numerical solution to the two-dimensional mass balance equation were found to be in excellent agreement with the tracer data.     

Effectiveness in the Use of Natural Gas for the Reduction of Atmospheric Emissions: Case Study—Industrial Sector in the Metropolitan Region of Santiago,Chile

Abstract

The purpose of this investigation was to quantify the potential of natural gas to reduce emissions from stationary combustion sources by analyzing the case study of the metropolitan region of Santiago, Chile. For such purposes, referential base scenarios have been defined that represent with and without natural gas settings. The method to be applied is an emission estimate based on emission factors. The results for this case study reveal that stationary combustion sources that replaced their fuel reduced particulate matter (PM) emissions by 61%, sulfur oxides (SO_x) by 91%, nitrogen oxides (NO_x) by 40%, and volatile organic compounds (VOC) by 10%. Carbon mon-oxide (CO) emissions were reduced by 1%. As a result of this emission reduction, in addition to reductions caused by other factors, such as a shift to cleaner fuels other than natural gas, technological improvements, and sources which are not operative, emission reduction goals set forth by the environmental authorities were broadly exceeded.     

Characterization of PM25 and PM10 in the South Coast Air Basin of Southern California: Part 2—Temporal Variations

ABSTRACT

The South Coast Air Quality Management District (SCAQMD) conducted a 1-year special particulate monitoring study from January 1995 to February 1996. This monitoring data indicates that high PM₁₀ and PM_{2 5} concentrations were observed in the fall (October, November, and December), with November concentrations being the highest. During the rest of the year, PM_2.5 and PM₁₀ masses gradually increased from January to September. Monthly PM₁₀ mass varied from 20 to 120 |ig/m³, and monthly PM₂₅ mass varied from 13 to 63 |j.g/m³. The PM_2.5-to-PM₁₀ ratio varied daily and ranged between 22 and 96%. Two types of high-PM days were observed. The first type was observed under fall stagnation conditions, which lead to high secondary species concentrations. The second type was observed under high wind conditions, which lead to high primary coarse particles of crustal components. The highest 24-hr average PM₁₀ concentration (226.3 |ig/m³) was observed at the Fontana station, while the highest PM₂₅ concentration (129.3 |ig/m³) was observed at the Diamond Bar station.     

Spatial and Temporal Variability of Ozone Exposure in Forested Areas of the United States and Canada: 1978—1988

Ambient O₃ exposures have reduced growth rates of tree genotypes in some areas of the United States. For characterizing O₃ exposures in forested areas, data from primarily population-oriented sites have been used. It has been speculated that exposures calculated from population-oriented sites provide estimates greater than those that would actually be experienced in the majority of forested areas. Accordingly, we compared 1988 O₃ data from three remote forested sites with data from several population-oriented monitoring sites in and around the mid? and southern Appalachian Mountains. The number of hours ≥0.08 ppm was lower at the remote forested sites than at the nearby population-oriented locations. In addition, we characterized the temporal variability of O₃ exposures in forested regions of the United States and Canada for the period 1978-1988. We found that the years of highest O₃ exposure in the eastern United States during 1978-1988 were 1978, 1980, 1983, and 1988, with 1988 being the worst year in four of seven eastern forest regions. In 1988, the Whiteface Mountain summit site (1483 m) experienced approximately 10 percent more hourly average concentrations ≥0.08 ppm than in the second highest O₃ exposure year (i.e., 1979). Consistently throughout the 11-year period, the highest O₃ exposures at the Whiteface Mountain site occurred during the late evening and early morning hours, with the result that the longterm 7-h (0900-1559h) exposure index could not distinguish those years in which the highest exposures occurred from those in which the lowest occurred. Similar to the Whiteface Mountain site, two high-elevation Shenandoah National Park sites experienced their highest O₃ exposures in 1988. With the exception of 1986, the lower elevation site (Dickey Ridge) consistently experienced more frequent occurrences of hourly average concentrations ≥0.08 ppm than the higher elevation site (Big Meadows).     

Dioxin/POPs legacy of pesticide production in Hamburg: Part 1—securing of the production area

α-Hexachlorocyclohexane (HCH), β-HCH, and γ-HCH (lindane) were recently included as new persistent organic pollutants (POPs) in the Stockholm Convention. Therefore, the chemicals need to be globally addressed, including the disposal of historic wastes. At most sites, the approximately 85 % of HCH waste isomers were dumped. At a former lindane factory in Hamburg and some other factories the HCH, waste was recycled producing residues with high polychlorinated dibenzo-p-dioxin and dibenzofuran (PCDD/PCDF) levels. The soil and ground water under the former pesticide factory was/is highly contaminated with HCH (260 tons), chlorobenzenes (550 tons), and PCDD/PCDF (6 kg toxic equivalents (TEQ)). This contamination did not result from disposal operations but from spillages and leakages during the 30 years of the factory's production history. A containment wall has been constructed around the production area to prevent the dispersal of the pollutants. The ground water is managed by a pump and treat system. Over the last 15 years, approximately 10–30 tons of this pollution reservoir has been pumped and incinerated. For the contaminated production buildings, specific assessment and demolition technologies have been applied. In addition to their HCH waste isomer deposition, former lindane/HCH productions need to be assessed for possible recycling practice of HCH and related PCDD/PCDF contamination of the production area and buildings. Since such recycling activities have taken place at several factories in different countries, the experience of assessment and management of the described production area and contaminated buildings could be valuable. Such assessment could be addressed within the frame of the Stockholm Convention.     

