Fuel Processing Technology 6566 2000. 379392 www.elsevier.

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An overview of PM 2.5 sources and control strategies

W. Gene Tucker
) National Risk Management Research Laboratory, U.S. Enironmental Protection Agency, Research Triangle Park, NC 27711 USA Received 22 February 1999; accepted 30 June 1999

Abstract The new national ambient air quality standard for particulate matter is summarized, with emphasis on fine particles, or particulate matter with aerodynamic diameter less than 2.5 mm PM 2.5 .. Sources of ambient and indoor PM 2.5 are summarized, followed by an overview of control strategies for both primary directly emitted. particles and gaseous precursors of ambient particles. The role of future findings on the health effects of particles of different sizes or compositions is noted, as is the potential importance of controlling indoor exposures for susceptible people. EPA risk management research on sources and control options is summarized. The cost-effectiveness of prevention and control technologies for PM 2.5 has not been well researched and documented. Optimum control strategies will likely include a variety of control options. Published by Elsevier Science B.V.
Keywords: Ambient PM; Indoor PM; Control strategies; Prevention

1. Introduction Because epidemiological associations had been found at particle concentrations below the existing national ambient air quality standard, a new national standard was promulgated in July 1997 w27x. Whereas the former standard applied to particulate matter less than 10 mm in aerodynamic diameter PM 10 ., the new standard also addresses particles smaller than 2.5 mm PM 2.5 .. The new standard, like the old one, considers only size

College of Integrated Science and Technology, James Madison University, MSC 4102, Harrisonburg, VA 22807, USA. Tel.: q 1-540-568-8771; fax: q 1-540-568-2761; e-mail: tuckerwg@jmu.edu 0378-3820r00r$ - see front matter Published by Elsevier Science B.V. PII: S 0 3 7 8 - 3 8 2 0 9 9 . 0 0 1 0 5 - 8

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and mass concentration; chemical composition and toxicity of the particles are not addressed. To meet the new standard, sources of both primary and secondary particles will need to be controlled. Control of primary particles, which are emitted directly into the air, involves emissions prevention or collection at the source. Control of secondary particles, which are formed in the atmosphere, requires reducing emissions of precursor constituents such as condensible organic compounds, sulfur oxides, nitrogen oxides, and ammonia. Fig. 1 shows a typical size distribution of particles in the ambient air, and how PM 10 and PM 2.5 relate to the total distribution. Particles are generally distributed bimodally by size in the atmosphere, with the minimum of the distribution between 1 and 3 mm aerodynamic diameter. Particles in the fine mode are created as primary particles at the source, mostly by combustion or other high-temperature processes, or as secondary particles in the atmosphere. Most of the mass of particles in the coarse mode comes from materials that have been ground down by mechanical processes, although fine-mode particles can also become attached w26x. Ambient PM is a complex mixture of sizes and types of particles that originate from many sources. The size, chemical composition, and source of particles may all play a role in human exposures, and health effects resulting from those exposures. Little information is available on the specific chemical makeup, especially the metal speciation and organic components of fine particles. Chemical characterization of PM from a broad

Fig. 1. PM 10 and PM 2.5 related to a typical size distribution for ambient particles adapted from USEPA w26x..

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range of locations with a variety of source types is needed to better determine the composition, range of transport, and variability of airborne particles. The types of sources that contribute to the two modes in the distribution shown in Fig. 1 are generally known. Particles in the fine mode include primary particles from high-temperature metallurgical and combustion processes, secondary particles from atmospheric reactions, and an unknown but theoretically small amount of fine particles that have been deposited and resuspended by wind or human activities. Particles in the coarse mode include coarse windblown and road dust, pollens and spores, and some industrial particles. PM 10 samples are generally dominated, on a mass basis, by coarse-mode particles. PM 2.5 samples can also have substantial amounts, on a mass basis, of coarse-mode particles from the left-hand tail of the coarse-mode distribution about 12.5 mm diameter.; this may be especially likely in areas with significant sources of resuspended dust. Since the epidemiological studies of PM health effects are based on geographically dispersed but mostly urban. locations with numerous and varied emission sources, the major sources of the particles are difficult to ascertain. Researchers most familiar with these studies have speculated that two types of sources may be particularly important: primary emissions from combustion sources, and secondary particles formed in the atmosphere. Table 1 lists the key causal factors that are the basis for current hypotheses on what aspects of particulate matter are responsible for observed health effects. Hypotheses regarding acidic particles, particles containing sulfates, ultrafine particles smaller than about 0.1 mm., and particles containing transition metals would implicate combustion sources. See Refs. w28,31x for recent reviews. There is a lot of uncertainty with respect to fugitive particles. Their emission rates are poorly quantified, but potentially large compared to emission rates of combustion and other industrial sources. Table 2 summarizes the U.S. national inventory for particle and gaseous precursor emissions from general categories of sources. Note that approximately 70% of the total primary PM 2.5 is from fugitive sources. This is presumably because the national total PM 10 emissions are so large, and the mass in the left-hand tail of the coarse mode see Fig. 1. is large compared to the mass of particles being created in the fine mode. Even though the estimates for PM 2.5 fugitive emissions are being reevaluated and may be revised downward somewhat, they will still constitute a large percentage of the national total. Emissions data summarized in Table 2 illustrate the large potential contribution of sulfur oxides wSO x principally sulfur dioxide SO 2 .x and nitrogen oxides wNO x
Table 1 Factors or constituents that are currently hypothesized to be significant in fine PM toxicity from Mauderly et al. w18x. PM mass concentration Particle sizersurface area Ultrafine PM Organic compounds Sulfate and nitrate salts Cofactors e.g., other pollutants, weather. Metals Acids Biogenic particles Peroxides Soot

