U'~.:iei1 States        Environr^r-.tai Crie-'i* -r-.o     EPA ^CHj c> ~'r'•'•'•• •>
            Env^cnmemai protecnor   Assessment Off r^         June 1979
            Agency          Research Tr.,ingif '?,>••. M :.'.••; i -
<>EPA    Suspended Particulate
           Matter

           A Report to Congress

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                                  EPA-600/9-79-006

                                       June 1979
Suspended  Particulate
               Matter
      A Report to Congress
                    by

              Lucile F. Adamson, Ph.D.

     Professor, Macroenvironmental and Population Studies
                Howard University
              Washington, D.C. 20059

                    and

              Robert M. Bruce, Ph.D.

                Health Scientist
       Environmental Criteria and Assessment Office
          Office of Research and Development
       Environmental Criteria and Assessment Office
          Office of Research and Development
          U.S. Environmental Protection Agency
       Research Triangle Park, North Carolina 27711

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                                DISCLAIMER







This report has been reviewed by the Office of Research and Development,



EPA, and approved for publication.  Mention of trade names or commercial



products does not constitute endorsement or recommendation for use.
                                    n

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                                  PREFACE







     This report was written in accordance with Section 403(a)(l) of the Clean



Air Act Amendments of 1977, P.L.  95-95, as noted under 42 U.S.C.  Section 7548.



The purpose of this report is to assess health and welfare effects caused by



suspended particulate matter in relationship to size, weight, and chemical



composition.



     The report does not constitute an in-depth review of the original



published literature; rather, it summarizes, through the use of recent reviews



by well-known experts in the field, the current scientific position with



regard to knowledge of airborne particles, their effects on public health and



welfare, and the respective levels at which these effects are thought to



occur.



     The Agency is pleased to acknowledge the efforts of all persons and



groups who have participated in preparing this document.

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                                 ABSTRACT







     This report is in response to Section 403(a)(l) of the Clean Air Act



Amendments of 1977, P.L. 95-95, as noted under 42 U.S.C. Section 7548.   The



report covers (1) a review of the physical and chemical characteristics of



airborne particles (source, composition, and sampling site as related to



size); (2) a review of the effects of particulate matter on public welfare



(ecological, materials, atmospheric, aesthetic); (3) the status of human



exposure to airborne particles as related to source; and (4) a review of the



effects of airborne particles on human health (lung deposition, chemical



composition, interactions, and potentiating conditions).



     Although there is a wide divergence of opinion among experts and



scientific groups with respect to the issues of particulates the following



can be concluded from the available information:



     1.   A major portion of the adverse health and welfare effects of air



          pollution is due to airborne particles.



     2.   Although pollution levels have declined in many U.S.  localities in



          recent decades, there is still need for improvement in several of



          our cities.



     3.   Additional  research is needed to improve the scientific basis for



          future airborne particle standards as outlined by EPA (cf.  Inhalable



          Particulate Research Plan, Project Officer, Dr.  Roger Cortesi, EPA,



          ORD).

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                                 CONTENTS
PREFACE	       iii
ABSTRACT	        iv
FIGURES	        vi
TABLES	       vii
LIST OF REVIEWERS	      viii
TECHNICAL SUPPORT 	        ix

1.   EXECUTIVE SUMMARY  	         1
2.   INTRODUCTION	         7
3.   CHARACTERISTICS OF AIRBORNE PARTICLES  	         8
     3.1  PHYSICAL CHARACTERISTICS OF AIRBORNE PARTICLES	         8
     3.2  CHEMICAL CHARACTERISTICS OF AIRBORNE PARTICLES	        12
4.   AEROSOLS:  SOURCES AND CONCENTRATIONS	        20
     4.1  SOURCES AND EMISSIONS	        20
     4.2  TRANSFORMATION AND TRANSPORT	        27
     4.3  CONCENTRATIONS	        28
5.   EFFECTS OF AIRBORNE PARTICLES ON HUMAN HEALTH	        36
     5.1  DEPOSITION OF AIRBORNE PARTICLES IN THE LUNG	        36
     5.2  HEALTH EFFECTS OF GENERAL AIRBORNE PARTICLE POLLUTION .        37
     5.3  CONDITIONS WHICH MAY POTENTIATE HEALTH EFFECTS OF
          AIRBORNE PARTICLES	        45
     5.4  HEALTH EFFECTS OF SPECIFIC CHEMICAL COMPOUNDS 	        47
     5.5  HEALTH COST ANALYSES	        57
     5.6  DEFICIENCIES IN THE SCIENTIFIC DATA BASE	        58
6.   EFFECTS OF PARTICULATE MATTER ON PUBLIC WELFARE	        62
     6.1  ECOLOGICAL EFFECTS	        62
     6.2  EFFECTS ON MATERIALS	        63
     6.3  ATMOSPHERIC AND CLIMATIC EFFECTS	        64
     6.4  AESTHETIC EFFECTS 	        65
7.   REFERENCES	     67-75

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                                  FIGURES

                                                                      Page

1.   Comparison of volume distributions measured by
     several investigators in different locations 	       10
2.   Estimation of TSP levels by the Hi-Vol method
     under varying conditions of particulate pollution	       18
3.   TSP annual means at 17 urban NASN stations	       30
4.   Benzo(a)pyrene seasonality and trends (1966 to 1975) in
     the 50th and 90th percentiles for 34 NASN urban sites.  ...       31

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                                  TABLES
 1.   Geometric mean and 90th percentile urban participate
     concentrations in the United States,  1971-1975 	        14
 2.   Correlations of chemical  content with particle size	        16
 3.   Global  estimates of particles smaller than 20 urn
     radius  emitted into or formed in the  atmosphere	        21
 4.   Nationwide estimates of particulate emissions, 1940-1970 .  .        23
 5.   Recent  nationwide emission estimates  1970-1977 	        24
 6.   Emission estimates for major sources  of certain
     airborne particles 	        26
 7.   Trends  in urban metal concentrations  and their
     possible causes	        32
 8.   Ratios  of urban (U) to suburban (S) concentrations in
     air, Cleveland, Ohio area	          34
 9.   Health  effects and dose/response relationships for
     particulates and sulfur dioxide	          39
10.   Threshold estimates for adverse health effects
     attributable to sulfur dioxide, particulate sulfate,
     and total suspended particulates (TSP), short-term
     exposures	         40
11.   Threshold estimates for adverse health effects
     attributable to sulfur dioxide particulate sulfates,
     and total suspended particulates (TSP), long-term
     exposures	     41-42
12.   Variables related to the health effects of airborne
     particles	        44
13.   Comparison of health cost studies.	     59-60
                                   VII

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                             LIST OF REVIEWERS
     Appreciation is extended to the following persons for their efforts in
reviewing this report.

Mr. John Bachmann, Office of Air Quality Planning and Standards, U.S.
     Environmental Protection Agency, Durham, N.C.

Mr. Michael A. Berry, Environmental Criteria and Assessment Office, U.S.
     Environmental Protection Agency, Research Triangle Park, N.C.

Dr. Donald E. Gardner, Health Effects Research Laboratory, U.S. Environmental
     Protection, Agency, Research Triangle Park, N.C.

Dr. Robert E. Lee, Health Effects Research Laboratory, U.S. Environmental
     Protection Agency, Research Triangle Park, N.C.

Mr. Thomas McMullen, Environmental Criteria and Assessment Office, U.S.
     Environmental Protection Agency, Research Triangle Park, N.C.

Dr. Fred Miller, Health Effects Research Laboratory, U.S.  Environmental
     Protection Agency, Research Triangle Park, N.C.

Ms. Beverly E. Tilton, Environmental Criteria and Assessment Office, Research
     Triangle Park, N.C.
                                   vm

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                             TECHNICAL SUPPORT

     The following persons are recognized and acknowledged for their
invaluable services in the preparation of this document.

Ms. Dela Bates, Environmental Criteria and Assessment Office, U.S.
     Environmental Protection Agency, Research Triangle Park, N.C.   27711

Ms. Vandy Duffield, Environmental Criteria and Assessment Office, U.S.
     Environmental Protection Agency, Research Triangle Park, N.C.   27711

Mr. Douglas Fennel 1, Environmental Criteria and Assessment Office,  U.S.
     Environmental Protection Agency,.Research Triangle Park, N.C.   27711

Mr. R.  Wayne Fulford, Health Effects Research Laboratory, U.S. Environ-
     mental Protection Agency, Research Triangle Park, N.C.   27711

Mr. Allen G. Hoyt, Environmental Criteria and Assessment Office, U.S.
     Environmental Protection Agency, Research Triangle Park, N.C.   27711

Ms. Bonnie Kirtz, Health Effects Research Laboratory, U.S. Environmental
     Protection Agency, Research Triangle Park, N.C.  27711

Ms. Evelynne Rash, Environmental Criteria and Assessment Office, U.S.
     Environmental Protection Agency, Research Triangle Park, N.C.   27711
                                    IX

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                             1.  EXECUTIVE SUMMARY



     This document is submitted as a Report to Congress, mandated by Section

403(a)(l) of the Clean Air Act Amendments of 1977, P.L. 95-95, as noted under

42 U.S.C. Section 7548, concerning the health and welfare effects of airborne

particle pollution.  The report provides an extended summary of these effects

primarily as described in the review by the National Academy of Sciences (MAS)

(Airborne Particles).   but also as described in other recent reviews.  These

reviews are:  (1)  Health Effects of Particulate Pollution:  Reappraising the

Evidence.  A. E. Bennett et al., 1978; (2) Environmental Health Criteria for

Sulfur Oxides and Suspended Particulates.  World Health Organization, 1978;

(3) Fine Particulate Pollution.  World Health Organization, 1977; (4) Intra-

urban Mortality and Air Quality:  An Economic Analysis of Pollution Induced

Mortality.  J. Gregor, 1977; (5) Total Suspended Particulates:  Review and

Analysis.  R. Wells, 1976; (6) Air Quality Criteria for Particulate Matter,

National Air Pollution Control Administration, 1969.  The report represents an

interim summary of health and welfare effects associated with airborne particles.

A comprehensive review of health and welfare effects and other aspects is

currently being conducted as part of the revision of the particulate matter
                                                                             t-
criteria document.  An external review copy of the criteria document will be

available by late 1979, with final publication by late 1980.  The material in

this interim report is summarized under several headings as indicated below.

Characteristics of Airborne Particles

       Airborne particles include a variety of chemical substances distributed

over a wide range of particle sizes.  The distinction between "fine particles"

[<2 micrometers,  ((jm)] and "coarse particles" (>2 pm)  is a fundamental one.

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There is now an overwhelming amount of evidence that not only are two modes



usually observed in the mass or volume distribution of well-mixed urban and



rural aerosols, but that the fine and coarse modes are normally quite diffe-



rent in chemical composition.  The fine and coarse particle modes originate



separately, are transformed separately, are removed from the atmosphere by



different mechanisms, require different control techniques, have different



chemical composition, have different optical properties, and exhibit differential



penetration of the respiratory tract.  Therefore, the distinction between fine



and coarse particles is of fundamental importance to any discussion of the



physics, chemistry, measurement, and respiratory tract deposition of aerosols.



     The major components of the fine fraction of the atmospheric aerosol are



sulfates, ammonium ions, hydrogen ions, condensed organic matter, and trace



levels of lead.  The fine fraction, as a percentage of total suspended parti-



culate matter, varies from 20 to 60 percent in urban areas.  The percentage of



the fine particle fraction which is formed mainly from atmospheric photo-



chemical reactions varies from 60 to 80 percent in these urban areas (percentages



based on short-term, intensive studies).   Also, several studies have shown that



potentially toxic carcinogenic species, such as polynuclear aromatic compounds,



arsenic, selenium, cadmium, and zinc, which can exist as vapors are more



concentrated in the fine particle fraction.



        Materials typically found in the coarse fraction include those pro-



duced from mechanical processes such as grinding operations; rubber tire



particles and other road dust; and also wind-blown dusts, sea salt, and pollen.



