Threshold Dependence of Mortality Effects for Fine and Coarse Particles in Phoenix,Arizona

ABSTRACT

Daily data for fine (<2.5 um) and coarse (2.5-10 um) particles are available for 1995-1997 from the U.S. Environmental Protection Agency (EPA) research monitor in Phoenix, AZ. Mortality effects on the 65 and over population were studied for both the city of Phoenix and for a region of about 50 mi around Phoenix. Coarse particles in Phoenix are believed to be natural in origin and spatially homogeneous, whereas fine particles are primarily vehicular in origin and concentrated in the city itself. For this reason, it is natural to focus on city mortality data when considering fine particles, and on region mortality data when considering coarse particles, and most of the results reported here correspond to those assignments.

After allowing for seasonality and long-term trend through a nonlinear (B-spline) trend curve, and also for meteorological effects based on temperature and specific humidity, a regression of mortality was performed on PM using several different measures for PM. Based on a linear PM effect, we found a statistically significant coefficient for coarse particles, but not for fine particles, contrary to what is widely believed about the effects of coarse and fine particles. An analysis of nonlinear pollution-mortality relationships, however, suggests that the true picture is more complicated than that. For coarse particles, the evidence for any nonlinear or threshold-based effect is slight. For fine particles, we found evidence of a threshold, most likely with values in the range of 20-25 ug/m³. We also found some evidence of interactions of the PM effects with season and year.

The main effect here is an apparent seasonal interaction in the coarse PM effect. An attempt was made to explain this in terms of seasonal variation in the chemical composition of PM, but this led to another counterintuitive result: the PM effect is highest in spring and summer, when the anthropogenic concentration of coarse PM is lowest as determined by a principal components analysis. There was no evidence of confounding between the fine and coarse PM effects. Although these results are based on one city and should be considered tentative until replicated in other studies, they suggest that the prevailing focus on fine rather than coarse particles may be an oversimplification. The study also shows that consideration of nonlinear effects can lead to real changes of interpretation and raises the possibility of seasonal effects associated with the chemical composition of PM.     

Mass and Elemental Composition of Fine and Coarse Particles in Six U.S. Cities

Inhalable particulate matter (IP) samples have been collected in six U.S. cities in conjunction with an air pollution health study. The IP were collected using dichotomous virtual impactors in two size ranges: fine particles (FP) having aerodynamic diameter (d_a) <2.5 μm, and coarse particles (CP) with 2.5 μm < da < 15 μm. The mass measurements were determined by beta-gauge attenuation. The elemental composition of the FP and CP were determined by X-ray fluorescence. The means and distributions for FP and CP and selected elemental data highlight the similarities and differences that exist among these cities in the health study. Examining the temporal variations gives additional information on the meteorology and sources influencing the FP and CP fractions of Inhalable particle mass.

Differences in the concentration (and ratios) of selected elements have indicated the varying presence of crustal, steel industry, automotive, oceanic and fuel combustion sources in these cities. The noted variation in the concentrations and character of ambient aerosols in these cities are pertinent to interpreting differences in population exposures.     

Continuous Monitoring of Ultrafine,Fine, and Coarse Particles in a Residence for 18 Months in 1999-2000

Abstract

Continuous monitors were employed for 18 months in an occupied townhouse to measure ultrafine, fine, and coarse particles; air change rates; wind speed and direction; temperature; and relative humidity (RH). A main objective was to document short-term and long-term variation in indoor air concentrations of size-resolved particles (0.01-20 μm) caused by (1) diurnal and seasonal variation of outdoor air concentrations and meteorological variables, (2) indoor sources such as cooking and using candles, and (3) activities affecting air change rates such as opening windows and using fans. A second objective was to test and compare available instruments for their suitability in providing real-time estimates of particle levels and ancillary variables.

