Real Time Measurement of the Size Distribution Of Particulate Matter by a Light Scattering Method

The body of information presented in this paper is directed to those individuals concerned with the measurement of the size distribution of particulate matter in air. The light scattering instrument described herein is characterized by the fact that it can accurately size particles almost independently of their index of refraction. The basic concept involves the simultaneous measurement of the intensity of light scattered by a single particle at two small scattering angles. The ratio of the two intensities is directly related io ine size of ihe pariicle, and for scattering angles of 5° and 10° the effective range of the instrument is 0.2 to 4 μm. The air flows through the optical system at such a rate that approximately 25 μs are required to determine the size of each particle, and concentrations as high as 10⁴ particles/cc can be measured without dilution and without serious coincidence effects. By employing a multichannel analyzer as the data storage and readout device it is possible to detect changes in particulate size distribution within a few seconds. Calibration of the instrument has been performed using polystyrene latex spheres and materials having a wide range of index of refraction and shape including carbon black, iron oxide and spores.     

Electrical Measurement of the Mass Concentration of a Self-Preserving Aerosol Size Distribution

Recently fifty-eight measurements of urban aerosol size distributions by Clark have shown that these distributions agree quite well with the self preserving form proposed by Friedlander within the size range of 0.05 to 5 microns radius. This paper shows that for an aerosol obeying the self preserving distribution model, the volume concentration (and, hence, the mass concentration for constant density) is directly proportional to the electric current collected when the aerosol is unipolarly charged, passed through a weak electric field to remove particles smaller than 0.05 micron and then collected by a current collector. It is shown that the linear relation between the mass concentration and collected current is independent of the unipolar charging method used. A test of this theory using Clark’s electric counter data was encouraging and suggests that the electric measurement of urban aerosol mass concentrations by properly designed instruments may be feasible.     

Evaluation of the RAMS Continuous Monitor for Determination of PM2.5 Mass Including Semi-Volatile Material in Philadelphia,PA

Abstract

The real-time ambient mass sampler (RAMS) is a continuous monitor based on particle concentrator, denuder, drier, and tapered element oscillating microbalance (TEOM) monitor technology. It is designed to measure PM_2.5 mass, including the semi-volatile species NH₄NO₃ and semi-volatile organic material, but not to measure PM_2.5 water content. The performance of the RAMS in an urban environment with high humidity was evaluated during the July 1999 NARSTO-Northeast Oxidant and Particles Study (NEOPS) intensive study at the Baxter water treatment plant in Philadelphia, PA. The results obtained with the RAMS were compared to mass measurements made with a TEOM monitor and to constructed mass obtained with a Particle Concentrator-Brigham Young University Organic Sampling System (PC-BOSS) sampler designed to determine the chemical composition of fine particles, including the semi-volatile species. An average of 28% of the fine particulate material present during the study was semi-volatile organic material lost from a filter during particle collection, and 1% was NH₄NO₃ that was also lost from the particles during sampling. The remaining mass was dominantly nonvolatile (NH₄)₂SO₄ (31%) and organic material (37%), with minor amounts of soot, crustal material, and nonvolatile NH₄NO₃. Comparison of the RAMS and PC-BOSS results indicated that the RAMS correctly monitored for fine particulate mass, including the semi-volatile material. In contrast, the heated filter of the TEOM monitor did not measure the semi-volatile material. The comparison of the RAMS and PC-BOSS data had a precision of ±4.1 μg/m³ (±9.6%). The precision of the RAMS data was limited by the uncertainty in the blank correction for the reversible adsorption of water by the charcoal-impregnated cellulose sorbent filter of the RAMS monitor. The precision of the measurement of fine par-ticulate components by the PC-BOSS was ±6-8%.     