Sources and Concentrations



     Exposures to airborne particles are determined not only by the amount and



type of emitted pollutants, local topography, and meteorological conditions,

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but also by one's residential or occupational proximity to sources of such
pollution and the rate, depth, and mode (mouth or nose) of breathing.  For
those pollutants that can accumulate in tissues, such as lead, cadmium, and
fat-soluble organic compounds, tissue levels can increase with duration and
frequency of environmental exposures.
     Although the mass emissions of airborne particles from natural sources
are thought to exceed those from man-made sources, naturally derived particles
are both quantitatively and qualitatively less significant to human exposures
in the urban environment.  As an example, it has been estimated that the
natural particle component of the Los Angeles aerosol is less than 30 percent
of the total.  These natural particles (sea salts, dust, etc.) are also
generally less hazardous to healthy individuals than are many of the particles
from man-made sources.  Indoor concentrations of airborne particles are some-
times as great or greater than outdoor concentrations, particularly in certain
occupational settings and in homes in which cigarette smokers live.  Typi-
cally, urban environmental concentrations greatly exceed those of rural loca-
tions.  Urban particulate pollution increased by 18 percent from 1940 through
1970, principally due to stationary fuel combustion sources and industrial
process losses.  Subsequent to 1970, particulate levels began to decline.   The
most significant downward trends in emissions were 33 percent for stationary
fuel combustion sources and 54 percent for industrial processes.  These down-
ward trends resulted from the change from coal to natural gas and oil, the
adoption of local smoke control ordinances, and the adoption of national emission
standards.  This decreasing trend that has been observed from 1970 through
1977 does not imply that all components of total suspended particulate are
decreasing.  However, a number of toxicologically significant particulates

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such as trace metals and polycyclic organic matter have decreased.   Prominent



among the metal components of total suspended particulate showing a decline



are vanadium, manganese, and nickel.  Nationwide lead averages have declined



since 1972 due to the introduction of the lower compression engines and the



use of lower lead gasoline.  This trend should continue with the shift of



usage from low-lead gasoline to no-lead gasoline.



Health Effects



     There has been increasing emphasis on examining what particle size fraction



is of significance for health impacts.  Recently,  the EPA evaluated available



information on the disposition of particles in the human respiratory tract.



The analysis is summarized in "Size Consideration  For Establishing A Standard



For Inhalable Particles."  This analysis provides  the theoretical basis for



designation of a size-specific airborne particle standard that would provide



for more effective control of those particles most likely to be responsible



for adverse health effects.  The analysis indicates that under the most sensitive



conditions (mouth breathing) particles of up to 15 micrometers in diameter can



penetrate to the upper portions of the lung (conducting airways).  This fraction,



termed inhalable particulate (IP) matter makes up  roughly 50 to 60 percent of



total suspended particulate matter and includes all of the fine (<2.5 urn) and



some of the coarse (2.5 to 15 urn) mode fraction.   Based on this analysis, a



major expansion of air pollution monitoring and health studies was initiated



in 1979 to monitor and evaluate the health effects of inhalable as well as



fine particulate matter.



     Past studies of particulate pollution have indicated that high levels of



airborne particle pollution are correlated with increased incidence, prevalence



and severity of respiratory diseases and with increased mortality from these

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and other diseases. The minimum concentration and duration of airborne particle
exposure at which these health effects become significant cannot be precisely
specified at this time.  Furthermore, due to the limitation of monitoring
methods used in these historical studies, it is difficult to correlate
health effects directly with particle size and chemical  composition.
     Various reviews of the available information, including a report by a
task force of the World Health Organization (1979), have concluded either that
levels approximating the present primary TSP standards are reasonable ones for
protection of public health or that there is not sufficient justification to
change these standards on the basis of present knowledge.  Others have concluded
that the standards are more stringent than can be justified on the basis of
present knowledge.  Additional research is needed on the chemical and physical
properties of particles in order to define better the characteristics and
magnitude of particulate exposures which are consistent with public health.
Welfare Effects
     Airborne particles produce well-documented effects on public welfare
which include adverse effects on building materials and other exposed sur-
faces, atmospheric conditions, and aesthetic conditions, as well as possible
influences on global temperatures and climate.  The aesthetic effects of
particulate pollution include the soiling of fabrics, buildings, and other
surfaces, cultural losses due to damage to exposed architectural and historic
artifacts, and degradation of visibility.  Airborne particles have been
associated with increased cloud cover and precipitation and have been
implicated in shifts in temperature and climate.  Moreover, airborne particles
can seriously damage vegetation, wildlife, and natural systems when removed
from the atmosphere by snow and rainfall.  Long-range transported fine sulfates

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and nitrates acidify soils and surface waters;  nitrates, organic, and
metallic substances in fine particulates can accumulate to harmful levels in
soil, water, and plants.
     It can be concluded that (1) a major portion of the adverse health and
welfare effects of air pollution is due to airborne particles;  (2) although
pollution levels have decreased in many localities in recent decades,  there is
still need for considerable improvement in some of our cities;  and (3) addi-
tional research is needed to improve the scientific basis for future airborne
particle standards.

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                               2.  INTRODUCTION

     Section 403(a) of the Clean Air Act Amendments of 1977, P.L.  95-95, as
noted under 42 U.S.C. Section 7548, requires the Administrator of the Environ-
mental Protection Agency, in cooperation with the National Academy of Sciences,
to submit before February 1979, a report to the Congress "on (1) the relationship
between the size, weight, and chemical composition of suspended particulate
matter and the nature and degree of the endangerment to public health or
welfare presented by such particulate matter (especially with respect to fine
particulate matter) and (2) the availability of technology for controlling
such particulate matter."
     This report is submitted in fulfillment of the first part [403(a)(l)] of
that requirement.  The form of the report is as follows:
     Following the Executive Summary and the Introduction, Sections 3 through
6 present brief statements of the current scientific position with regard to
knowledge of airborne particles and their effects on public health and wel-
fare.  References to prior reviews and to research reports are provided for
those readers who wish additional documentation or detail.

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                   3. CHARACTERISTICS OF AIRBORNE PARTICLES



3.1  PHYSICAL CHARACTERISTICS OF AIRBORNE PARTICLES

3.1.1 Size of Ambient Aerosol Particles

3.1.1.1  Aerodynamic Equivalent Diameter —Inasmuch as airborne particles are

quite variable in shape, density, and chemical properties, their size and

weight are generally characterized by an indirect measure referred to as the

aerodynamic equivalent diameter:  the diameter of a spherical particle of

density 1.0 which would fall through air in earth's gravitational field at the

falling speed of the observed particle.  Aerodynamic equivalent diameter is,

therefore, a function of both shape and density and is not necessarily indica-

tive of the actual diameter of the observed particle.  References in this

report to particle diameter refer to this measure.

3.1.1.2 Size Distribution-'-Suspended atmospheric particles range in diameter

from a few nanometers (nm) to several hundred micrometers (urn).*  The numeri-

cal distribution of particles within this range normally exhibits two or three

maxima.   The bimodal distribution, with maxima at about 0.3 and 10 pm and a

minimum at about 2 pro. is most common; but trimodal distributions (with the

third peak (nuclei mode) corresponding to particles with diameters less than

0.1 jjm) are also observed in ambient aerosols.  Two micrometers is often used

as the approximate demarcation point between "fine" and "coarse" particles.

Within the definition of fine particles two distinct populations can exist,

the "Aitkin nuclei" (<0.1 urn), emitted as such or formed by vapor condensation,
* This corresponds to a range from approximately the ultramicroscopic diameter
 of the smaller viruses to the diameter of dust particles which are easily
 visible.   A nanometer is one one-thousandth of a micrometer (micron).
                                     8

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and the "accumulation mode" particles (0.1 to 2 pm), formed chiefly by coagu-
lation and condensation of smaller particles.  In fresh emissions,  the Aitkin
nuclei are usually numerically predominant, whereas in well-aged aerosols most
of the fine particles are in the accumulation mode.  The ratio of mass and
volume to particle size varies with the geographical location, the predominant
type of pollution (fugitive dust or photochemical products) and the age of the
aerosol.   Examples of volume distribution curves for particles measured by
several investigators at different locations are shown in Figure 1.   For more
information on particle size, see Chapter 2 of the National Academy of Sciences
document prepared for EPA titled Airborne Particles.
3.1.1.2  Variation of Particle Size According to Source--To a large extent,
the initial size of an airborne particle depends upon its source.  Secondary
particles, formed in the atmosphere by condensation and/or chemical reactions
of gases (such as sulfuric acid or organic solvent droplets), are very small
initially.  Although they rapidly grow by coagulation, most of them remain in
the submicrometer range, also referred to as the accumulation mode.
     Combustion processes, including automotive operation, produce particles
which are mostly less than 1 urn in diameter, including particles of soot,
various organic materials, and lead salts from leaded gasoline combustion.
Many other chemical processes, such as sulfuric acid manufacture, also produce
submicrometer-sized particles.  Other sources which produce substantial amounts
of fine particle emissions include metallurgical processes, paper mills,
cement plants, and asphalt plants.
     Grinding processes and most natural processes usually produce predominantly
large particles (>2 urn).  However, there is  no reason to assume that they do
not also produce fine particles.

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P)
 a
a
     100
      80
      60
      40
      20
L.A..1969,
342 RUNS
                   I  I  I II III!    I  I

                        MPLS       /
                  (PETERSON, 1967),'
                     45',7 RUNS /
                                    COLORADO./ /
                                    1970,3 RUNS,  /
                                                 \  I
                                  f  '/   JAENICKE*.   i
                                    '.'     &JUNGE*.  \
                                  k\
                          SEATTLE
                      •' //        (1967) \ ,

                      '                   •• \
     MPLS
 (CLARK, 1965)
"  56 RUNS f f
           ''^•^(NOLL)   V,'  .-•'OKITA''..
          is i    ~-'-*^   i/'*'    '   (1955)
   i  i t^wTnl -- T  ill hTPt "I  i i n nil    i  i  i 11 ml  'J •

       0.01
O.J
                                                10
                                                            100
                     PARTICLE DIAMETER (Dq), micrometers
    Figure 1. Comparison of volume distributions measured by several investigators
    in different locations.1
                                     10

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3.1.2  Physical State of Airborne Participate Matter



     Airborne particles, a phrase that is used interchangeably with "ambient



aerosol," consist of both liquid and solid particles.   Although these phrases



are not normally understood to encompass particles of pure water, fine particles



often serve as condensation or stabilizing nuclei and are associated mechanically



with rain, fog, mist, and hail.



     Aqueous droplets of dissolved or hydrated gases or solids are included



conceptually within the definition of airborne particles.  The fine particle



fraction, especially, may contain a substantial liquid component at normal



temperatures and humidities.  Depending on the relative humidity, the liquid



content of the fine particle fraction will vary considerably; for example, 50



percent of the fine particle fraction is water at 80 percent relative humidity.



     Many of the fine particles (0.1 to 2 urn) are hygroscopic and, in some



cases, deliquescent; and may change back and forth from the liquid to solid



state with changes in ambient humidity.  Solution/solid droplets of this



nature include those of ammonium sulfate, sodium sulfate, sodium chloride, and



ammonium nitrate.



     Other hygroscopic particles, while not undergoing a phase change, will



exhibit changes in size with changes in humidity.  Examples are particulate



sulfuric acid, glycols, sugars, organic acids, and alcohols.  Sulfuric acid



and ammonium bisulfate are aqueous solution droplets at all relative humid-



ities from 30 to 100 percent.



     Because the true mass of aqueous particles is not detected by methods



which weigh or measure reflectance of filter-collected particle samples, water



is often exempted from mass measurements of particulates.  Therefore, as noted
                                     11

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above, measurements  of  airborne  particles by these methods will underestimate



both the mass  and  content  of  aerosols containing, for example, aqueous solutions



or volatile  or gaseous  materials such as soluble organic compounds, nitric

                 2
acid, or ammonia.    However,  as  noted above, the reverse error--the iji situ



formation  of spurious particles  on the collection filter due to chemical and



physical interaction of the filter with atmospheric gases—also occurs and



has been cited as  a  source of overestimation of the sulfate and nitrate content


                     3  4 50
of ambient particles. '  '     For example, two types of filters in common use



were reported  to collect 10 to 20 times as much artifactual as ambient parti-

                4

culate nitrate.



3.1.3.  Primary and Secondary  Airborne Particles



     Primary particles  are those that are emitted as such; secondary particles



are those  formed in  the  atmosphere.  Many of the ambient air particles are



"secondary"  aerosols:   particles which are formed from materials (such as



sulfur oxides  and  organic  vapors) which are emitted as gases but which, upon



cooling or upon chemical reaction within the atmosphere, condense to form



particles.    It has been  estimated that secondary particles constitute as much



as one-half  of urban aerosols and 25 percent of the particulate pollution in



the nation as  a whole.



     Primary particles  (those emitted as particles) are both coarse and fine,



while most but not all   secondary particles are in the "fine" size range.