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Table 2 Summary of U.S. national inventory of particle and precursor emissions Approximate national emissions 10 3 Mgryear. PM 2.5 Industrial processes Combustion sources Electric utility Industrial and commercial Residential Vehicular Managed burningqwildfires Fugitive sources Roads Agriculturalrsilvacultural crops Construction Natural sources Geogenic wind erosion. Biogenic from HC precursors. Rounded totals
a b a NO x

PM 10 1000 300 700 500 900 800 13,000 5000 4000 5000 unk b 30,000

SO x 1600 13,000 4000 10 700 10

500 100 500 500 700 700 2000 900 800 800 unk b 8000

900 6000 4000 900 12,000 200

20,000

20,000

As NO 2 nitrogen dioxide.; however, most NO x is emitted as NO. An unknown amount of natural hydrocarbon emissions e.g., terpenes. is photochemically converted to atmospheric aerosols. Adapted from USEPA w25x.

principally nitric oxide NO.x gaseous precursors to ambient PM concentrations. If their combined 40 million tonsryear were completely converted to sulfate and nitrate particles, their emissions would be equivalent to about 60 million tonsryear of primary PM 2.5 . However, ambient PM 2.5 in the U.S. is typically 3050% sulfate and much less nitrate, except in southern California where nitrate may be as much as 45% in some winter periods w26x. This implies a conversion to PM 2.5 of somewhat less than 10 million tonsryear, or somewhat less than 20% of the gaseous precursor emissions. Fig. 2 shows geographically the areas that do not meet the PM 10 standard of 150 mgrm3 24 h average. and 50 mgrm3 annual average.. It also indicates the source types that are thought to be the major causes of non-attainment with the standard. The number of additional areas of the country that will not meet the new PM 2.5 requirements, and the additional sources needing control, will be determined largely by analysis of concentration and composition data from the new network of ambient monitoring stations. There is further uncertainty about exposures to airborne particles inside buildings. Considering the high fraction of time that people especially those who may be most health-susceptible. spend indoors, there is a need to quantify the three major sources of indoor exposure: particles from outdoors, direct emissions from indoor sources, and resuspended particles from indoor activities a type of fugitive source.. Table 3 summarizes the various types of sources of particles found in buildings. Cigarette

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Fig. 2. Areas designated non-attainment for PM 10 particles, by emission type adapted from Bachmann et al. w2x..

smoking, cooking, and penetration of outdoor particles through the building envelope have all been reported to make significant contributions to indoor concentrations of fine particles, but a substantial portion is due to unexplained indoor sources w29x.

Table 3 Sources of exposure to indoor particles Outdoor origin Outdoor air through infiltration, ventilation. Tracked-in soil Carried-in dusts from industrial workplaces from other places Indoor origin Smoking, cooking Space heating especially kerosene, wood. Ventilation systems, humidifiers Office machines Dust mites, pets Diseased people bacteria, viruses. Personal activities e.g., hobbies. Maintenancerrenovation activities

Resuspension of particles of either outdoor or indoor origin Cleaning activities Maintenancerrenovation activities People movements

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2. The new national ambient air quality standard for PM 2.5 Concentration limits and the compliance timeline for the new national ambient air quality standard for PM 2.5 are shown in Table 4. Approximately 1500 monitoring stations are being set up across the United States in locations to reflect the population distribution rather than the distribution of major sources, which has been more of a factor in the past.. Compliance with the standard, often referred to as in attainment, will be determined by calculations using data from the monitoring stations. The calculations consider averaging over time and in some cases over more than one station in a geographic area, and allow exceedances of the standard for a certain amount of time see details in Ref. w27x.. Areas that are not in attainment will have to have plans, usually developed by States, that describe strategies to be used for bringing the areas into compliance. These plans, most often referred to as State Implementation Plans SIPs., are where actual PM 2.5 control strategies will be developed.