Despite different measuring principles, the instruments employed in this study agreed reasonably well for particles less than 10 μm in diameter. The three instruments measuring fine and coarse particles (aerodynamic diameter between 0.3 and 20 μm) agreed to within 30% in their overall estimates of total volume. Two of these instruments employed optical scattering, and the third used an aerodynamic acceleration principle. However, several lines of evidence indicated that the instrument employing aerodynamic acceleration overestimated concentrations for particle diameters greater than 10 μm. A fourth instrument measuring ultrafine and accumulation-mode particles (0.01-1 μm) was operated with two different inlets providing somewhat different particle size ranges. The two inlets agreed in the ultrafine region (<0.1 μm) but diverged increasingly for larger particles (up to 0.445 μm).

Indoor sources affecting ultrafine particle concentrations were observed 22% of the time, and sources affecting fine and coarse particle concentrations were observed 12 and 15% of the time, respectively. When an indoor source was operating, particle concentrations for different sizes ranged from 2 to 20 times the average concentrations when no indoor source was apparent. Indoor sources, such as cooking with natural gas, and simple physical activities, such as walking, accounted for a majority (50-90%) of the ultrafine and coarse particle concentrations, whereas outdoor sources were more important for accumulation-mode particles between 0.1 and 1 um in diameter. Averaged for the entire year and including no periods when indoor sources were apparent, the number distribution was bimodal, with a peak at ~10 nm (possibly smaller), a shallow minimum at ~14 nm, and a second broad peak at ~68 nm. The volume distribution was also bimodal, with a broad peak at ~200 nm, a minimum at ~1.2 μm, and then an upward slope again through the remaining size fractions.

A database was created on a 5-min averaging time basis. It contains more than 90,000 measurements by two of the instruments and approximately 30,000 by the two optical scattering instruments. About 4500 hour-long average air change rates were also calculated throughout the year using a dedicated gas chromatograph with electron capture detection (GC/ECD). At high air change rates [>0.8 air changes per hour (hr^?1)], particle concentrations were either elevated (when no source was present) or depressed (when an indoor source was operating) by factors of up to 2 compared with low air change rates.     

Fine Particles and Oxidant Pollution: Developing an Agenda for Cooperative Research

ABSTRACT

This paper describes a background for the North American Research Strategy for Tropospheric Ozone (NARSTO) cooperative program integrating studies of O₃ and PM_{2 5}. It discusses several important aspects for rationalizing NARSTO's trinational investigative approach, including (1) an outlook on the state of knowledge about fine particles in the troposphere and their origins in Canada, Mexico, and the United States; (2) the need for enhancement and strengthening of key field measurements in relation to tropospheric chemistry and a health effects component; and (3) the use of a central theme for advancing air quality modeling using evolving techniques to integrate and guide key process-oriented field campaigns. The importance of organizing a scientific program to acquire “policy-relevant” information is stressed, noting cooperative research directions that address combined PM_2.5 and O₃ issues, illustrated through exploration of hypothetical pathways of PM_2.5 response to choices of O₃ and PM precursor emission reductions. The information needed for PM_2.5 research is noted to intersect in many cases with those of O₃, but diverge in other cases. Accounting for these distinctions is important for developing NARSTO's strategy over the next decade.     

Sampling Submicrometer Particles Suspended in Near Sonic and Supersonic Free Jets

This paper is concerned with sampling submicrometer particles in perisonic flows. The study employed a high volume (30-45 L/min) condensation aerosol generator to produce stearic acid particles having a mean diameter of 0.8μm and a geometric standard deviation of 1.28. The aerosol was diluted with dry air and accelerated to Mach 0.6, 0.8, 1.26, or 1.47 through a flow nozzle. Aerosol mass concentrations were determined using a small bore probe in the jet and by a large bore probe sampling isokinetically upstream of the jet nozzle. The results of both samples were compared to compute the sampling error associated with I ho high spood jot sample. The mass of stearic acid colloctod on polycarbonate mombrono flltors was determined by gravimoirlc and chromalogrophlc mothods. Studies at Mach 0.8 with four sampling probes having Inlet wall to bore area ratios ranging from 3.8 to 0.28 (a knife edge) demonstrated that probe wall thickness effects are not significant when the sample is extracted isokinetically. Subisokinetic experiments using the knife edged probe showed relative errors of 124 ± 12% when sampling at 2 0% of the isokinetic condition. The subisokinetic results are compared favorably with the extended empirical results of other authors. For the supersonic cases it is shown that the subsonic velocity downstream of the sampling probe bow shock can be used in estimating the sampling error.     