3.2  CHEMICAL  CHARACTERISTICS OF AIRBORNE PARTICLES



     The specific  chemical composition and characteristics of any atmospheric



aerosol sample will  depend upon  the sources of the particles and on any reac-



tion or selection  that occurs during the residence time of the particle in the
                                     12

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atmosphere.   Ambient aerosols are typically mixtures of greatly diluted emissions
from numerous sources and are collected (or inhaled) after varying periods of
settling, atmospheric mixing, atmospheric chemical reactions,  and exposure to
atmospheric humidity and washout.  Therefore, the chemical characteristics of
different samples can be extremely variable and complex.
     Some of the chemical characteristics of ambient particles which are
environmentally significant are composition, water solubility, acidity, hygro-
scopicity, deliquescence, efflorescence, and toxicity of both  the atomic and
molecular components of the particle.
3.2.1  Composition
     Chemical categories of airborne particles which are of particular concern
are toxic (including carcinogenic) organic compounds, inorganic fibers, toxic
metals, and inorganic acids.  To a large extent, chemical analyses of aerosols
have determined atomic rather than molecular identities.   A summary of the
composition of ambient aerosol samples determined by the National Air Sampling
                            fi-ft
Network is given in Table 1.     It can be seen that, of the components
listed, sulfate is present in greatest amount, followed in order by nitrate
anion.  Of the metals, average concentrations were highest for iron and lead.
     Acidity of airborne particles derives primarily from the  presence of
sulfuric acid, which is formed chiefly as secondary particles  by oxidation of
emitted sulfur oxides.  Nitric acid, which is also present, is generally in
the vapor state.  Some of the sulfuric acid is neutralized by atmospheric
ammonia and other cations.  Sometimes, however, it remains partially un-
neutralized even in the presence of more than enough ammonia for theoretical
               g
neutralization.   It has been hypothesized that coating of the acid particle;
by organic material protects them against neutralization.
                                     13

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        TABLE 1.  GEOMETRIC MEAN* AND 90th PERCENTILE URBAN PARTICIPATE
                CONCENTRATIONS IN THE UNITED STATES, 1971-1975
Pollutant
Suspended parti culates0
Fractions:
Nitrates6
Sul fates
Ammonium (salts)
Beryllium
Cadmium
Chromium
Cobalt
Copper
Iron
Lead
Manganese
Nickel
Titanium
Vanadium
Concentration, ug/r
Geometric mean 90th
-61
2.56
8.42
0.05
LD.f
L.D.
0.006
L.D.
0.114
1.18
0.86
0.03
L.D.
0.032
L.D.
n3
4.-i b
percent! le
-97
6.16
18.36
0.91
0.08
0.007
0.140
LD
0.37
2.32
1.78
0.92
0.034
0.08
0.07
 Based on 50th percentile
 90th percentile of quarterly composite measurements.
cRepresent 1792 sampling sites.
 Represents 300 of the 1,792 Hi-Vol sampling sites.
ePossibly high by 70 to 90% due to artifacts.
 L.D. - Less than discrimination limit.
                                     14

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3.2.2  Composition as Related to Size


     There are certain correlations between particle size and chemical  com-


position, as indicated by the two summaries given in Table 2.        Sulfate,


nitrate, elemental carbon, condensed organic vapors, ammonium ion, and lead


occur chiefly in the fine-particle fraction and make up the major part of that


fraction.  In six U.S. cities, the mean diameter of particles containing


metals ranged from a low of 0.4 to 0.7 pm for lead and vanadium to a high of


2.4 to 3.5 urn for iron.  Particle diameters for polycyclic organic matter were


found by another study to range from 0.3 to 0.5 pm.


     Various metals, as indicated by Table 2, plus alkaline particles and


plant parts, occur chiefly in the coarse fraction.  This fraction consists


largely of mechanically produced particles such as soil, road and tire dust,


and rock dust.


3.2.3 Effect of Sampling Method on Measured Particle Pollution --The two


classical and historically most significant approaches to measuring the mass


of airborne particles are based on gravimetric measurement of particles collected


on a filter (Hi-Vol Sampler) and on optical transmission or reflectance of


particles collected on filters (British Smoke Shade and AISI tape samplers).


The British Smoke Shade method* measures the degree of blackening of a filter

                                     3
through which a low velocity (0.05 ft /min) stream of ambient air has been


drawn for a specified length of time.  The mass of particles accumulated on


the filter is measured in terms of reflectance and converted to a mass basis


by means of a "standard smoke" calibration and ultimately reported in micrograms


per cubic meter.


     The gravimetric method used most commonly in the United States has been


the High-Volume (Hi-Vol) Method.  Particles from a high-velocity  (40 to 60
*Hereinafter referred to as the Smoke Shade method.


                                     15

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     TABLE 2.  CORRELATIONS OF CHEMICAL CONTENT WITH PARTICLE SIZE
       a) Predominant Particle Size for Various Substances
                                                           Variable
                                                            Nickel

                                                            Tin
                                                            Vanadium
                                                            Antimony
                                                            Manganese
                                                            Zinc
                                                            Copper
Ammonium salts
Soot
     b) Ratios of Element Distribution Between Fine and Coarse Particles
Normally fine
Sul fates

Organic (con-
densed vapors)

Lead

Arsenic

Selenium

Hydrogen ion

Normally coarse Normally bimodal
Iron Chloride
Calcium
Titanium Nitrate

Magnesium

Potassium

Phosphate

Silicon

Aluminum
                                                  20
          (St.  Louis Urban Aerosol, 18-day average, Aug.-Sept.,  1975)
          Predominantly fine
         Element   Fine/coarse
                     Predominantly coarse
                     Element   Fine/coarse
         Sulfur
         Lead
8.90
3.67
  Calcium
  Silicon
     Iron
Potassium
 Titanium
0.09
0.13
0.29
0.33
0.55
                                16

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ft /min) ambient air stream are collected on a filter and weighed.   Larger



particles, including blowing dust particles, can be entrained in the rapid air



stream and collected by this method.  Therefore, except at very high levels of



fine particle pollution, and assuming constant sampler flow rate, measurements



of ambient particulate matter typically give higher values by Hi-Vol than by



the Smoke Shade method. The disparity is greatest at lower levels of parti-



culate pollution (when coarse particles represent a larger fraction of the



Hi-Vol sample).  For example, an urban pollution Hi-Vol measurement of 200


    3                                                                3
pg/m  was reported to correspond to a Smoke Shade reading of 100 ug/m , while


           3                                                     21
at 500 ug/m  the two methods yielded approximately equal results.    However,



with unusually dark particles, the Smoke Shade method can give values higher


                                          22
than the corresponding gravimetric values.    Markedly varying particulate



concentrations during the sampling period may result in Hi-Vol sample biases



because the collection efficiency decreases non-uniformly over the sampling



interval as more particles are deposited on the filter (Figure 2).   Under-



estimation of particulate levels can result under conditions of constant TSP



levels (Figure 2A) and under conditions of increasing TSP levels (Figure 2B).



If particulate levels are declining (Figure 2C), an overestimation can result.



     It should be kept in mind (1) that the Smoke Shade Method can under- or



overestimate the collected particulate matter depending upon whether the



particles are unusually optically light or dark since this method depends on



reflectance, whereas gravimetric methods are col or-independent; (2) that some



overestimation of particle mass by the Hi-Vol method will occur due to inter-



action of the acid gases (i.e., S02, N02, HN03) with the alkaline surface of


                       3 4
the glass fiber filter;  '  and (3) that both methods will fail to adequately



quantify the mass of those particles that consist of air pollutants dissolved



or suspended in or on aqueous droplets.
                                     17

-------
                  CONSTANT TSP WITH TIME
 c
 1
w"
 «
                      ASSUMED AVERAGE FLOW RATE
                              -l/ZtQj + a,)
                          OVERESTIMATES FLOW
                          UNDERESTIMATES TSP
TSP
                     TIME
                 INCREASING TSP WITH TIME
 c
 1
co"
 QC

 O
 u.
               HIGHEST FLOW AT LOWEST TSP
               LOWEST FLOW AT HIGHEST TSP
               RESULT: UNDERESTIMATES TSP
                     TIME
                 DECREASING TSP WITH TIME
 c
 I
«n~
 e
 u
               HIGHEST FLOW AT HIGHEST TSP
               LOWEST FLOW AT LOWEST TSP

               RESULT:  OVERESTIMATES TSP
                     TIME
Figure 2. Estimation of TSP levels by the Hi-Vol method under varying
conditions of paniculate pollution.
                    18

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     In addition to the above instruments that have been used routinely in the



United States and England for measuring the total  mass of aerosols,  impactors



afford the additional option of separating the airborne particles according to



size for subsequent chemical analysis.   Impactors  that separate aerosol particles



depend upon the relative balance between inertial  and aerodynamic forces.   In



the conventional type of aerosol impactor (e.g., cascade), an airstream turns



abruptly as it approaches a flat surface.  Particles with the largest inertia



tend to maintain a straight trajectory and impact  on the surface, whereas



smaller particles will follow the air streamlines  and not be collected.



Inertial impactors such as these have been used extensively to collect air-



borne particles (e.g., CHESS data); however, difficulties with particle bounce,



reentrainment, and non-uniform deposition have limited their use.  To reduce



particle bounce error the impaction surface may be coated with a non-volatile



grease; however, large weighing errors are often encountered using greased



surfaces.   The problem inherent in collection by impaction onto surfaces is



eliminated by using a "virtual" impactor in which  particles are impacted into



a slowly pumped void and in turn pulled onto a filter.  The dichotomous "virtual"


                                           85
impactor as described by Stevens and Dzubay   was  designed with an aerosol



inlet such that the instrument fractionated particles into <3.5 urn and >3.5 urn



with an upper limit of 20 urn.  In order to provide a data base for evaluating



health effects of fine and inhalable particles, the dichotomous sampler and



the aerosol inlet were modified to give cut points of 2.5 urn and 15 urn, res-



pectively.  These particles are to be collected from air samples and deposited



on Teflon filters with a 1.0 urn pore size.  The monitoring network describing



the collection of these inhalable particles has been described by Rodes in

                                                          oc

an Environmental Science and Technology article by Miller.
                                     19

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                   4.  AEROSOLS:  SOURCES AND CONCENTRATIONS







4.1  SOURCES AND EMISSIONS



4.1.1 Global



     Particulate air pollution sources can be categorized as man-made or



natural.  Man-made atmospheric particles are formed by condensation of emitted



gasses, by chemical reactions (including combustion), or by mechanical pul-



verization.  Natural sources include such processes as volcanic action, ocean



spray, dusting of soil, forest fires, and the release of particulate organic



matter from vegetation.  Reentrainment of dust originating from both natural



and man-made sources occurs when previously deposited particles are resuspended



by air movement or other processes.



     Global estimates of particulate emissions are presented in Table 3 for


                                  23
both man-made and natural sources.    This estimate, as well as those by


                    24                   25
Robinson and Robbins   and Hidy and Brock   show that on a global scale anthr-



opogenic particulate sources constitute from perhaps 5 percent to 50 percent



of the total, regardless of particle size and age.    Such estimates of global



aerosol budgets include both primary and secondary particulate; however, they



do not distinguish between fine and coarse particles and cannot be applied



directly to urban regions.   Most aerosol in urban regions is clearly dominated



by emissions from human activity, particularly by the production of sulfur


                                                           26
dioxide from the combustion of oil and coal.   Miller et al.    developed an



approach to an urban budget for the Los Angeles basin showing the relative



importance of human and naturally produced particulate matter, which includes



both primary and secondary particles.
                                     20

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           TABLE 3.  GLOBAL ESTIMATES OF PARTICLES SMALLER THAN 20 urn

                RADIUS EMITTED INTO OR FORMED IN THE ATMOSPHERE23
Type of particles                                    Number in atmosphere,
                                                           109 kg/yr


Natural

     Soil and rock debris3                                   100-500
     Forest fires and slash-burning debris                     3-150
     Sea salt                                                  (300)
     Volcanic debris                                          25-150

     Particles formed from gaseous emissions

          Sulfate from H2S                                   130-200
          Ammonium salts from NH3                             80-270
          Nitrate from NO                                     60-430
          Hydrocarbons from plant exudations                  75-200

                                       Subtotals           773-2,200

Manmade

     Particles (direct emissions)                              10-90

     Particles formed from gaseous emissions

          Sulfate from S02                                   130-200
          Nitrate from NO                                      30-35
          Hydrocarbons                                         15-90
                                       Subtotal              185-415
                                       TOTAL               958-2,616
alncludes unknown amounts of indirect man-made contributions.
                                     21

-------
4.1.2  Nationwide



     Table 4 provides historical data on nationwide estimates of total


                                                             27
participate emissions in the United States from 1940 to 1970.    These data,



derived from major source categories of primary particles, indicate an average



increase of about 0.6 percent per year, from 20.7 to 24.6 million tons.  This



represents an overall increase of approximately 18 percent attributed to



anthropogenic sources, primarily fuel combustion in stationary sources and



industrial process losses.  Table 5 indicates that since 1970 estimated



emissions have decreased due to increased use of particulate control devices,



even though fuel use and industrial output have increased substantially.