Modifications to the Sunset Laboratory Carbon Aerosol Monitor for the Simultaneous Measurement of PM2.5 Nonvolatile and Semi-Volatile Carbonaceous Material

Abstract

Semi-volatile organic carbonaceous material (SVOC) in fine particles is not reliably measured with conventional semicontinuous carbon monitors because semi-volatile carbonaceous material is lost from the collection media during sample collection. Two modifications of a Sunset Laboratory carbon aerosol monitor allowing for the determination of semi-volatile fine particulate organic material are described. Collocated conventional and modified instruments were operated simultaneously using a common inlet. Comparisons were made with integrated PC-BOSS data for quartz filter retained nonvolatile organic carbon (NVOC) and elemental carbon (EC), SVOC, and total carbon (TC = SVOC + NVOC + EC) and good agreement was observed between TC concentrations during studies conducted in Rubidoux, CA. Precision of the comparison was σ=±1.5 μg-C/m³ (±8%). On the basis of experiments performed with the modified Sunset monitor, a dual-oven Sunset monitor was developed and extensively tested in Lindon, UT; Riverside, CA; and in environmental exposure chambers. The precision for the measurement of TC with the dual-oven instrument was σ = ±1.4 μg-C/m³ (±13%).     

The Southeastern Aerosol Research and Characterization Study,Part 3: Continuous Measurements of Fine Particulate Matter Mass and Composition

Abstract

Deployment of continuous analyzers in the Southeastern Aerosol Research and Characterization Study (SEARCH) network began in 1998 and continues today as new technologies are developed. Measurement of fine particulate matter (PM_2.5) mass is performed using a dried, 30 °C tapered element oscillating microbalance (TEOM). TEOM measurements are complemented by observations of light scattering by nephelometry. Measurements of major constituents include: (1) SO₄ ^2? via reduction to SO₂; (2) NH₄ ⁺ and NO₃ ^? via respective catalytic oxidation and reduction to NO, (3) black carbon (BC) by optical absorption, (4) total carbon by combustion to CO₂, and (5) organic carbon by difference between the latter two measurements. Several illustrative examples of continuous data from the SEARCH network are presented. A distinctive composite annual average diurnal pattern is observed for PM_2.5 mass, nitrate, and BC, likely indicating the influence of traffic-related emissions, growth, and break up of the boundary layer and formation of ammonium nitrate. Examination of PM_2.5 components indicates the need to better understand the continuous composition of the unmeasured “other” category, because it contributes a significant fraction to total mass during periods of high PM_2.5 loading. Selected episodes are presented to illustrate applications of SEARCH data. An SO₂ conversion rate of 0.2%/hr is derived from an observation of a plume from a coal-fired power plant during early spring, and the importance of local, rural sources of NH₃ to the formation of ammonium nitrate in particulate matter (PM) is demonstrated.     

The Correlation between Light Scattering and Mass Concentration of Tobacco Smoke

Reports by others^1,2 have pointed to tobacco smoke as a significant source of air pollution in indoor spaces. Studies by Charlson, et al., ³ Kretzschmar,⁴ and Eccleston, et al. ⁵ have yielded mass concentration-light scattering correlations for several natural aerosols. This note presents a value for the mass concentration/ light scattering ratio for tobacco smoke. This ratio provides a means of assessing air quality in indoor spaces using an instrument with a fairly short (?1 min) time constant.     

Determination of PM2.5 Sulfate and Nitrate with a PC-BOSS Designed for Routine Sampling for Semi-Volatile Particulate Matter

ABSTRACT

Ambient particles contain substantial quantities of material that can be lost from the particles during sample collection on a filter. These include ammonium nitrate and semi-volatile organic compounds. As a result, the concentrations of these species are often significantly in error for results obtained with a filter pack sampler. The accurate measurement of these semi-volatile fine particulate species is essential for a complete understanding of the possible causes of health effects associated with exposure to fine particles. Past organic compound diffusion denuder samplers developed by the authors (e.g., the Brigham Young University Organic Sampling System [BOSS]) are not amenable to routine field use because of the need to independently determine the gas-phase semi-volatile organic material efficiency of the denuder for each sample. This problem has been eliminated using a combined virtual impactor, particle-concentrator inlet to provide a concentrated stream of 0.1-2.5-μm particles. This is followed by a BOSS diffusion denuder and filter packs to collect particles, including any semi-volatile species lost from the particles during sampling. The samp ler (Particle Concentrator-Brigham Young University Organic Sampling System [PC-BOSS]) contains a post-denuder multifilter pack unit to allow for the routine collection of several sequential samples. The PC-BOSS can be used for the determination of both fine particulate nitrate and semi-volatile organic material without significant “positive” or “negative” sampling artifacts. Validation of the sampler for the determination of PM_2.5 sulfate and nitrate based on comparison of results obtained at Riverside, CA with collocated PC-BOSS, annular denuder, and Chem Spec samplers indicates the PC-BOSS gives accurate results for these species with a precision of ±5-8%. An average of 33% of the PM_2.5 nitrate was lost from the particles during sampling for both denuder and single filter samplers.     