Characterization of Several Integrative Sampling Methods for Nitric Acid,Sulphur Dioxide and Atmospheric Particles

Laboratory and field experiments were performed to evaluate integrative measurement methods for atmospheric nitrates, sulphate and sulphur dioxide. Denuder tubes and several filter media were tested under laboratory and field conditions. Effects of sampling variables such as temperature and relative humidity, flow rates, concentration, loading capacity and artifacts due to NO, NO₂ and SO₂ were also evaluated. The integrative filter sampling method and the ion chromatographic analytical procedure gave a measurement precision (relative standard deviation) of ±11.5 percent for particulate NO₃ ^? on Teflon and ±15.6 percent for gaseous HNO₃ on nylon; for both these constituents, the detection limit was about 0.1 μ m^?3.     

Effects of Wind Direction on Coarse and Fine Particulate Matter Concentrations in Southeast Kansas

Abstract

Field data for coarse particulate matter ([PM] PM₁₀) and fine particulate matter (PM_2.5) were collected at selected sites in Southeast Kansas from March 1999 to October 2000, using portable MiniVol particulate samplers. The purpose was to assess the influence on air quality of four industrial facilities that burn hazardous waste in the area located in the communities of Chanute, Independence, Fredonia, and Coffeyville. Both spatial and temporal variation were observed in the data. Variation because of sampling site was found to be statistically significant for PM₁₀ but not for PM_2.5. PM₁₀ concentrations were typically slightly higher at sites located within the four study communities than at background sites. Sampling sites were located north and south of the four targeted sources to provide upwind and downwind monitoring pairs. No statistically significant differences were found between upwind and downwind samples for either PM₁₀ or PM_2.5, indicating that the targeted sources did not contribute significantly to PM concentrations. Wind direction can frequently contribute to temporal variation in air pollutant concentrations and was investigated in this study. Sampling days were divided into four classifications: predominantly south winds, predominantly north winds, calm/variable winds, and winds from other directions. The effect of wind direction was found to be statistically significant for both PM₁₀ and PM_2.5. For both size ranges, PM concentrations were typically highest on days with predominantly south winds; days with calm/variable winds generally produced higher concentrations than did those with predominantly north winds or those with winds from “other” directions. The significant effect of wind direction suggests that regional sources may exert a large influence on PM concentrations in the area.     

Kinetic Sequential Sampling (KSS) System: An Automated Sampling System for Measuring Vertical Concentration Profiles of Airborne Particles

ABSTRACT

An electronically controlled lift system carrying a realtime particle monitor has been developed for sampling air sequentially, at different heights within the breathing zone. Data are automatically logged at the different receptor levels, for the determination of average vertical concentration profiles of airborne particulate matter. The system is easy to operate, portable, and easily extended to different heights or modified for use with other types of monitors (e.g., a portable CO analyzer). For measuring airborne particle concentrations, a Grimm Dust Monitor 1.104/5 was used. The results of trial runs, which were carried out indoors and in a relatively open semi-rural area, are presented, and applications of the kinetic sequential sampling (KSS) system are discussed.     