Recent emission estimates, based on 1977 emission factors, show that total



emissions from transportation have essentially remained constant throughout


                     28
the 1970-1977 period.    This constant trend is the net effect of the decrease



in the amount of particulate discharged per mile traveled (emission rates) and



the increase in vehicle miles traveled.  In other source categories, namely



stationary fuel combustion and industrial processes, there were significant



downward trends of 33 percent and 54 percent, respectively.



     Estimates for natural sources of particulate far outweigh those attribu-



ted to man on a global scale; however, on a nationwide basis estimates do not



include those particles that are formed in the atmosphere by photochemical



reactions, namely, secondary particles (e.g., sulfates).  On a nationwide



basis the effective manmade impact of secondary particles is extremely



difficult to quantify.



4.1.3  Variation of Chemical Composition with Source



     Although it is not generally possible to identify in detail the specific



sources of an ambient aerosol, there are characteristic chemical differences
                                     22

-------
       TABLE 4.   NATIONWIDE ESTIMATES OF PARTICULATE EMISSIONS,  1940-19703
                               (10  tons/year)
Source category
Fuel combustion in
stationary sources
Transportation
Solid waste disposal
Industrial process
losses
Agricultural burning
Miscellaneous
Total
Total controllable
1940
9.6
0.4
0.4
8.8
1.6
6.4
27.1
20.7
1950
9.0
0.4
0.6
10.8
1.8
3.3
25.9
22.6
1960
7.6
0.5
1.0
11.9
2.1
2.1
25.3
23.2
1970
6.8
0.7
1.4
13.3
2.4
1.0
25.6
24.6
aBased on 1970 emission factors.

 Miscellaneous sources not included.
                                     23

-------
                                    TABLE 5.   RECENT NATIONWIDE EMISSION ESTIMATES 1970-1977
                                            (10  metric  tons/yr,  expressed as TSP)
ro
Source Category
TRANSPORTATION
Highway vehicles
Nonhighway vehicles
STATIONARY FUEL COMBUSTION
Electric utilities
Industrial
Residential, commercial
and institutional
INDUSTRIAL PROCESSES
Chemicals
Petroleum refining
Metals
Mineral products
Oil and gas production
and marketing
Industrial organic
solvent use
Other processes
SOLID WASTE DISPOSAL
MISCELLANEOUS
Forest wildfires, and
managed burning
Agricultural burning
Coal refuse burning
Structural fires
Miscellaneous organic
solvent use
TOTALS:
1970
1.2
0.7
0.5
7.1
4.1
2.6

0.4
11.9
0.3
0.1
2.1
7.8

0

0
1.6
1.1
0.9

0.5
0.3
0.1
0

0
22.2
1971
1.1
0.7
0.4
6.6
4.0
2.2

0.4
11.3
0.2
0.1
1.9
7.4

0

0
1.7
0.8
1.1

0.7
0.2
0.1
0.1

0
20.9
1972
1.2
0.8
0.4
6.4
4.1
2.0

0.3
10.6
0.2
0.1
1.9
6.9

0

0
1.5
0.7
0.7

0.5
0.1
0
0.1

0
19.6
1973
1.2
0.8
0.4
6.5
4.4
1.8

0.3
10.3
0.2
0.1
2.1
6.4

0

0
1.5
0.6
0.6

0.4
0.1
0
0.1

0
19.2
1974
1.2
0.8
0.4
5.6
3.8
1.5

0.3
8.9
0.2
0.1
1.9
5.5

0

0
1.2
0.6
0.7

0.5
0.1
0
0.1

0
17.0
1975
1.1
0.8
0.3
5.0
3.7
1.1

0.2
6.5
0.2
0.1
1.4
3.7

0

0
1-1
0.5
0.6

0.4
0.1
0
0.1

0
13.7
1976
1.1
0.8
0.3
4.6
3.3
1.1

0.2
6.2
0.2
0.1
1.5
3.2

0

0
1.2
0.5
0.8

0.6
0.1
0
0.1

0
13.2
1977
1.1
0.8
0.3
4.8
3.4
1.2

0.2
5.4
0.2
0.1
1.3
2.7

0

0
1.1
0.4
0.7

0.5
0.1
0
0.1

0
12.4
    NOTE:  A zero in this table indicates emissions of less than 50,000 metric tons/yr.

-------
in emissions from different sources.   Some of these chemical  entities are
summarized in Table 6, which includes the results of rough emission estimates
from a number of reports.
     Mobile sources are the major emitters of airborne lead (88 percent of
                                                            29
total lead emissions), most of it as chlorides and bromides.     Vehicles are
also responsible for 38 percent of total anthropogenic hydrocarbon emissions,
some of which are particulate or form secondary particles.  Mobile sources
                                                         31
release less than 2 percent of the sulfur oxides emitted.
     Stationary fuel combustion sources emit particles containing a number of
substances of concern, including polycyclic organic matter (POM) and other
organic material, carbon (soot, which is mainly of health significance because
of its surface catalytic and adsorptive properties in relation to other pollu-
tants), and certain metals.  These sources also emit 81 percent of the national
sulfur oxide emissions,   most of which are assumed to be converted to particles.
Eighty percent of benzo(a)pyrene* emissions were estimated to come from coal
combustion, as compared to only 4 percent from stationary oil burning and 2
                            32
percent from mobile sources.    Coal combustion emissions are also distinguished
                                                                               33
by the fact that they include 88 percent of the nationwide beryllium emissions-
Stationary oil combustion, on the other hand, generates 83 percent of nickel
and 90 percent of vanadium emissions.  Therefore, it would appear that except
in the vicinity of atypical local sources, four metals can serve as virtual
identifying markers for combustion-linked airborne particles: lead for mobile
sources, beryllium for coal, and nickel and vanadium for oil.  Such source-
characteristic differences have been used in the chemical balance method to
*Benzo-a-pyrene (BaP) emissions are virtually all in the particulate state
after cooling to atmospheric temperature.
                                     25

-------
TABLE 6.   EMISSION  ESTIMATES  FOR MAJOR  SOURCES  OF  CERTAIN.AIRBORNE PARTICLES
Pollutant
          Smelting,
Mobile    metal-
sources   lurgical
Stationary
combustion,          Total  emissions
Coal   Oil   Other
Year
Tons
% of total
Particles3 4
a h
SO a'D 2
X
NO a 35
X
Hydrocarbons3' 59
e f
Benzo(a)pyrene ' 2
Metals9
Beryllium
Cadmium
Chromium
Copper
Manganese
Nickel
Lead 88-93
Titanium
Vanadium
emissions
36

13

<1

<1


3
43
68
84
74
11
2

1
of pollutant
32 2

60 13

19 7 22C

<1 <1 27d
80 4

88 6
52h
9 10J
7
11
83

83 101
9 90

1972

1972

1972

1972
1975

1970
1970
1970
1970
1970
1970
1970
1970
1970

19.8 x 106
c.
33.2 x 10°

24.6 x 106

27.8 x 106
978

170
2,200
17,000
14,000
18,000
7,300
230,000
52,800
20,000
*Ref. 3.4, Tables 4.1 and 4.2.
 Emitted chiefly as gases but with substantial conversion to secondary particles.
 .Other stationary fuel combustion.
 Evaporated solvents.
fValues stated by authors to be only approximate.
TRef. 41.
9Ref. 33, Table 1.
•Incineration of radiators and plated metal.
•Pigment production and use.
'•'Refractory production.
                                     26

-------
prepare an emission inventory for particles collected in the Los Angeles



area.5'35



     Noncombustion stationary source emissions have identifiable components



that are characteristic of the processes involved.   Thus, sulfuric acid plants



emit sulfuric acid mist; emissions from an open hearth furnace have been found



to be 89 percent iron oxide; particles from cement plants are chiefly calcium



oxide and calcium carbonate.   Smelters and other metallurgical processes emit



metal-containing particles, including 84 percent of the nation's total copper


          33
emissions;   particles with a high proportion of bio-organic materials are



emitted by such sources as flour mills, grain elevators, and paper/pulp mills;



and aerosols collected near the sea will include substantial fractions of sea



salts.



4.2  TRANSFORMATION AND TRANSPORT



     The makeup of a mixture of particles changes with time after emission.



Insofar as elapsed time is correlated with distance from the source, these



changes will be reflected in the changes with distance.  The most significant



transformations with time and distance are:  (1)  Condensation of vapors to



form secondary particles (which produces high concentrations, near the point



of emission, of particles less than 0.1 urn diameter); (2) particle coagulation



and growth (particle interactions occurring very rapidly to produce larger



particles from the condensation particles in the "accumulation mode" (0.1 to 2



urn) which persist in the atmosphere for days and for great distances); (3)



chemic.al transformations such as oxidation of sulfur oxides and photochemical



smog formation (occurring relatively slowly, so that products of these reactions



are higher at moderate distances than at the site of emission); and (4) fallout,
                                     27

-------
rainout, and other removal mechanisms (which cause a steady decrease in



particle mass and in mean particle diameter with increasing time and distance).

                                                                  •>c

     Long-range transport of sulfate and other inorganic compounds   as well


                                      37
as of polycyclic aromatic hydrocarbons   has been reported.  Even coarse



particles can be transported over long distances if they are injected above



the atmospheric mixing layer as by volcanoes or by air mass movements over dry



deserts.  These processes of aerosol transformation and transport are described


                                50
in detail in Airborne Particles.    Their net effect is that at increasing



distances from the source, the aerosol concentration decreases and is increasingly



dominated by accumulation mode particles with a mean diameter in the range of



0.4 to 1 urn, the nuclei having been removed by coagulation and the coarse



particles by sedimentation.



4.3  CONCENTRATIONS



4.3.1  Trends in Airborne Particle Pollution



     The routine episodes of high levels of visible smoke pollution which



characterized wintertime in some U.S.  cities before World War II no longer



occur.   The extensive replacement of coal as a home-heating fuel and the



enforcement of local smoke emission ordinances brought about gradual decreases



from the earlier high levels of urban smoke pollution, whether from coal or



other fuels.    Since the passage of the Clean Air Act of 1970 and promulga-

                                                                   o

tion of the ambient air quality standards for TSP (primary, 75 ug/m ) and



several other pollutants, particulate emissions are being further reduced.



Seventy-two percent of the sites monitored showed lower airborne particle



concentrations in 1976 than in 1970.   Improvement has been more marked in the



Northeast and Great Lakes regions than in the western areas of the country
                                     28

-------
where windblown dust is often a significant aerosol  constituent.   The general


pattern of change between 1970 and 1976 was little change at sites where 1970


concentrations were low and improvements at sites with higher 1970 concentrations.


     At 53 percent of the sites, concentrations in 1976 were greater than


those of 1975.  The areas showing this reversal of the previous downward trend


were generally in the Southeast, Midwest, and West.   These same areas had dry


soil conditions in 1976 due to the drought experienced by large areas of the


country at that time.  It has been suggested that the resultant increase in

                                                                           38
wind-blown dust was the reason for most of the increase in 1976 TSP levels.


Nationwide trends in total suspended particulate pollution are summarized for


1970-1977 in Table 5.


     The gradual decrease shown by TSP data gathered at 17 of the National Air


Surveillance Network (NASN) stations during the period 1966 to 1977 is shown


in Figure 3.


     The TSP curves of Figure 3 are not representative of every component of


airborne particulate matter.  A recent analysis of BaP trends during the


10-year period of 1966 to 1975 was based upon 34 urban (24 coke ovens) and 3


rural sites.  These trends for the urban sites (Figure 4) are consistent with


previous results indicating a steady decline of BaP.