Size Distribution and Sources of Aerosol in Launceston,Australia, during Winter 1997

ABSTRACT

As part of a pilot study into the chemical and physical properties of Australian fine particles, a suite of aerosol samples was collected at Ti Tree Bend in Launceston, Tasmania, during June and July 1997. This period represents midwinter in the Southern Hemisphere, a period when aerosol sources in Launceston are dominated by smoke from domestic wood burning. This paper describes the results from this measurement campaign, with the aim of assessing the effect of wood smoke on the chemical and physical characteristics of ambient aerosol. A micro orifice uniform deposit impactor (MOUDI) was used to measure the size distributions of the aerosol from 0.05 to 20 n m aerodynamic diameter. Continuous measurements of fine particle mass were made using a PM_2.5 tapered element oscillating microbalance (TEOM) and light scattering coefficients at 530 nm were measured with nephelometers.

Mass size distributions tended to be bimodal, with the diameter of the dominant mode tending to smaller sizes with increases in total mass. Non-sea salt potassium and polycyclic aromatic hydrocarbons (PAHs) were used as chemical tracers for wood smoke. Wood smoke was found to increase absolute particle mass (enough to regularly exceed air quality standards), and to concentrate mass in a single mode below 1 μm aerodynamic diameter. The acid-base equilibrium of the aerosol was altered by the wood smoke source, with free acidity hydrogen ion, non-sea salt sulfate, and ammonium concentrations being higher and the concentration of all species, including nitrate (to differing extents), focused in the fine particle size ranges. The wood smoke source also heavily influenced the aerosol scattering efficiency, adding to a strong diurnal cycle in both mass concentration and light scattering.     

Analysis and Simulation of Wintertime Light Scattering by the Urban Aerosol in Dallas-Fort Worth

ABSTRACT

Wintertime atmospheric light scattering in Dallas, TX, was estimated through the use of aerosol models. Input data for the aerosol models were provided by measurements of aerosol chemistry, physical particle size distributions, and distributions of particulate sulfur by particle size, and by predictions by an atmospheric simulation model. Light scattering measurements provided a basis for testing the aerosol models. The SCAPE thermodynamic equilibrium model was used to estimate the amount of liquid water associated with particles and the ELSIE Mie scattering model was applied to estimate the resulting light scattering. The calculations were based on aerosol properties measured in Dallas during December 1994 and February 1995, and changes in scattering due to hypothetical changes in the aerosol were predicted. The predicted light scattering was compared to scattering measured by an Optec nephelom-eter; agreement was within 20% in every case.     

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.     

Effect of the Fine Fraction of Particulate Matter versus the Coarse Mass and Other Pollutants on Daily Mortality in Santiago,Chile

ABSTRACT

Daily counts of non-accidental deaths in Santiago, Chile, from 1988 to 1996 were regressed on six air pollutants— fine particles (PM_2.5), coarse particles (PM_10–2.5), CO, SO₂, NO₂, and O₃. Controlling for seasonal and meteorological conditions was done using three different models— a generalized linear model, a generalized additive model, and a generalized additive model on previously filtered data. Single- and two-pollutant models were tested for lags of 1-5 days and the average of the previous 2-5 days.

The increase in mortality associated with the mean levels of air pollution varied from 4 to 11%, depending on the pollutants and the way season of the year was considered. The results were not sensitive to the modeling approaches, but different effects for warmer and colder months were found. Fine particles were more important than coarse particles in the whole year and in winter, but not in summer. NO₂ and CO were also significantly associated with daily mortality, as was O₃ in the warmer months. No consistent effect was observed for SO₂. Given particle composition in Santiago, these results suggest that combustion-generated pollutants, especially from motor vehicles, may be associated with increased mortality. Temperature was closely associated with mortality. High temperatures led to deaths on the same day, while low temperatures lead to deaths from 1 to 4 days later.     