3. Control strategies for PM 2.5 The major categories of sources of PM 2.5 and gaseous precursors are listed in Table 5, with approximate annual emissions on a national basis. While any particular area that is in non-attainment status will have its own distribution of these sources, it is likely that control strategies will address one or more of these source types. Two general approaches will be taken to estimate which sources are contributing most to ambient monitoring stations in the non-attainment area: source inventories and source-oriented dispersion. modeling to estimate impacts on the ambient stations, and chemical characterization of particles collected at the ambient sites coupled with receptor-oriented modeling to calculate contributions of various source types.

Table 4 National ambient air quality standard for fine particulate matter PM 2.5 . Ambient concentration limits 24 h average Annual mean Timeline 1997 19982001 20012004 2002 20022005 20052008 20122017 65 mgrm3 15 mgrm3

New NAAQS for PM 2.5 National monitoring network set up Initial 3-year monitoring data sets available Periodic 5-year review of standard Areas designated attainment or non-attainment. States submit implementation plans States have up to 10 years to comply 12 years with extensions.

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In addition to these estimates of mass contributions, there may very well be some consideration of particle toxicity. By the time the implementation plans are being developed in the 20022008 time period, health researchers may have sufficient evidence to support one or more of the casual hypotheses for PM toxicity listed in Table 1. Such evidence may influence priorities on which sources to control, even before any changes are made in the ambient standard. When different source types contribute about equally to exceedances of the mass-based standard, sources of the most toxic particles may be given higher priority for control. Since many of the currently available estimates of PM 2.5 emissions are based on data on PM 10 rather than direct PM 2.5 measurements, there is great uncertainty in the fine particle emissions inventory. In addition, there is a general lack of data on the chemical composition of fine particle emissions. The need for emission characterization is greatest for sources with constituents such as metals and acidic components. that are candidates for causal mechanism studies of respiratory health effects, and for sources having the largest mass contributions to PM 2.5 in the environment. As Table 6 implies, there are few data on the effectiveness and costs of emissions prevention, emissions reduction, or exposure reduction technologies for fine particles i.e., PM 2.5 .. Reliable data on emission prevention for either industrial or indoor sources are nearly non-existent. Most of the available data on cost-effectiveness of emission controls are for industrial sources of total PM and at best, for PM 10 .. Although limited data are available on the efficiency and cost of air cleaning to remove particles from indoor air, there are virtually no data on the effectiveness of air cleaning in reducing indoor exposures to fine particles. Since indoor concentrations of particles approach outdoor concentrations when outdoor concentrations are high, or are about twice outdoor concentrations when outdoor concentrations are low e.g., Refs. w20,22x., and since people spend roughly an order of magnitude more time indoors than outdoors, it will be important to evaluate controls for indoor exposures.

4. EPA research related to PM 2.5 control strategies Research related to fine PM control strategies is being conducted by EPA in two areas: Source Characterization, where the focus is on new knowledge about the emission rates, chemical and physical compositions, and toxicities of particles from various sources; and Risk Management Ealuation, where the emphasis is on developing new information about the effectiveness and costs of prevention and control technologies for emissions of PM 2.5 . The overall objectives of the source characterization research are to 1. develop new or improved emission factors for sources of primary fine particles and ammonia, one of the gaseous precursors of secondary fine particles; 2. develop new information on the size distribution and composition of primary particles, to improve source profiles fingerprints. for source apportionment studies; and 3. chemically characterize and toxicologically test source particles, to improve understanding of mechanisms of PM toxicity and to obtain measures of health risk of various types of PM emissions. Current focus is on field and laboratory studies to develop improved emission factors for

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Table 5 Overview of current knowledge on U.S. emissions of fine particles Numbers in regular type are typical values, selected from the referenced literature; entries in italics are estimates or judgements by the author.. Source type Constituents of concern Total U.S. emission rate 10 3 Mgryear. PM 2.5 Roads
a,b,c

Approximate U.S. population in close proximity millions.