     Table 7 shows the trends of atmospheric trace metal levels in U.S. urban


areas from 1965 to 1974.33


     Prominent among the metals showing a decline are vanadium, manganese, and


nickel.  Nationwide lead averages have declined since 1972 because of the


lower lead content of gasolines sold in recent years.
                                     29

-------
              HIGHEST VALUES:
             .227   182   306  213   183  151   144   121   158  119   100   123
     100
"I
§
111
o
o
o
0.
      90
      80
      70
      60  -
               LOWEST VALUES:
               25   22   25   21
             1966
                                                                        76
              Figure 3. TSP annual means at 17 urban NASN stations.
        NOTE:  TSP means (EPA data) from all of those stations for which
                data were available for each of the years 1966-1977 were
                used to derive the composite averages shown. Stations
                included were Grand Canyon Nat. Park, Honolulu, Chicago,
                Indianapolis, New Orleans. Arcadia Nat. Park, Baltimore,
                Detroit, Cleveland, Toledo, Youngstown, Pittsburgh, Houston,
                Norfolk, Shenandoah Nat. Park. Seattle, and Charleston.
                                        30

-------
m
4
 c

 UJ
 o
 u
    10
                                I      I
            90 PERCENT! LE
     OF QUARTERLY MEASUREMENTS
                     50 PERCENT)LE
        _   OF QUARTERLY MEASUREMENTS^
                                I
            1966   67
                        68
 69     70

TIME, year
                                           71
                                                 72    73
74
                                                                   75
     Figure 4. Benzolalpyrene seasonality and trends (1966 to 1975) in the 50th
     and 90th percentita for 34 NASN urban sites.63
                                   31

-------
                 TABLE 7.  TRENDS IN URBAN METAL CONCENTRATIONS AND
                                 THEIR POSSIBLE CAUSES33
        Metal
Observed trends
      Possible causes
Fuel-Combustion-Related Metals
        Beryllium
        Lead

        Nickel
        Titanium

        Vanadium
Industry-Related Metals
        Cadmium
        Chromium
        Cobalt
        Copper

        Iron


        Manganese
Unknown
Down last 5 years

Down
Up

Down

Down

No trend
Unknown
No trend

Down
Down
Lower lead content in gasolines
  after 1969
Reduction of Ni in residual oils
Increasing use of coal in
  electric utilities
Reduction of V in residual  oils
Controls in metal industry
  and improved incineration
  practices
Unknown
Contamination from hi-vol
  commutator
Improved incineration or
  waste burning practices,  fuel
  switching, controls in steel
  industry
Controls in metals industry
                                           32

-------
4.3.2  Comparative Exposure to Airborne Particles



4.3.2.1  Urban Versus Rural Exposures



     The generally higher exposures of urban residents to airborne particles



is one illustration of the impact of source proximity.  For example,  data from



the National Air Sampling Network in 1970 show that the mean annual average



benzo(a)pyrene concentration was 1.9 ng/m  (range 0.1 to 19.3) at 120 urban


                                                                31
stations versus 0.2 (range 0.1 to 0.4) for 20 nonurban stations.



     Such urban/rural differentials also exist for other constituents of



airborne particles.  The urban/suburban ratios for 22 trace elements  in air of



the Cleveland area are shown in Table 8.  The median ratio is 2.2 and in no



case did the suburban exceed the urban concentration.



     Other comparisons of urban and nonurban aerosol exposures and the apparent



effects of their differences on disease and death rates are presented and



discussed in Airborne Particles.



4.3.2.2  Indoor Versus Outdoor Residential Exposures



     Because there is continual air exchange between interiors and exteriors



of homes, outdoor aerosols—particularly the fine particles—will be included



among the indoor airborne particles.  However, this exchange also serves to



dissipate airborne particles generated by indoor sources.  Indoor sources



include combustion processes such as those of cigarettes, furnaces, fireplaces,



and stoves, and aerosol dispensers of consumer products.  Although indoor



concentrations of airborne particles, in the absence of smokers, are believed



to be usually less than those outdoors, some studies have found higher indoor



levels.  It is recognized that the current emphasis upon improved insulation



and weatherstripping for homes as an energy conservation measure could have



either beneficial or adverse effects on indoor air quality, depending on
                                     33

-------
TABLE 8.  RATIOS OF URBAN (U) TO SUBURBAN (S) CONCENTRATIONS IN AIR,
                     CLEVELAND, OHIO AREA36
Element  U/S
Element  U/S
Element
U/S
Antimony
Chloride
Beryllium
Chromium
Cobalt
Bismuth

6.9
6.5
6.1
5.6
3.4
3.3

Mercury
Iron
Cadmium
Sodium
Magnesium
Manganese
Calcium
3.0
2.8
2.5
2.4
2.4
2.2
2.0
Silicon, tin
Copper, vanadium
Aluminum
Zinc
Arsenic
Selenium
Bromide
1.8
1.8
1.7
1.6
1.4
1.3
1.2
                              X = 2.8
                             34

-------
whether, as a consequence, the indoor air is more or less polluted than the



outdoor air.


                    39-41
     Three documents      recently prepared for EPA specifically address the



problem of indoor air pollution, including indoor airborne particles.   Because



it is now known that indoor airborne particle concentrations sometimes are



higher than the limits allowed outdoors by the ambient air quality standard



while simultaneous outdoor concentrations are not, and because most individuals



are exposed for longer periods each day to indoor than to outdoor environments,



there is increasing concern as to the health impact of air quality in non-occupa-



tional indoor environments.  Accordingly, it has been recommended that further



monitoring of indoor air quality should be carried out and that epidemiological



studies of relationships between indoor air pollution and health effects be


          40
conducted.    Some health studies such as the Harvard Air Pollution Health


      52
Study,   are already incorporating indoor monitoring.



4.3.2.3  Environmental Versus Occupational Exposures



     In some occupational environments, the airborne particle concentration



greatly exceeds that of the external environment.  Examples are workplaces



such as textile and paper mills, steel works, smelters, metallurgical processing



plants, coke ovens, and mines.



     These high occupational exposures frequently involve exposure to higher



proportions of coarse particles than found in  environmental exposures.  They



are of some importance to evaluating effects of particles because they may



modify the response of an individual to airborne environmental pollution, and



because they are the source of much of our information concerning the health



effects of airborne particles.
                                     35

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                5.  EFFECTS OF AliBME PSASfflClES «WI WRN
5.1  DEPOSITION OF AIRBORNE  PARTICLES IN THE UING



     Adverse health effects  of airfronrae partiieiuilaibe matter ffioflHiow rd



of the  particles in the  respiratory tract,  lira imam., Dhe  mespfitnatery tbracit 
-------
of the human respiratory system.  The analysis also recommended that a second



particle size cut-point of <2.5 urn diameter be incorporated in the air sampling



devices, based upon considerations of the chemical composition and the size



distribution of airborne particles and on the predominant penetration of



particles <2.5 urn diameter into the gas-exchange region of the respiratory



tract.  This analysis pointed out that data collected in this size range could



be used in conjuction with epidemiological health parameters to refine an



inhaled particulate standard in the future.



5.2  HEALTH EFFECTS OF GENERAL AIRBORNE PARTICLE POLLUTION

                                                                3

     The present primary ambient air quality standard of 75 ug/m  for particulate



matter is required on an annual basis for the protection of public health.  In



the NAS document entitled Airborne Particles,   scientific information concerning



the health effects of airborne particles is described.   A more concise review


                                                                  43
by one of the contributors to that volume has also been published.    Tabular



summaries of evidence presented by different workers for particular health


                                                                      44
effects are provided in the statement by the American Thoracic Society   and



in Airborne Particles.



     Exposure to airborne particles as it actually occurs almost always is



accompanied by simultaneous exposure to other air pollutants and to other



environmental chemicals.  Although there is a tendency to regard these other



pollutants as merely obstructing the view of the scientist seeking to detect



the true effect of one particular pollutant, it must be kept in mind that the



other pollutants are probably modifying the "true" effect of the pollutant



studied and that the observed responses to the mixed but real exposure condi-



tions are the ones that are relevant to human health.  As an example, where
                                     37

-------
airborne particle pollution is coincident with sulfur oxides pollution, it is



desirable to evaluate the health effect of these pollutants jointly.



     There are indications that particles contribute more heavily than sulfur



dioxide does to the health effects of this combination.  For example, health



indices in London have improved during a period (1950-1970) in which particulate



pollution declined greatly along with a smaller reduction in sulfur dioxide.



In any case, there is good evidence that excessive airborne particle/SOp



pollution does cause illness and death, as well as increased prevalence,



incidence, and severity of respiratory disease and symptoms.  Incidence and



progression of bronchitis and emphysema have been especially clearly linked to



such pollution.  The effects are most evident in the oldest and youngest age



groups and in those people who are sick.   There is also evidence of delayed



appearance and of long-term persistence of the adverse effects of airborne



particle exposures.



     The fact that urban residence is associated with increased incidence of


      45
cancer   and that mutagenic (Ames-test positive) components are extractable


                             46-49
from urban airborne particles      suggest the possibility that airborne



particles are also to some degree carcinogenic.



     Table 9 provides estimated concentrations of particulates and sulfur


                               50
dioxide that may affect health.    Estimates of adverse health effects attribut-



able to sulfur dioxide, particulate sulfates, and total suspended particulates



(TSP) are presented for short-term and long-term exposures, respectively,  in



Tables 10 and 11, reproduced from Airborne Particles.     Additional  discussion



of the evidence concerning this dose-response relationship is  contained in



Airborne Particles.
                                     38

-------
                 TABLE 9.   HEALTH EFFECTS AND DOSE/RESPONSE RELATIONSHIPS  FOR  PARTICULATES AND SULFUR DIOXIDE
Averaging time
for pollution
measurements
24 hour





Weekly mean
6 Winter months
Annual



Place
London
New York
City
Chicago
New York
City
Birmingham
New York
London
Britain
Britain

Buffalo
Berlin
Particles,
mg/m3
2.00
0.75
0.50
6 COHSa
3 COHS
Not stated
0.145 (+?)
0.18-0.22
2.5 COHS
0.20
0.20
0.07
0.10
0.10
0.08
0.18
S02
mg/m3
1.04
0.71
0.50
0.50
0.70
0.70
0.286
0.026
0.52
0.40
0.20
0.09
0.10
0.12
0.45b
0.73C
Effect
Mortality
Mortality
Exacerbation of bronchitis
Mortality
Morbidity
Exacerbations of bronchitis
Increased prevalence of respiratory symptoms
Increased prevalence of respiratory symptoms
Mortality
Increased prevalence or incidence of
respiratory illness
Bronchitis sickness absence from work
Lower respiratory infection in
in children
Bronchitis prevalence
Respiratory symptoms and lung func-
tion in children
Mortality
Decreased lung function
Reference
88
97
97
94
93
89
95
95
92
87
101
90
96
99-100
102-103
91
^Coefficient of Haze Units.
Dmg S03/cm2/30 days.
cmg S03/100 cm2/day.

-------
              TABLE 10.  THRESHOLD ESTIMATES FOR ADVERSE HEALTH EFFECTS ATTRIBUTABLE TO SULFUR DIOXIDE,  PARTICULATE
                            SULFATE, AND TOTAL SUSPENDED PARTICULATES (TSP), SHORT-TERM EXPOSURES
Exoosure level . ua/m3
Adverse effect Research
human health approach
Mortality Epidemiology


Aggravation Epidemiology
of chronic
lung disease
Aggravation Epidemiology
of asthma
-t»
o
Aggravation of Epidemiology
combined
heart and
lung disease
Irritation of Epidemiology
respiratory
tract
Type of
estimate
Worst case
Least case
Best judgment
Worst case
Least case
Best judgment
Worst case
Least case
Best judgment

Worst case
Least case
Best judgment

Worst case
Least case
Point est

S02
30
500
300-400
119
500
365
23
>365
180-250

180
>365
365-500

340
340
340
Parti cu late
sulfate
No data
No data
No data
6
No effect
10
6
10
8-10

6
10-17
8-10

No data
No data
No data

TSP
250
500
250-300
100
>250
>250
75
>260
100

61
260
70-100

170
192
170
Safety margin, % contained
in primary standard
S02 std.
Duration 365 M9/1"3
24 hr
24 hr
24 hr
24 hr
24 hr
24 hr
24 hr
24 hr Less
24 hr

24hr
24hr Less
24 hr

2-3 days
2-3 days
2-3 days
0
37
0-9
0
37
0-37
0
than 100
0

0
than 100
0-37

0
0
0
Suspended
sulfates
(no std.)
No data
No data
No data
No data
No data
0
0
0
0

0
0
0

No data
No data
No data
TSP std.
260 ug/m3
0
92
0-15
0
Less than
0
0
Less than
0

0
Less than
0

0
0
0






100


100



100





Safety Margin =  Effects  threshold minus standard divided by standard x 100.