Assessment on the effectiveness of environmental regulation in China—evidence from a panel data analysis

Environmental Science and Pollution Research - In the context of global warming and environmental deterioration, the environment impact assessment is a crucial institutional guaranty to assure less...     

The fluorocarbon-ozone theory—VI. Atmospheric modeling: Calculation of the diurnal steady state

In the recent past there has been a general effort to develop one-dimensional models of stratospheric transport and photochemistry which include the effects of Rayleigh scattering of the solar radiation and diurnal changes in the solar zenith angle. Direct integration of the diurnal problem is so expensive and time consuming that it cannot be generally applied. It is therefore necessary to seek other numerical approaches which will allow accurate diurnal averaging while retaining most of the features of the more sophisticated 24 h average models.In the present paper we describe an approach to the diurnal problem which includes all of the important features of conventional one-dimensional models (Rayleigh scattering, diffusion of all species, updating of photolytic rate constants, etc.) and, at the same time gives an accurate diurnal steady state and accurate diurnal steady ozone perturbations with modest computation times.It is shown that the “diurnal correction” prior to recent redeterminations of the rate constant for the reaction HO₂ + NO → OH + NO₂ was 70%. With the inclusion of the new rate information the “diurnal correction” is 30%. The ozone depletion calculated for steady state fluorocarbon release at 1975 levels, with the assumptions outlined in this paper are 7.9% and 14.2% for the old and new HO₂ + NO rates respectively.     

Ammonia abatement and its impact on emissions of nitrous oxide and methane in Europe—Part 1: method

Agriculture is an important source of NH₃, which contributes to acidification and eutrophication, as well as emissions of the greenhouse gases CH₄ and N₂O. Because of their common sources, emission reduction measures for one of these gases may affect emissions of others. These interrelations are often ignored in policy making. This study presents an analysis of the effects of measures to reduce NH₃ emissions on emissions of N₂O and CH₄ from agriculture in Europe. The analysis combines information from the NH₃ module of the Regional Air pollution INformation and Simulation (RAINS) model for Europe with the IPCC method for national greenhouse gas inventories. The IPCC method for estimating agricultural emissions of N₂O and CH₄ is adjusted in order to use it in combination with the RAINS database for the European agricultural sector. As an example, we applied the adjusted method to the agricultural sector in the Netherlands and found that application of several NH₃ abatement options may result in a substantial increase in N₂O emissions while the effect on CH₄ emissions is relatively small. In Part 2 of this paper we focus on the resulting emissions for all European countries for 1990 and 2010.     

The Ozone Productivity of n-Propyl Bromide: Part 2—An Exception to the Maximum Incremental Reactivity Scale

Abstract

In an earlier paper the ozone-forming potential of n-propyl bromide (NPB) was studied with a new methodology designed to address issues associated with a marginal smog-forming compound. However, the U.S. Environmental Protection Agency (EPA) subsequently revised its policy and now recommends using the Maximum Incremental Reactivity (MIR) scale to rank the ozone-forming potential of all volatile organic compounds (VOCs), including those of marginal ozone productivity. Nevertheless, EPA contemplated exceptions to the box-model-derived MIR scale by allowing use of photochemical grid-model simulations for case specific reactivity assessments. The California Air Resources Board (CARB) also uses the MIR scale and CARB has a Reactivity Scientific Advisory Committee that can consider exceptions to the MIR scale. In this study, grid-model simulations that were recommended by EPA are used to evaluate the incremental ozone impacts of NPB using an update to the chemical mechanism developed in an earlier paper. New methods of analysis of the grid-model output are further developed here to quantify the relative reactivities between NPB and ethane over a wide range of conditions. The new grid-model-based analyses show that NPB is significantly different and generally less in ozone-forming potential (i.e., reactivity) than predicted by the box-model-based MIR scale relative to ethane, EPA’s “bright-line” test for non-VOC status. Although NPB has low reactivity compared to typical VOCs on any scale, the new grid-model analyses developed here show that NPB is far less reactive (and even has negative reactivity) compared to the reactivity predicted by the MIR scale.     