Relating Summer Ambient Particulate Sulfur,Sulfur Dioxide,and Light Scattering to Gaseous Tracer Emissions from the MOHAVE Power Project

ABSTRACT

Project MOHAVE was initiated in 1992 to examine the role of emissions from the 1580 MW coal-fired MOHAVE Power Project (MPP) on haze at the Grand Canyon National Park (GCNP), located about 130 km north-northeast of the power plant. Statistical relationships were analyzed between summertime ambient concentrations of a gaseous perfluorocarbon tracer released from MPP and ambient SO₂, particulate sulfur, and light scattering to evaluate whether MPP's emissions could be transported to the GCNP and then impact haze levels there. Spatial analyses indicated that particulate sulfur levels were strongly correlated across the monitoring network, regardless of whether the monitoring stations were upwind or downwind of MPP. This indicates that particulate sulfur levels in this region were influenced by distant regional emission sources. A significant particulate sulfur contribution from a point source such as MPP would result in a non-uniform pattern downwind. There was no suggestion of this in the data.

Furthermore, correlations between the MPP tracer and ambient particulate sulfur and light scattering at locations in the park were virtually zero for averaging times ranging from 24 hr to 1 hr. Hour-by-hour MPP tracer levels and light scattering were individually examined, and still no positive correlations were detected. Finally, agreement between tracer and particulate sulfur did not improve as a function of meteorological regime, implying that, even during cloudy monsoon days when more rapid conversion of SO₂ to par-ticulate sulfur would be expected, there was no evidence for downwind particulate sulfur impacts. Despite the fact that MPP was a large source of SO₂ and tracer, neither time series nor correlation analyses were able to detect any meaningful relationship between MPP's SO₂ and tracer emission “signals” to particulate sulfur or light scattering.     

An Aerosol Sampler for Determination of Particle Concentration as a Function of Size and Time

A high flow rate four-stage impacfor was developed for the determination of aerosol concentration as a function of both particle size and time. The unit is very useful for long-term sampling intervals (24 hr) and for sampling very dusty atmospheres. Gas-borne particulate matter is collected out on four rotating drums, each with a collection surface area of about 10 sq in.; this allows a large quantity of materials to be collected without danger of particle build-up and blow-off. A particle size-collection efficiency calibration for the unit is presented together with experimental data on wall losses, surface coatings, and other important operational considerations.     

The 1999 Fresno Particulate Matter Exposure Studies: Comparison of Community,Outdoor, and Residential PM Mass Measurements

ABSTRACT

Two collaborative studies have been conducted by the U.S. Environmental Protection Agency (EPA) National Exposure Research Laboratory (NERL) and National Health and Environmental Effects Research Laboratory to determine personal exposures and physiological responses to par-ticulate matter (PM) of elderly persons living in a retirement facility in Fresno, CA. Measurements of PM and other criteria air pollutants were made inside selected individual residences within the retirement facility and at a central outdoor site on the premises. In addition, personal PM exposure monitoring was conducted for a subset of the participants, and ambient PM monitoring data were available for comparison from the NERL PM research monitoring platform in central Fresno. Both a winter (February 1-28, 1999) and a spring (April 19-May 16, 1999) study were completed so that seasonal effects could be     

Measurement, Collaborative Learning and Research for Sustainable Use of Ecosystem Services: Landscape Concepts and Europe as Laboratory

Policies at multiple levels pronounce the need to encompass both social and ecological systems in governance and management of natural capital in terms of resources and ecosystems. One approach to knowledge production and learning about landscapes as social–ecological systems is to compare multiple case studies consisting of large spaces and places. We first review the landscape concepts’ biophysical, anthropogenic, and intangible dimensions. Second, we exemplify how the different landscape concepts can be used to derive measurable variables for different sustainability indicators. Third, we review gradients in the three dimensions of the term landscape on the European continent, and propose to use them for the stratification of multiple case studies of social–ecological systems. We stress the benefits of the landscape concepts to measure sustainability, and how this can improve collaborative learning about development toward sustainability in social–ecological systems. Finally, analyses of multiple landscapes improve the understanding of context for governance and management.     