Chemical Composition of Fine Particles in the Tennessee Valley Region

ABSTRACT

Fine particles in the atmosphere have elicited new national ambient air quality standards (NAAQS) because of their potential role in health effects and visibility-reducing haze. Since April 1997, Tennessee Valley Authority (TVA) has measured fine particles (PM_2.5) in the Tennessee Valley region using prototype Federal Reference Method (FRM) samplers, and results indicate that the new NAAQS annual standard will be difficult to meet in this region. The composition of many of these fine particle samples has been determined using analytical methods for elements, soluble ions, and organic and elemental carbon. The results indicate that about one-third of the measured mass is SO₄ ^-2, one-third is organic aerosol, and the remainder is other materials. The fraction of SO₄ ^-2 is highest at rural sites and during summer conditions, with greater proportions of organic aerosol in urban areas throughout the year. Additional measurements of fine particle mass and composition have been made to obtain the short-term variability of fine mass as it pertains to human exposure. Measurements to account for semi-volatile constituents of fine mass (nitrates, semi-volatile organics) indicate that the FRM may significantly under-measure organic constituents. The potentially controllable anthropogenic fraction of organic aerosols is still largely unknown.     

Hot Filter/Impinger and Dilution Sampling for Fine Particulate Matter Characterization from Ferrous Metal Casting Processes

Abstract

A study using two stack-sampling methodologies for collecting particulate matter (PM) emissions was conducted using a hot filter followed by a cold impinger sampling train and a dilution sampler. Samples were collected from ferrous iron metal casting processes that included pouring molten iron into a sand mold containing an organic binder, metal cooling, removal of the sand from the cooled casting (shakeout), and postshakeout cooling. The shakeout process contributed more to PM emissions than the metal pouring and cooling processes. Particulate matter less than 2.5 μm in aerodynamic diameter (PM_2.5) mass emissions for the entire casting cycle ranged from 3.4 to 4.7 lb/t of metal for the hot filter/impinger method and from 0.8 to 1.8 lb/t of metal for the dilution method. Most of the difference was due to PM captured by the impingers, much of which was probably dissolved gases rather than condensable vapors. Of the PM fraction captured by the impingers, 96–98% was organic in nature. The impinger PM fraction contributed 32–38% to the total suspended particle mass and caused a factor of 2–4 positive bias for PM_2.5 emissions. For the pouring and cooling processes only, the factor increased to over seven times.     

Calculation of the Charging Rate of Fine Particles by Unipolar Ions

Theories of particle charging based on boundary value solutions to the diffysional equation may not be applicable to electrostatic precipitators where the ion density is rarely more than an order of magnitude greafer than the particle concentration. A new charging equation, based on kinetic theory, is presented which evaluates the charging rate in terms of the probability of collisions between the flust particles and ions. In the presence of an external electric field, the surface of the particle is divided into three charging regions, and separate charging rates are calculated for each region. The total charging rate is the sum of these three individual rates. For large particles and high electric fields, this theory predicts essentially the same charging rate as the classical field charging equation of Rohmann and Pauthenier. For low electric fields, the theory reduces to White’s diffusional charging equation. Agreement is within 25% of Hewitt’s experimental results over the entire range of variables where data are available. For practical charging times, agreement is within 15%.     

Radiation Charging: A Novel Way to Charge Fine Particles Electrically

The purpose of this paper is to describe a scheme to electrically charge fine particles using electric and magnetic fields in conjunction with ionizing radiation. Once charged, particulate matter can be removed from the air stream by directly applying a transverse electric field. In addition, since electrostatic forces can assist filtration and wet collection systems, it may be possible to design new and improved filtration and wet scrubber systems using radiation charging. The objectives of this paper are: (1) to present expressions that predict the charge acquired by particles and (2) to present the results of preliminary experiments.     