A History of the Production and Use of Carbon Tetrachloride,Tetrachloroethylene, Trichloroethylene and 1,1,1-Trichloroethane in the United States: Part 2—Trichloroethylene and 1,1,1-Trichloroethane

Carbon tetrachloride (CTC), tetrachloroethylene (PCE), trichloroethylene (TCE) and 1,1,1-trichloroethane (TCA) were four of the most widely used cleaning and degreasing solvents in the United States. Part 2 of this article describes the history of TCE and TCA. TCE production in the United States began in the early 1920s. TCE was used as a replacement for petroleum distillates in the dry-cleaning industry, and became the solvent of choice for vapor degreasing in the 1930s. TCE’s use as a degreaser decreased in the 1960s due to toxicity concerns and the increasing popularity of TCA. Significant TCA use began in the 1950s with the development of suitable stabilizer formulations. In the 1990s, TCA was phased out under the Montreal Protocol due to its role in stratospheric ozone depletion.     

The dioxin/POPs legacy of pesticide production in Hamburg: Part 2—waste deposits and remediation of Georgswerder landfill

α-HCH, β-HCH, and γ-HCH (lindane) were listed as persistent organic pollutants in the Stockholm Convention. Therefore, they need to be globally addressed including the wastes remaining from historic use and production. While at most lindane production sites the unintentionally produced 85 % HCH waste isomers have been deposited, at a former pesticide factory in Hamburg-Moorfleet HCH waste isomers have been recycled from 1953 to 1984 by thermal decomposition to chlorobenzenes and resulted in high polychlorinated dibenzo-p-dioxin/polychlorinated dibenzofuran (PCDD/PCDF)-contaminated residues. The management of the PCDD/PCDF-contaminated waste from the former pesticide factory in Hamburg has been assessed and quantified. Based on past accredited PCDD/PCDF measurements, the registered 3,700 tonnes of disposed thermal HCH decomposition residue contained 333 to 854 kg of PCDD/PCDF toxicity equivalent (I-TEQ) in 53–102 tonnes total sum of PCDD/PCDF. The wastes have been deposited together with other wastes in landfills in Hamburg and other parts of Germany. For the Georgswerder landfill (Hamburg), where approximately 50 % of the PCDD/PCDF is disposed, current and previous situation and remediation activities are described. While PCDD/PCDF leaching from the landfill is controlled and incinerated, more water soluble organochlorines (vinyl chloride, cis-1,2-dichlorethene, chlorobenzenes) and benzene remain as a challenge for groundwater management. A comprehensive aftercare program has been established and will need to be operated by future generations including renewal of containment systems. Former lindane/HCH productions need—in addition to HCH deposits—to be assessed for possible recycling practice of HCH and related PCDD/PCDF-containing deposits. This could systematically be addressed within the Stockholm Convention implementation.     

Exploring the impact of transition in energy mix on the CO2 emissions from China’s power generation sector based on IDA and SDA

Environmental Science and Pollution Research - The energy transition from coal and oil to renewable energy, nuclear energy, and natural gas is a fundamental way for emission reduction of...     

Characterization of PM25 and PM10 in the South Coast Air Basin of Southern California: Part 1—Spatial Variations

ABSTRACT

In December 1994, the South Coast Air Quality Management District (SCAQMD) initiated a comprehensive program, the PM₁₀ Technical Enhancement Program (PTEP), to characterize fine PM in the South Coast Air Basin (SCAB). A 1-year special particulate monitoring project was conducted from January 1995 to February 1996 as part of the PTEP. Under this enhanced monitoring, HNO₃, NH₃, and speciated PM₁₀ and PM_2.5 concentrations were measured at five stations (Anaheim, downtown Los Angeles, Diamond Bar, Fontana, and Rubidoux) in the SCAB and at one background station at San Nicolas Island. PM_2.5 and PM₁₀ mass and 43 individual species were analyzed for a full chemical speciation of the particle data. The PTEP data indicate that the most abundant chemical components of PM₁₀ and PM₂₅ in the SCAB are NH₄+ (8-9% of PM₁₀ and 14-17% of PM₂₅), NO₃ ^- (23-26% of PM₁₀ and 28-41% of PM₂₅), SO₄= (6-11% of PM₁₀ and 9-18% of PM_{2 5}), organic carbon (OC) (15-19% of PM₁₀ and 18-26% of PM_2.5), and elemental carbon (EC) (5-8% of PM₁₀ and 8-13% of PM₂₅). On an annual average basis, PM₂₅ comprises 52-59% of the SCAB PM₁₀. Annual average PM₁₀ and PM_2.5 concentrations showed strong spatial variations, low at coastal sites and high at inland sites. Annual average PM₁₀ concentrations varied from 40.8 ug/m³ at Anaheim to 76.8 ug/m³ at Rubidoux, while annual average PM_2.5 concentrations varied from 21.7 ug/m³ at Anaheim to 39.8 ug/m³ at Rubidoux. The chemical characterizations of the PM_2.5 and PM₁₀ concentrations, as well as their spatial variations, were examined; the important findings are summarized in this paper, and the temporal variations are discussed in the companion paper.¹