Aerosol chemical composition and light scattering in Portland,Oregon: The role of carbon

Measurements of light scattering and the chemical composition of the fine aerosol from the Portland (Oregon) Aerosol Characterization Study (PACS) of 1977–1978 are reported. Scattering coefficients for sulfate, nitrate, carbonaceous aerosol and residual mass were determined by stepwise multiple linear regression. Unlike other cities the scattering efficiencies for sulfate, nitrate and carbonaceous aerosol were approximately the same. Carbonaceous aerosol was found to account for about 50% of both the fine aerosol mass and the light scattering.     

A Comparison of the Size Distribution of Particulates Emitted from Air,Mechanical, and Steam Atomized Oil Fired Burners

Particulate size distributions were obtained in the effluent gases from three steam generating boilers of a power station employing mechanical, steam, and air systems for heavy fuel atomization. Samples were obtained with an eight-stage cascade impactor. The air atomized burner produced the lowest particulate loading, the greatest percentage of particulates by weight in the submicron range, and particulates with the lowest combustible content.     

The Southeastern Aerosol Research and Characterization Study, part 3: continuous measurements of fine particulate matter mass and composition

Deployment of continuous analyzers in the Southeastern Aerosol Research and Characterization Study (SEARCH) network began in 1998 and continues today as new technologies are developed. Measurement of fine particulate matter (PM2.5) mass is performed using a dried, 30 degrees C tapered element oscillating microbalance (TEOM). TEOM measurements are complemented by observations of light scattering by nephelometry. Measurements of major constituents include: (1) SO4(2-) via reduction to SO2; (2) NH4+ and NO3- via respective catalytic oxidation and reduction to NO, (3) black carbon (BC) by optical absorption, (4) total carbon by combustion to CO2, and (5) organic carbon by difference between the latter two measurements. Several illustrative examples of continuous data from the SEARCH network are presented. A distinctive composite annual average diurnal pattern is observed for PM2.5 mass, nitrate, and BC, likely indicating the influence of traffic-related emissions, growth, and break up of the boundary layer and formation of ammonium nitrate. Examination of PM2.5 components indicates the need to better understand the continuous composition of the unmeasured "other" category, because it contributes a significant fraction to total mass during periods of high PM2.5 loading. Selected episodes are presented to illustrate applications of SEARCH data. An SO2 conversion rate of 0.2%/hr is derived from an observation of a plume from a coal-fired power plant during early spring, and the importance of local, rural sources of NH3 to the formation of ammonium nitrate in particulate matter (PM) is demonstrated.     

The Relation between Moderate Resolution Imaging Spectroradiometer (MODIS) Aerosol Optical Depth and PM2.5 over the United States: A Geographical Comparison by U.S. Environmental Protection Agency Regions

Abstract

Aerosol optical depth (AOD) acquired from satellite measurements demonstrates good correlation with particulate matter with diameters less than 2.5 µm (PM_2.5) in some regions of the United States and has been used for monitoring and nowcasting air quality over the United States. This work investigates the relation between Moderate Resolution Imaging Spectroradiometer (MODIS) AOD and PM_2.5 over the 10 U.S. Environmental Protection Agency (EPA)-defined geographic regions in the United States on the basis of a 2-yr (2005–2006) match-up dataset of MODIS AOD and hourly PM_2.5 measurements. The AOD retrievals demonstrate a geographical and seasonal variation in their relation with PM_2.5. Good correlations are mostly observed over the eastern United States in summer and fall. The southeastern United States has the highest correlation coefficients at more than 0.6. The southwestern United States has the lowest correlation coefficient of approximately 0.2. The seasonal regression relations derived for each region are used to estimate the PM_2.5 from AOD retrievals, and it is shown that the estimation using this method is more accurate than that using a fixed ratio between PM_2.5 and AOD. Two versions of AOD from Terra (v4.0.1 and v5.2.6) are also compared in terms of the inversion methods and screening algorithms. The v5.2.6 AOD retrievals demonstrate better correlation with PM_2.5 than v4.0.1 retrievals, but they have much less coverage because of the differences in the cloud-screening algorithm.