-------
TABLE 11.   THRESHOLD ESTIMATES FOR ADVERSE  HEALTH EFFECTS ATTRIBUTABLE TO SULFUR DIOXIDE
   PARTICULATE SULFATES,  AND TOTAL SUSPENDED PARTICULATES (TSP),  LONG-TERM EXPOSURES
Fxnosurp IPVP!. un/m3 	

Adverse effect Research
human health approach
Excess Epidemiology
mortality

Increase in Epidemiology
prevalence
of chronic
bronchitis
Increased fre- Epidemiology
quency or
severity of
acute respi-
ratory ill-
ness in
otherwise
healthy
families
Increase in Epidemiology
family ill-
ness during
influenza
epidemics

Type of
estimate
Worst case
Least case
Best judgment
Worst case
Least case
Best judgment

Worst case
Least case
Best judgment






Worst case
Least case
Best judgment




S02
120-198
250
250
50-90
404
95

91
200
91






106
250
106



Suspended
sulfate
No data
No data
No data
96
20
14

9
23
9






14
18
14




TSP
135
175
175
60-100
180
100

75
200
100






126
151
151



Duration,
years
Unknown
Unknown
Unknown
3
12
5

1
3
3






1
Unknown
3


Safety margin, % contained
in primary standard

S02 std.
80 ug/m3
50-148
212
212
0-12
405
19

14
250
14






33
212
33


suspended
sul fates
(no std.)
0
0
0
0
0
0

0
0
0






0
0
0



TSP std.
75 (jg/m3
80
133
133
0-33
140
33

0
167
33






68
101
101



-------
                                                    TABLE 11 (continued).

Adverse effect Research
human health approach
Increased Epidemiology
lower
respiratory
tract infec-
tions in asth-
matics
Subtle de- Epidemiology
crease in
ventilatory
function

Type of
estimate
Worst case
Least case
Best judgment



Worst case
Least case
Best judgment

Exposure level, pg/m3


S02
32
186
91



118-131
400-500
200


Suspended
sulfate
8
20
8



9
28
11



TSP
100
No
100



75-141
200
100

Safety margin, % contained
in primary standard

Duration,
years
Unknown
Unknown
Unknown



1
9
8-9


S02 std.
80 ug/m3
0
133
14



48-64
400-525
150

Suspended
sul fates
(no std.)
0
0
0



0
0
0


TSP std.
75 ug/m3
33
—
33



0-88
167
33

Safety Margin = Effects  threshold minus standard divided by standard x 100.

-------
     The severity of the health effects at any given airborne particle concen-
tration and the lowest pollution level requirecTto evoke significant adverse
health effects in the most sensitive populations are not eas-ily determined.
With so many factors determining exposures (Table 12) and with so many variables
influencing the response to a given exposure, any epidemiological study of
dose/response relationships must necessarily cope with uncertainties in both
the dose and response functions.  Therefore, there is some disagreement among
scientists as to the level at which airborne particle pollution becomes hazardous.
     The conclusions of many of the studies cited in Tables 9-11 have been
                            51                   ' '   " '•
questioned by Bennett et al.   (report prepared for the American Iron and—
Steel Institute) generally on the basis of the fact that one or more relevant
variables were uncontrolled.  The extent to which the correlations of health
effects with pollution indicated by such studies should be discredited must
remain a matter of judgment.  As is apparent from the above mentioned tabulation
of related variables, it can be expected that there will be some uncontrolled
variabTes in any epidemioTogic study of the health effects of air pollution.
     In addition to differing judgments as to the reliance that can be placed
on various studies with their varying levels of imperfection, there are also
sometimes differences of opinion as to how even such information as is avail-
able in a given study should be interpreted.
     In addition to variations in the design and interpretation of various
studies, other factors also undermine precise assessment of the epidemio-
logical evidence.  These include differences in methodology of airborne parti-
cle measurement; the possibility that health effects of exposure to air pollu-
tion may not appear or may persist until many years later;   the high mobility
of the Aaerican population that causes the enviroment of a given population to- w*
be only partially representative' of exposure of that population; the changing
                                     43

-------
                   TABLE 12.  VARIABLES  RELATED TO THE HEALTH EFFECTS OF AIRBORNE PARTICLES
     Exposure  factors
  Response factors
 Incidental factors
(Linkage factors )
  1.  Emissions  (kind  and  amount)
  2.  Synergistic  combinations
  3.  Topography
  4.  Climate, weather,  humidity
  5.  Seasonal and diurnal  changes
  6.  Place  of residence
  7.  Occupation
  8.  Duration of  exposure
  9.  Smoking (active  and  passive)
 10.  Physical activity
 11.  Breathing  mode (mouth or  nose)
1.  Temperature
2.  Physical condition
3.  Concurrent disease
4.  Nutritional status?
5.  Prior exposure
6.  Smoking history
7.  Age
 1.  Income
 2.  Education
 3.  Social class
 4.  Raceb
 5.  Sexb
 6.  Sanitation
 7.  Health insurance
 (Exp.  No.  6 - 10)
 (Exp.  No.  6 - 10)
 (Exp.  No.  6 - 10)
 (Exp.  No.  6 - 10)
 (Exp.  No.  7,9,10)
 (Resp. No. 2,3)
 (Resp. No. 2-4)
                         8. Access  to  medical  care   (Resp.  No.  2-4)
                                                      (Resp.  No.  3, Exp.  No. 6)
 9.  Population density
10.  Ageb
                                                      (Resp.  No.  2,5)
 Causal  exposure  or response  factors,  through which incidental factor
 may be  linked to health effects of air pollution.
3Somewhat uncertain.

-------
pattern and nature of air pollution; and changing social  and behavioral  pat-
terns which modify the impact of such variables as race,  sex, and smoking.
5.3  CONDITIONS WHICH MAY POTENTIATE HEALTH EFFECTS OF AIRBORNE PARTICLES
     Associations between the health effects of airborne  particles and corre-
lated variables can be categorized as three types.   A number of variables
(which we will call exposure factors) can be assumed to influence causally the
extent of exposure to airborne particle pollution;  variables of a second type
(response factors) directly 'influence the response of an  exposed person to a
given exposure; and variables of the third type (incidental  factors), while
correlated with pollution-related morbidity and mortality,  are assumed to be
non-causally linked to health effects through association with one or more of
the exposure or response factors.  Examples of some variables of each type are
shown in Table 12.
     The factors listed in Column 1 of Table 12 directly  determine the exposure
of a particular person to airborne particles.  They include the nature and
amount of pollutants emitted (No. 1-2), the geographic and atmospheric factors
that determine the extent to which pollutants will accumulate in or be removed
from the ambient air (No. 3-5), and the individual determinants that vary with
personal behavior or circumstance (No. 6-11).
     Some of these variables have been discussed in Sections 6.2 and 6.3.
     A second category of factors (Column 2) will determine the response of
each individual to a given level of airborne particle pollution.  These
response factors include external potentiating variables, such as temperature,
and physiological factors.
     Since low temperature alone can cause increased mortality in the elderly,
low temperature may increase the vulnerability of the old or sick to superimposed
                                     45

-------
air pollution exposure.  Studies have shown correlations of low temperature
with airway resistance and with symptoms exhibited during air pollution
                                50
episodes by bronchitis patients.    However, the extent to which the health
effects of temperature and of air pollution are independent or interacting is
not clear.
     The physiological factors named in Column 2 (items 2 through 7) all
relate to general physical condition and therefore to the capacity of the
individual to resist pollution-imposed stress.  There is abundant documentation
to show that people with concurrent respiratory disease are especially vulnerable
to air pollution and that, conversely, air pollution has decided impact on the
incidence of respiratory disease.  Many epidemiologic studies have taken
advantage of these relationships by monitoring the symptomatic reaction of
respiratory disease patients or the prevalence of respiratory disease during
air pollution episodes.  The quantitative aspects of these correlations,
especially the minimal level of air pollution likely to evoke an adverse
respiratory response, are still under debate.
     The different responses of different age groups to air pollution are also
well documented.  Although the increased vulnerability of the elderly to air
pollution may be in part related to increased cumulative exposures to prior
air pollution, it is presumably chiefly due to the decreased physical fitness
in older age groups with resultant increases in susceptibility both in disease
and to air pollution.  There is also evidence that children and especially
                                                  50
infants are also more vulnerable to air pollution.
     The third column of Table 12 lists some incidental factors:   variables
which appear to be correlated with pollution-related morbidity or mortality
                                     46

-------
but which are categorized here as being thus linked only indirectly,  through



one or more of the more direct exposure or response factors.   Possible



causal linkages are indicated in Column 4.  We have suggested that factors 1-5



can most reasonably be assumed to be linked through exposure factors  while



correlations of 6-10 with health effects seem more likely to be mediated by



response factors.



     The linkage of income level, for example, with pollution-related health



effects can reasonably be seen as due to the decreased occupational and residen-



tial exposures to air pollution which increased income can command.  Protec-



tive effects related to education, race, social class, and sex are also postu-



lated to be mediated chiefly through variations in exposure.   Such categoriza-



tion of race and sex as indirect or non-causal factors is somewhat uncertain.



However, there is no clear evidence of direct effects of these variables on



response to air pollution unmediated by other exposure or response factors.



5.4  HEALTH EFFECTS OF SPECIFIC CHEMICAL COMPOUNDS



     Airborne particles can be of health significance because some of their



chemical components are potentially toxic per se and also because less hazard-



ous particles, on interaction with other air pollutants or constituents, can



be transformed into more hazardous ones.



5.4.1  Intrinsically Injurious Particles



     A given inhaled particle may exert an adverse health effect either through



chronic local tissue damage by an insoluble particle deposited in the deep



lung or through solution and absorption of toxic components of the particle.



Detailed understanding of the active agents and mechanisms which produce the



adverse health effects is still largely non-existent.  However, several chemical
                                     47

-------
components of the ambient aerosol are known or suspected to be contributors to



these effects, either because of epidemiological observations or because of



other information available from experimental, occupational, or clinical



studies.



5.4.1.1  Fibers—Asbestos was first recognized as an occupational health



hazard responsible for the condition known as pulmonary asbestosis and later



as an occupational carcinogen when retrospective epidemiological studies



showed that occupational exposure is strongly associated with malignancy of



the lung, pleura, peritoneum, and gastrointestinal tract.   The effects typically



become manifest 20 or more years after exposure.  There is increasing evidence



that the general population may also suffer from inhalation exposure to asbestos,



since asbestos fibers are found in the ambient air and pulmonary asbestos



bodies are found in post-mortem examination of a large proportion of urban


          54
residents.     To protect the general population from exposure to high ambient



levels of asbestos, the EPA promulgated an emission standard in 1973 which



curtailed asbestos emissions from specific industries.   The projected total



reduction by 1977 from implementation of the standard was  93 percent.



5.4.1.2  Toxic Metals--Several metals which are known to be associated with



airborne particles and which are known to be toxic are of  concern.



     Lead is the air pollutant metal which, on a nationwide basis,  is believed



to pose the greatest hazard.   Airborne lead, at least 88 percent of which is



from combustion of leaded gasoline, has been associated with increased lead


                                                   29
concentrations in the blood of children and adults.     Primary exposure to



airborne lead occurs from inhalation, while secondary exposure may occur



through ingestion of foods and nonfood items which are contaminated by airborne



lead.   In people, lead affects the erythrocytes, the central and peripheral
                                     48

-------
nervous systems, soft tissues (kidney, liver), and bone.   The latter sequesters
95 percent of the body burden of lead.  Irreversible brain damage is one of
the observed effects of overt lead poisoning in infants and children.
     Biological effects which have been correlated with blood lead levels
include elevated erythrocyte protoporphyrin and mild anemia (15 to 40 ug of
lead/dl blood), peripheral nervous disorders and central  nervous system damage
(50 to 60 |jg/dl), and severe neuro-behavioral impairment (80 to 120 ug/dl),
sometimes resulting in convulsions and death.  The minimum "safe" level of
exposure to lead, as manifested by blood lead levels, is apparently variable
among individuals.   Formerly, blood lead concentrations less than 40 ug/dl
were considered harmless.   However, it has now been documented that hemato-
                                                                   29
logical effects do occur at lead concentrations as low as 10 ug/dl.
Association of relatively low (<40 ug/dl) blood lead levels with learning
deficits and with lower IQ scores has also been reported.    It is apparent
that current airborne lead levels may be having undetected but quite serious
effects on young urban residents.  (NASN data for 1974 indicate that lead
concentrations were less than 0.5 ug/m  at all nonurban stations but were 1.0
or higher at 32 percent of the urban stations.)  Concern about the effects of
airborne lead has prompted the EPA to propose and promulgate an air quality
standard for lead based on health considerations.   The present lead standard
         3
(1.5 ug/m  averaged over a calendar quarter) has as its goal a population mean
blood lead level of 15 ug/dl or less among children who do not receive signi-
ficant exposure to lead-based paints.  Such an average would ensure blood lead
levels not exceeding 30 |jg/dl for 99 percent of such children.
     Mercury is a highly toxic metal which occurs in air both as particles and
vapor.  Toxicity is due to accumulation in nerve tissue which ultimately can
                                     49

-------
lead to insomnia, loss of memory, and severe neurobehavioral and personality



changes.  Children and the fetus are the most susceptible to mercury poisoning.