Measurement of Fine Particles in Diesel Emissions Using a Real-Time Aerosol Monitor

Abstract

A real-time monitoring methodology to determine diesel fine particles in diesel emissions has been evaluated. The range of particle size captured by the monitor was ～0.1 μm to 1 μm. DustTrak real-time monitors were connected to the dilution tunnel of the vehicle exhaust to measure the emissions during the vehicle tests under both dynamic and steady-state driving conditions, and concentration data were recorded every 5 sec. Test variation of the real-time monitoring among different test days was similar to that measured by traditional filter-based gravi-metric method, whereas the repeatability of the monitor data within the same-day tests was better than that of gravimetric method. Correlations between the two methods were established for different fuels tested on a single light duty vehicle. When the emissions from the reference fuel was used to convert the monitor’s response to diesel fuels, the levels determined by the real-time monitor were consistent with those measured by gravimetric method among different fuels tested. Use of the real-time monitor could provide information on the levels of fine particles that is more relevant to the public health than the total particles.     

Indoor Fine Particles: The Role of Terpene Emissions from Consumer Products

Abstract

Consumer products can emit significant quantities of terpenes, which can react with ozone (O₃). Resulting byproducts include compounds with low vapor pressures that contribute to the growth of secondary organic aerosols (SOAs). The focus of this study was to evaluate the potential for SOA growth, in the presence of O₃, following the use of a lime-scented liquid air freshener, a pine-scented solid air freshener, a lemon-scented general-purpose cleaner, a wood floor cleaner, and a perfume. Two chamber experiments were performed for each of these five terpene-containing agents, one at an elevated O₃ concentration and the other at a lower O₃ concentration. Particle number and mass concentrations increased and O₃ concentrations decreased during each experiment. Experiments with terpene-based air fresheners produced the highest increases in particle number and mass concentrations. The results of this study clearly demonstrate that homogeneous reactions between O₃ and terpenes from various consumer products can lead to increases in fine particle mass concentrations when these products are used indoors. Particle increases can occur during periods of elevated outdoor O₃ concentrations or indoor O₃ generation, coupled with elevated terpene releases. Human exposure to fine particles can be reduced by minimizing indoor terpene concentrations or O₃ concentrations.     

Development and Evaluation of an Impactor for a PM2.5 Speciation Sampler

ABSTRACT

A conventional impactor for a particle speciation sampler was developed and validated through laboratory and field tests. The speciation sampler consists of the following components: a PM_2.5 conventional impactor that removes particles larger than 2.5 μm, an all-glass, coated honeycomb diffusion denuder, and a 47-mm filter pack. The speciation sampler can operate at two different sampling rates: 10 and 16.7 L/min. An experimental characterization of the impactor’s performance was conducted. The impactor’s collection efficiency was examined as a function of critical design parameters such as Reynolds number, the distance from the nozzle exit to the impac-tion plate, and the impaction substrate coating method. The bounce of particles larger than the cut point was successfully minimized by using a greased surface as the im-paction substrate. Additionally, a series of field intercomparison experiments were conducted at both 10 and 16.7 L/min airflow. PM_2.5 mass and SO₄ ^2- concentrations were measured and compared with the Federal Reference Method (FRM) and found to be in good agreement. Results of the laboratory chamber tests also indicated that the impactor’s performance was in good agreement with the FRM.     

PADRE: A Computerized Data Reduction System for Cascade Impactor Measurements

An interactive computer resource for analyzing, evaluating, and archiving particle size distributions as determined by cascade impactors for environmental measurement is decribed. The Particle Data Reduction (PADRE) computer program assists users in obtaining high quality size-mass distribution data for archival in the Fine Particle Emissions Information System (FPEIS). PADRE users interactively store, edit, reduce, and analyze observed impactor data from anywhere in the continential United States. Extensive data quality checks and computer- prompted, user-directed program operations assist users in obtaining meaningful information within minutes of entering impactor data. Design goals, program operation, sample sessions and plans for future system development are discussed.     

Design and Calibration of A High Volume Cascade Impactor

The purpose of this study was to develop an air sampling device capable of classifying large quantities of airborne particulate matter into discrete size fractions. Such frac-tionation will facilitate chemical analysis of the various particulate pollutants and thereby provide a more realistic assessment of the effects of particulate matter on human beings.