PM 10 18,000 250

Agricultural productiona,b,c including erosion. Construction activitiesa,b,c

Fine silica and other crustal elements plus reentrained carbon, asbestos, and metal compounds Fine silica and other crustal elements Fine silica and other crustal elements plus industrial reentrainment of carbon, asbestos, and metal compounds Products of uncontrolled combustion Polycyclic organic matter POM. Products of incomplete combustion, PM precursor NO x . Fine silica and other crustal elements Ar, Cr, Hg, Mn, Ni, Pb, Sb, Se, V, Cl, and PM precursors SO x , NO x . Cr, Fe, Ni, Pb, V, POM, Cl, PM precursors SO x , NO x .

3300

2000 1 1700 1

11,100 8500

Mostly in rural areas Mostly in urban areas

Open burning including wild-fires, agricultural burning. a,b,c Residential wood combustiona,b,c Diesel engine combustiona,b,c Mineral products productiona,b,c Pulverized coal boilersa,d

1130 1 550 450 100 Unknown

1320 ;600 500 200 160

Mostly in rural areas Mostly in rural and suburban areas Mostly in urban areas Near urban areas Utility: mostly rural Industrial: mostly near urban areas Mostly in urban areas

Heavy fuel oil combustiona,e

; 30

30

Residential fuel oil combustiona Waste incinerationa,f,g,h Metal smelting and refining a,i Automobiles j Outdoor air introduced into the indoor environment Tracked-in dust Indoor activities that generate or resuspend particles.

POM, PM precursor NO x . As, Be, Cr, Cd, Hg, Ni, Pb, PCDDrF, PCBs Cd, Cr, Pb, Zn, SO x V, carbon, organics, PM precursor NO x . Fine and coarse particles Pb, other heavy metals, pesticides Metals, pesticides, combustion aerosol organics

; 20 Unknown Unknown ; 20 Unknown Unknown Unknown

20 ; 45 400 ; 20 Unknown Unknown Unknown

Mostly in urban areas Mostly near urban areas Mostly in rural areas Mostly near urban areas 250 W.G. Tuckerr Fuel Processing Technology 6566 (2000) 379392 250 250

1 Estimates of fine particle emissions from these fugitive sources, although large compared to other sources in this table, are very uncertain and need to be confirmed. a Ref. w25x. b Ref. w6x. c Ref. w8x. d Refs. w1,3,7,1315,17,30x. e Refs. w4,5,9,12x. f Refs. w19,23,24x. g Refs. w10,16x. h Ref. w21x. i Ref. w11x. j Average of 10 mgrmile; 2=10 12 vehicle miles traveled.

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Table 6 Overview of current knowledge on control of fine particles values for efficiencies and costs are estimates or judgements by the author. Source type Roads Primary control options, efficiencies for PM 10 Vacuum sweeping 050%., Water flushing and sweeping 096%., Paving and roadside improvements, Covering trucks, Speed and traffic reduction Low tillage, punch planting, crop strips, vegetative cover, windbreaks; Chemical stabilizers, irrigation Wet suppression of unpaved areas, material storage, handling and transfer operations; Wind fences for windblown dust Low wind speed and appropriate wind direction Approximate costs of PM 10 controls Dependent on type of control, time of event, frequency of eventryear, and volume of traffic. Very limited published data

Agricultural production including erosion. Construction activities

Dependent on crop type and regional weather conditions. Little data Dependent on type of control, time of event, land area of event, and activity level of equipment. Very limited published data Unknown

Open burning including wild-fires, agricultural burning. Residential wood combustion Diesel engine combustion Mineral products production

Replace with cleaner burning stoves or furnaces Combustion modification, improved fuel characteristics, particle traps Enclosing crushing, transfer areas; Water spray suppression; Chemical stabilization of unpaved traffic areas

;US$1000 per replaced stove or furnace Very limited published data Dependent on type of control and activity level of equipment. Little data

Pulverized coal boilers

ESPs, Fabric Filters

Heavy fuel oil combustion Residential fuel oil combustion Waste incineration Metal smelting and refining Outdoor air introduced into the indoor environment Tracked-in dust

Cyclones, ESPs Proper maintenance, modern furnaces Fabric filters, ESPs, venturi scrubbers ESPs, cyclones Air cleaners for ventilation air 3098%. a ; Whole-building air cleaners 3098%. a ; In-room air cleaners 3098%. a Cleaning e.g., vacuuming.; Whole-building air cleaners 3098%. a ; In-room air cleaners 3098%. a Source control, including maintenance; Whole-building air cleaners 3098%. a ; In-room air cleaners 3098%. a