Release of mercury into the atmosphere from natural sources far outweighs the  .



release from the major man-made source, coal combustion.  On the average, the



ambient concentrations in the large industrial cities are well below the 1



ug/m  level, and toxic airborne exposures are unlikely except in the vicinity



of point sources.



     Cadmium accumulates in the body, especially in the kidney, where it has a



very long biological half-life.  Cadmium dust, when inhaled at high concentra-



tions, can lead to severe kidney and lung damage.  In view of the cumulative



nature of this metal and of the resulting health effects, it seems appropriate



to minimize the exposure of the general population.  The average concentration

                                                             o

in the ambient air is extremely low (approximately 0.002 |jg/m ) but may reach


                  3                                                57
levels of 0.3 ug/m  near industrial point sources such as smelters.     The-EPA



is presently evaluating what type of regulatory action, if any, is needed to



protect public health.



     Arsenic is emitted mainly by metal smelters, coal combustion facilities,



and the pesticide industry.   In air, arsenic occurs mainly in particulate



form.   Approximately 80 percent of absorbed arsenic is retained and widely



distributed in the tissues.   Arsenic may cause both acute and chronic poisoning,



but acute poisoning is rare.   Both subacute and chronic poisoning can result



from polluted air.   Effects of arsenic poisoning include skin and mucous



membrane abnormalities, gastrointestinal  and nervous symptoms, and disorders



of the circulatory system and the liver.   In spite of the epidemiological



association between exposure to arsenic and cancer of the skin, lungs,  and
                                     50

-------
liver, a suitable animal model has not been developed that demonstrates carci-

nogenicity of arsenic.   The epidemiologic studies involved exposure not only

to arsenic compounds but to high levels of sulfur dioxide (at smelters) and of

other heavy metals (at power plants).   NASN reported annual  average con-

centrations of arsenic in air ranging (in 1964) from nondetectable levels to

         3                                      3
0.75 mg/m , with an overall average of 0.02 ug/m .   The EPA is presently
                                                         CO
considering listing arsenic as a hazardous air pollutant.

     Beryllium is considered to be one of the most toxic metals in industrial

use.  The major emission source is coal combustion (88 percent of total emis-

sions).   All acute cases of beryllium disease have been associated with beryl-

lium either in occupational settings or in communities adjacent to point

sources.  The Committee on Toxicology of the National Academy of Sciences

concluded that a 30-day average concentration of 0.01 ug/m  in ambient air was

a proven safe level since no cases of beryllium poisoning from exposures at or

                               59
below that level were reported.    Beryllium is also reported to be carcino-

genic,   although the point is presently being contested.  Quarterly composite

NASN data for 1970-1975 show that the beryllium concentrations at both urban
                                                                3
and non-urban sites were below the detectable limit (0.0008 ug/m ).

     General urban atmospheric pollution with manganese is occurring as man-

ganese-containing additives are substituted for lead antiknock compounds.

In view of the pneumonitis and increased mortality from pneumonia which have

in the past been caused by manganese pollution in the vicinity of point
        CO
sources,   it will be important to monitor closely and control within safe

limits any future increase in particulate manganese.

     In summary, it can be said that of the toxic metals in airborne particles,

only lead is present in the urban general atmosphere at average concentrations
                                     51

-------
which may be hazardous.  Other toxic metals (including manganese, mercury,

cadmium, arsenic, and beryllium) are potential health hazards in the vicinity

of point source emissions.

5.4.1.3  Polycyclic Organic Matter (POM)--These compounds are adsorbed on
                  32
airborne particles   and are included in the "benzene soluble organic fraction".

The major human health concern relating to POM is the possible causation of

cancer by one or more members of this group of organic compounds.  POM is

associated with airborne particles emitted from both mobile and stationary

sources (such as diesel engines and coke ovens) during the combustion or

pyrolysis of hydrocarbons.

     A detailed assessment of the health effects of POM has been recently
         CO
prepared.    Occupational studies have clearly demonstrated an increase in

lung cancer with exposure to POM.  Epidemiological studies in community set-

tings have demonstrated, after correction for smoking, that urban residents

have a twofold greater risk for the development of lung cancer as compared  to

residents of rural environments.  It is assumed that POM contributes to some

unknown fraction of this increase.  It is believed that the risk of lung

cancer development by exposure to POM is real, that the magnitude of that risk

to the general population cannot be accurately determined based on our current

knowledge, that it is almost certainly much less than the lung cancer risk

associated with cigarette smoking, but that in real-life situations with

concurrent exposures to cigarette smoking and other foreign chemicals, the
*BaP is the POM for which the most information concerning emissions is available.
It is used as an indicator of the presence and concentration of POM as a
class.  However, the validity of this use of BaP as a surrogate for POM is
uncertain.
                                     52

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                                                    63
absolute risk of POM exposure is probably magnified.     Urban trend data for a



specific POM (benzo(a)pyrene)* show an 80 percent decline from 1966 to 1975.



5.4.1.4  Sulfur Dioxide/Sulfuric Acid/Sulfate Salts—In addition to the survey



of the physiological effects of airborne sulfur compounds given in Airborne



Particles,   two other reviews of this subject have been recently published.   '



Therefore, the effects of these substances will be only briefly discussed



here.  The reader should consult the cited reviews for more detail.



     Epidemiological evidence concerning the toxicity of sulfur oxides and



sulfates is complicated by the concurrent presence of other particulate matter



and other pollutants.  However, it is clear that high TSP levels coupled with



high sulfur oxides can lead to sickness and fatalities.  Observed increases in



morbidity and mortality during air pollution episodes are discussed below and



in the various reviews cited.



     The source of most of the particulate sulfur compounds is fossil fuel



combustion, sulfur dioxide being the major form emitted.  This gas is quite



soluble in water and occurs as sulfurous acid in aqueous airborne particles.



It is also oxidized to sulfuric acid, which in turn is neutralized to some



extent, forming neutral sulfates.



     Much of the evidence suggesting that the sulfate aerosol contributes to



the  health effects of air pollution is based on experimental work with animals.



In various studies at exposure levels of 1000 ug/m  or less, sulfuric acid has



not  been shown to cause increased pulmonary airflow resistence, chronic changes



in liver and lungs,  kidney, and pancreas (in combination with other pollutants),



decreased carbon monoxide diffusion capacity, and cellular changes in the



bronchial mucosa.  Because it  is a strong acid, sulfuric acid may  be expected
                                     53

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to have a greater irritant effect on respiratory mucosa than do sulfate salts.

However, because of the presence of ammonia in the respiratory tract, much or

all of the inhaled sulfuric acid may be neutralized before contacting the

mucosa.  The extent to which such neutralization actually occurs will depend

on several other factors, including particle size.  As noted above, ambient

sulfuric acid has been shown to persist even in the presence of more than
                                           Q
enough ammonia for complete neutralization.

     Animal experiments have shown that neutral sulfate salts are also respi-

ratory irritants to varying degrees, with zinc sulfate and zinc ammonium

sulfate being highly irritating and ferric and manganese sulfates being inert.

There has been little research on the effect of sulfate salts on humans.

5.4.1.5  Other Particles—A number of other types of particles can be assumed

to contribute to the health impact of airborne particles.

     Nitric acid vapor and particulate nitrates are formed, to some extent,

from nitric oxide in a manner analogous to the formation of sulfuric acid and

particulate sulfates from sulfur dioxide.   Orel and Seinfeld,   in a recent

report, compare the formation, sizes, and concentrations of ambient sulfate

and nitrate particles.   Unlike sulfuric acid, the nitric acid that is formed

tends to remain in the gas phase, although it may be an important component of

acidic precipitation.     Although it is recognized that respirable nitrates

may be of health significance, little information is available as to their

health effects.

     Cigarettes are the source of much of the airborne particle exposures for

smokers and of some for non-smokers, especially in indoor environments.

Because cigarette smoke particles are small, contain adsorbed pyrolysis pro-

ducts known to be carcinogenic, are deposited and remain for extended periods
                                     54

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in the smokers'  lungs, and are deliberately or involuntarily inhaled at high



concentrations,  they represent a special  and extreme case of hazardous airborne



particles.   The  greater susceptibility of smokers to the adverse health effects



of airborne particles (e.g., asbestos) and to air pollution episodes is well



documented.  Although one cannot assume that all  of the harmful  factors in



cigarette smoke  are associated with particles, a  substantial fraction of them



probably is.



5.4.2  Chemical  Interactions with Other Pollutants



     A recent report examines the role of solid/gas interactions in air pollu-



tion.    Particle interactions with other air pollutants involve both surface



adsorption of pollutant gases and surface-catalyzed chemical reactions.  These



processes can produce modified particles which may be either more or less



hazardous than the original ones.



5.4.2.1  Adsorption—Because many airborne particles incorporate substances



which are surface active and because they have large surface areas relative to



their mass, these particles are effective sorbents of other air pollutants.



Most POM, for example, which is normally emitted  as hot vapors,  condenses into


                            32
fine particles upon cooling.    Particles can convey into the non-ciliated



portion of the lung water-soluble toxic substances that would otherwise have

                                                              CO CO

been largely exhaled or removed in the upper respiratory tract  '    An analy-



sis of the southern California aerosol on four successive days showed that the



most abundant form of carbon in the particles (50 percent) was elemental



carbon.    Because of their adsorptive efficiency, fine carbon particles can



synergistically increase the effects of other pollutants. The co-carcinogenic



effect of benzo(a)pyrene has been shown experimentally to be potentiated by



the presence of carbon particles with which, in automotive emissions, it is
                                     55

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normally associated.   Benzo(a)pyrene   and other polycyclic organic matter
adsorbed on soot have been shown to be released from the particles by body
fluids.
5.4.2.2  Surface Chemical Reactions—Particles participate in various chemical
reactions with atmospheric gases.  Preeminent, perhaps, are the solution by
water droplets of gases and the aggregation of other particles with these
water droplets, establishing an aqueous reaction medium where chemical trans-
formations occur.  Sulfur dioxide is oxidized to sulfuric acid in the presence
of aqueous atmospheric aerosol.  The rate of this reaction is dependent on
temperature, pH, and the presence of catalytic trace elements.  Soluble salts
of ferrous iron, manganese, and vanadium are among those which catalyze the
oxidation of sulfur dioxide.  In a further particle/gas interaction, the
sulfuric acid droplets can then be neutralized by atmospheric ammonia.
     There are epidemiological and experimental indications that adverse
health effects of sulfur dioxide at concentrations normally present in the
ambient air are largely or entirely dependent on the coincidental presence of
particles.     The interaction causing this synergism is presumably due both to
the particle-catalyzed oxidation of sulfur dioxide in the environment and to
sulfur dioxide oxidation which occurs after dry-particle transport of the
adsorbed gas into the warm, humid atmosphere of the respiratory tract.  Syner-
gistic effects of sulfur-dioxide and particle exposures are discussed in
                   50
Airborne Particles.    Sulfur dioxide has also been reported to increase
                                                                      72
synergistically the carcinogenic activity of benzo(a)pyrene particles.
     Other aspects of particle surface chemistry are suggested by the report
                 73
of Linton et a!.;   for example, in coal fly ash, numerous elements including
lead, chromium, manganese, sulfur, iron, potassium, sodium, lithium, and
                                     56

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vanadium have strongly enhanced surface concentrations and Teachabilities

relative to those of the glassy particle matrix.   Lead, for example,  while

present at a concentration of 0.06 percent on the basis of bulk analysis, had

a surface concentration of 4 percent and was highly Teachable.   Preliminary

studies also established the surface predominance of lead, bromine,  chlorine,

sulfur, phosphorus, potassium, and sodium in automobile exhaust particles.