A 30 cfm, 5 stage cascade impactor of the slit-type has been constructed and calibrated. The calibration aerosol consisted of six different sizes of monodispersed methylene blue produced with a spinning disc generator. The test aerosol sizes varied from 1.35 to 14 μm. The calibration was challenged with heterodispersed aerosols of methylene blue, Arizona road dust, and DOP.     

The Southeastern Aerosol Research and Characterization Study: Part II. Filter-Based Measurements of Fine and Coarse Particulate Matter Mass and Composition

Abstract

The Southeastern Aerosol Research and Characterization Study (SEARCH) was implemented in 1998–1999 to provide data and analyses for the investigation of the sources, chemical speciation, and long-term trends of fine particulate matter (PM_2.5) and coarse particulate matter (PM_10–2.5) in the Southeastern United States. This work is an initial analysis of 5 years (1999–2003) of filter-based PM_2.5 and PM_10–2.5 data from SEARCH. We find that annual PM_2.5 design values were consistently above the National Ambient Air Quality Standards (NAAQS) 15 µg/m³ annual standard only at monitoring sites in the two largest urban areas (Atlanta, GA, and North Birmingham, AL). Other sites in the network had annual design values below the standard, and no site had daily design values above the NAAQS 65 µg/m³ daily standard. Using a particle composition monitor designed specifically for SEARCH, we found that volatilization losses of nitrate, ammonium, and organic carbon must be accounted for to accurately characterize atmospheric particulate matter. In particular, the federal reference method for PM_2.5 underestimates mass by 3–7% as a result of these volatilization losses. Organic matter (OM) and sulfate account for ≥60% of PM_2.5 mass at SEARCH sites, whereas major metal oxides (MMO) and unidentified components (“other”) account for ≥80% of PM_10–2.5 mass. Limited data suggest that much of the unidentified mass in PM_10–2.5 may be OM. For paired comparisons of urban-rural sites, differences in PM_2.5 mass are explained, in large part, by higher OM and black carbon at the urban site. For PM₁₀, higher urban concentrations are explained by higher MMO and “other.” Annual means for PM_2.5 and PM_10–2.5 mass and major components demonstrate substantial declines at all of the SEARCH sites over the 1999–2003 period (10–20% in the case of PM_2.5, dominated by 14–20% declines in sulfate and 11–26% declines in OM, and 14–25% in the case of PM_10–2.5, dominated by 17–30% declines in MMO and 14–31% declines in “ other”). Although declining national emissions of sulfur dioxide and anthropogenic carbon may account for a portion of the observed declines, additional investigation will be necessary to establish a quantitative assessment, especially regarding trends in local and regional emissions, primary carbon emissions, and meteorology.     

Toxicity of Chemical Components of Fine Particles Inhaled by Aged Rats: Effects of Concentration

Abstract

This study tested the hypothesis that exposure to mixtures containing fine particles and ozone (O₃) would cause pulmonary injury and decrements in functions of immunological cells in exposed rats (22–24 months old) in a dose-dependent manner. Rats were exposed to high and low concentrations of ammonium bisulfate and elemental carbon and to 0.2 ppm O₃. Control groups were exposed to purified air or O₃ alone. The biological end points measured included histopathological markers of lung injury, bronchoalveolar lung fluid proteins, and measures of the function of the lung’s innate immuno-logical defenses (macrophage antigen-directed phagocytosis and respiratory burst activity). Exposure to O₃ alone at 0.2 ppm did not result in significant changes in any of the measured end points. Exposures to the particle mixtures plus O₃ produced statistically significant changes consistent with adverse effects. The low-concentration mixture produced effects that were statistically significant compared to purified air but, with the exception of macrophage Fc receptor binding, exposure to the high-concentration mixture did not. The effects of the low- and high-concentration mixtures were not significantly different. The study supports previous work that indicated that particle + O₃ mixtures were more toxic than O₃ alone.