Capital cost US$50100 per kW, annual cost 25 millsrkWh, total installed cost US$2550 per m3 rh Unknown Unknown Total installed cost US$1530 per m3 rh Total installed cost US$1530 per m3 rh Capital cost US$310 per m3 rh of outdoor air treated. Capital cost US$110 per m3 rh of indoor air treated. US$200800 per room No published analyses. Capital cost US$110 per m3 rh of indoor air treated. US$200800 per room Highly variable; no published analyses. Capital cost US$110 per m3 rh of indoor air treated. US$200800 per room W.G. Tuckerr Fuel Processing Technology 6566 (2000) 379392

Indoor activities that generate or resuspend particles.

a

Range of single-pass efficiency for removing particles. The effectiveness of air cleaners in reducing exposures to indoor particles is very dependent on installation and operating conditions, and is generally less than the single-pass efficiency.

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on-the-highway diesel vehicles, wood stoves and fireplaces, oil- and coal-fired boilers, and open burning of biomass. Other areas of emphasis are validation of instrumentation for measuring rates and size distributions of emissions from fugitive dust sources, and ammonia emissions from animal feeding operations. Source priorities are established in consultation with EPAs Office of Air Quality Planning and Standards OAQPS.. Field studies of sources are being arranged in connection with one or more of EPAs ambient monitoring supersites. Chemical profiles of source emission samples and ambient samples collected at an appropriate supersite monitoring station will be developed, and source apportionments will be calculated to estimate contributions of the source to the ambient air at the monitoring site. This will develop improved emission factors and source profiles that can be used in implementation planning by the states, using either source- or receptor-oriented modeling. A similar approach will be used to apportion indoor exposure to fine PM among indoor and outdoor sources. The overall objective of the risk management evaluation research is to evaluate the cost and effectiveness of currently available options for reducing emissions of primary particles and gaseous precursors of secondary particles, and exposures to ambient and indoor fine particles. Current focus is on pilot-scale field evaluation of devices for industrial and utility boilers. A paper study is also underway to develop a framework for evaluating fine PM control strategies for all types of sources. Laboratory- and house-scale studies are being conducted to understand how penetration of outdoor particles into buildings is affected by particle size, composition, environmental conditions, and building operational conditions.

5. Summary Growing concerns about the health risks of fine particles have led to the promulgation of a revised national ambient air quality standard for PM smaller than 2.5 mm in aerodynamic diameter PM 2.5 . in the U.S. The existing data base on national emissions shows that sources of both primary and secondary particles make significant contributions. On a nationwide basis, the greatest mass of primary and precursor emissions come from combustion, fugitive, and industrial sources, in that order. In specific localities, any of these source categories can be dominant. It appears that the new emphasis on fine particles will focus risk management research on large sources and combustion sources of various types. The role of fugitive sources in creating exposures to fine particles is less clear, and field studies to obtain better emissions data are needed. The importance of exposures inside buildings is also unclear; the penetration of outdoor particles into buildings of various types and the role of indoor sources of particles need further study. Current knowledge of the costs and effectiveness of control options for PM 10 is limited and poorly documented. Carefully documented data on control options for PM 2.5 are nearly non-existent. A risk management research program is now in the early stages of developing new information to address several questions: What sources contribute to the fine particle exposures that are of greatest concern to the health research and regulatory community?

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What are the emission rates and physical and chemical characteristics of particles from these sources? What are the most cost-effective prevention and control options for these sources e.g., process changes, upgrades of existing controls, application of new technology.? Risk management researchers are currently emphasizing source characterization research that produces new information on PM 2.5 emission factors and chemical profiles to enable better source apportionment by either source- or receptor-oriented modeling. They are also extending collaborations with health researchers to increase toxicity testing of particles for a wide variety of sources. Types of sources include on-the-highway diesel trucks, residential wood combustion, oil- and coal-fired boilers, fugitive dust-generating construction activities, open burning of biomass, and indoor sources of fine PM. Research results will enable the U.S. Environmental Protection Agency to assist state and local regulatory agencies in the development of cost-effective local prevention and control strategies for reducing exposures to fine particles. These strategies are likely to be based on a combination of industrial process changes, improved operation of existing particle control devices, installation of new control equipment on selected sources, increased control of gaseous precursors to ambient fine particles, and control of particles in buildings.

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