The non-uniformity was attributed to volatilization-condensation processes.

Since it is the particle surface which contacts and is extracted by body

fluids upon ingestion or inhalation, this non-uniformity will have the effect

of increasing the effective dose resulting from inhalation of airborne parti-

cles.

5.5  HEALTH COST ANALYSES

     With regard to the development of recommended guidelines for the protec-

tion of public health, there has been much discussion relating to the desir-

ability and magnitude of safety factors, the desirability of regulating parti-

cular types or sizes of particles, the extent to which air quality standards

should be designed to protect especially vulnerable groups,* and to the economic

benefits to be derived.  To provide data related to the latter consideration

(cost/benefit trade-offs), a number of studies have attempted to estimate the

                                           74
costs of air pollution.  A report by Herman   presents a survey of studies

published between 1967 and 1977 concerning the health costs of air pollution.

It concludes that sulfur oxides and particles are a more serious threat to

health than are other
*Such groups might include the aged, the sick, children, those with above-
 average levels of outdoor activity, and that 10 percent of the healthy popula-
 tion (Airborne Particles) which is reported to exhibit exaggerated responses
 to sulfur dioxide exposure.    The Clean Air Act requires protection of
 such susceptible groups.
                                     57

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air pollutants.  It was stated that "no study surveyed for this report dissents
directly or indirectly from the conclusion that sulfur oxides and particulate
matter impose the greatest health costs on the American population."  A tabular
comparison of health cost studies was given in the report by Herman.  Those
parts of the table summarizing studies which were concerned mainly with sulfur
oxide and particle pollution are presented here in Table 13.  Estimates from
the various studies of the health penalty imposed by these pollutants are
given in the eighth row of the table.
     Because such studies attempt to assign monetary valuations to essentially
indeterminate costs such as lost earnings as well as to more tangible expenses
such as medical costs, and because they usually do not include such real but
non-quantifiable effects as the psychic and emotional penalties of disease and
premature death, they are admittedly only coarse approximations.
5.6  DEFICIENCIES IN THE SCIENTIFIC DATA BASE
     Much needed information concerning the effects of airborne particles on
public health and welfare is not available.   A recent report by the Inhalable
Particles Research Committee   outlines the most urgent research needs.  These
include:   (1)  definitive animal toxicology experiments establishing acute and
chronic effects resulting from individual and multiple pollutant exposures not
admissible with human subjects, (2) comprehensive clinical studies of physio-
logical responses in human volunteers to low level individual and multiple
pollutant exposures, and (3) expanded collection and evaluation of epidemio-
logical data in communities selected so that relationships between particle
pollution and observed health effects can be described.
                                     58

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                   TABLE 13.  COMPARISON OF
Reference
Year(s) studied
Pollutant(s)
Illness
Death
Measurement
of
pollutant(s)
Dose-response
function
Population
at risk
Results:
addi tional
cases of
disease
or death
Results:
do' 1 ar
estimate( s)
DM ini tion
of estimate
Stu&P Of
estimate
72
Lave and Seskin
1963
sulfates
participates
respiratory disease,
cardiovascular disease,
and cancer
yes
no measurement;
50% improvement
assumed
inferred frum previous
epidemiological
studies
nationwide
50% abatement would
cut i 1 Inpss and death
from respiratory dis-
ease 25%, cancer 15%,
and cardiovascular
disease 10%"
Savings' respi ratory-
S1.222M; canc£r-$390M;
cardiovascular-$468M
medical costs and
lost earnings
nationwide
73
Jaksch and Stoevener
1969-1970
particulates
respiratory diseases,
allergies, skin diseases,
circulatory, digestive,
genitourinary disorders,
eye diseases
no
18 Portland monitors;
24-hour readings every
4 days; isopleths drawn,
values assigned to people
taking account of differ-
ent exposures due to
home, work, travel
regression analysis: age,
sex. marital status, no.
in household, race,
fitness, drinking,
smnking, occupation,
humirti ty , temperature ,
1 pol lution measure
?,500 Portland residents
20 micrograms per cubic
meter increase to 80
microgram particulate
levels had "minimal
effect" on cost of
outpatient visits
addi tional 3. 5C per
visit or $1000 per year
medical costs only
ISO, 000 members of
Mi ser-Permanenle
Mt-dica 1 Care Program in
Portland , Oregon
74
Waddell
1970
sul fur dioxide,
particulates, sulfates
irritation symptoms,
heart and lung (elderly),
asthma, acute lower
respiratory, chronic
bronchitis
yes
used the average
26% improvement in
pol lution levels
reported for 1970
death: 26% abatement
reduces death rate 2.33%
(estimated from Lave &
Seskin 50%-4.5% relation);
i 1 1 ness: reductions
estimated from CHESS
data
Irritation-50M, asthma-4M,
heart & lung-4M, acute
lower-50M, ch. bronch.-6M
i 1 1 ness: reductions:
irritation: 75-100%,
heart and lung: 10-30%,
others: 10-50%
S0.7-4.4B death:--
$0.9-3.26 illness--
savings if 26% reduction
in air pol 1 ution
i 1 Iness and death:
medical costs and lost
earnings
approximately 1S5H people
-urban population
nationwide
75
Finklea et a! .
1970
sulfates
heart and lung disease,
lower respiratory (LRD)
disease (chi Idren) ,
chronic respiratory
disease (CRD), asthma
yes
NASN sulfate readings
extrapolated to four
types of population
density (less than 2500
per city to more than
2M); 1-24 monitors per
type in each of 9 regions
dose-response functions
constructed for acid
sulfate aerosols from a
number of studies, includ-
ing CHESS; "best judgment"
rather than mathematical
fit used
heart and lung--3.7M,
4. 1M asthmatics, 35. 2M
children. 137. 4M--
premature death
13,000 excess deaths,
44. 7M aggravated heart and
attacks, 0.376M excess LRO
0.565M nonsmoker excess
CRO symptoms
—
--
Nat ionwide
76
Johnson et al. (EPA)
.1970
sul fur dioxide,
sulfates, particulates
Acute resp. --influenza ,
a. bronchi ti s , pneumonia
Chronic resp. --emphysema, c.
bronchitis,, bronchiecstasis,
c. interstitial pneumonia
no
anrva 1 SMSA averages
of each pol lutant;
168 SMSAs; center-city
NASN readings.
excess disease rates
from 9 CHESS study
communities appl ied
to SMSAs with same
combi nat ion a^d
levels of pol lutants
48. 8N center-city res.
Acute: 1,901 .000 rases
(adult--17-65);
5,863.000 cases (childreO
Chronic: 679.000 (adult)
Acute: S4/5. 9 n.i 1 1 ion
Chronic: $104.6 mil 1 ion
medic a co>ts . lost
earnings , house*' fe
disability, lost school
IC'8 center c i t >es
48. S mi 11 ion people
59

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 HEALTH  COST  STUDIES74
77
Liu and Yu
1970
sulfur dioxide,
participates
yes: not specified
yes
S02:
19G8-70 SO, averages
in 40 SMSA$ where average
exceeded 25 micrograms per
cubic meter; one per SMSA,
particulates: 1968-70
averages from same SMSAs
illness-calculated from
lf>2 CHISS observations
using "Monte Carlo" method
death-reqress ion anal>sis:
^ cue? *b, income, educa-
tion, ^ weather variables
explains 82% of death rate
78
Carpenter et al .
1972
sulfur dioxide,
particulates
respiratory and
heart disease
no
pollutant measurements
used to classify neighbor-
hoods according to three
levels of SO- and partic-
particulates in Allegheny
County (encompasses
Pittsburgh)
regression analysis: sex.
ape , occupation , smoki ng ,
neighborhood median
income, how hospital bill
paid, whether surgery
performed. % occupancy
of hospital , race. 3
measures of pollution
5
Gregor
1968-1972
sulfur dioxide,
particulates
no
yes
sulfur dioxide: 5-year
mean of annual averages
measured at 5-49 stations;
particulates: 5-year mean
of annual averages,
42-47 stations; means for
each census tract in
Allegheny Co. (Pittsburgh)
regression analysis:
% adults with high school
education, population
density, precipitation,
temperature, 2 pollution
measures
79
Heintz, Hershaft, Horak
1973
sulfur dioxide, sulfate
compounds, particulates
same as Waddel 1
same as Waddel 1
same as Waddel 1:
no measurement;
assumed 26% improvement
in pol lution level s
same as Waddel 1 , see
"Results" below
80
Lave and Seskin
1979 (projected)
sul fur .oxides,
particulates
al) illness
yes
smallest SO reading.
ari thmet ic Sean of
participate readings
taken biweekly in 1960-1961
and 1969 in each of
112-117 SMSAs
regression equation:
2 pollution variables.
% of people 65 and over,
income, population density,
% non-white explains
83% of the death rate
 40 S^SAs. 1pp.  64 million  32,600 patients  in 28
(1970 Statistical Abstract) hospitals
app. 950,000 Allegheny
County residents
                                                                      same  as Waddell
SO, and paM iculatf s
account for- apg. 1% of
total death rate
S0? accounts for 7% of
excess illness rate.
participates ?8%
deMh-41.930.6 mi 11 inn
iIlness-1249.5 million
i 1 ! ness-medical costs .
lost earnings, "psychic"
costs
appro* i mat P '/ 64 T- i H ion
people in 40 SMSAs
133.600 additional
hospital-days, plus
1-3.5 days longer in
hospital suffered by
residents of more
polluted neighborhoods
$9.9 mi 11 ion extra
hospital ization costs
in 1972
medical costs only
32.600 rpvpiratory and
hpart hospital patients
in Al iegheny County
1% SO,, and particulate
reduction in 1968-1972
would have reduced death
rate .01-. 06/100. 000 for
younger than 45; .1-.5,
45-64; .3-12.6. 65*
potential sav ing of
17. 5 mi 11 ion per year
"wi 1 ) inqnes^ to pav"-
*200 for 1/1000 reduction
in annual chance of dying
Allegheny County
(Pittsburgh area)
residents
26% ihatemeiil '-educes
death rate 2.33%
i 1 Iness savings:
see Waddel 1
dealh-$3.2 bi U ion
i 1 lnes-»-$C S hi 11 ion:
savings it 26% reriuct-
tion in a>r pollution
h.iddei 1 f iqurps updated
tn account for rising
wages, population
increase, etc
appro* imatelv 155
mi 1 1 i on- urban
popul^t ion nat ionwide
tPA-prnjected ^o and 88%
levels "t particulates
and su'fur oxiaes bs 19~9
would reduce U.S. death
and iMness
V.b. & t; i T! i.in > -u - ;M)-
1079 ("V -if I'.'/: i- ••
medica 1 co^l s p'~c JVL te
tc 19'9. i1«^cciinteri ^t
medical L.-st^ . "^i^t
earninqs. and nuuse*' f
equivalent earnings
nationwide
°«,
e

                                                      60

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     To support the health oriented research there is need for more detailed
characterization of particulates - sizes,  quantities, composition,  and distri-
bution—plus a better understanding of the physical  and chemical  transforma-
tions of particles between their emission  and their deposition in lungs and on
soils, foilage, etc.   Finally,  fundamental to all  the above research is the
refinement of techniques capable of measuring those properties of particulate
pollution that emerge as important.
                                     61

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              6.  EFFECTS OF PARTICULATE MATTER ON PUBLIC WELFARE







     The effects of airborne particles on public welfare consist, chiefly,  of



adverse effects on plants, animals, and soils; on materials; on visibility  and



other aesthetic conditions; on meteorological conditions; and possibly on



climate.                                                       ;           .



6.1  ECOLOGICAL EFFECTS



     Airborne particles can cause injury to vegetation.   The type of injury



which may occur is dependent on particle size and composition.   Excessive



deposits of dust particles, such as those from cement plants, can cause crusts



to form on the leaves, twigs, and flowers of plants if moisture is present.



The presence of the crust prevents sunlight from reaching the leaves, thus



inhibiting the process of photosynthesis.   Studies of these phenomena have



been made in the vicinities of dust-emitting cement kilns and are extensively



reviewed in Airborne Particles.



     The stomata in the leaves may become clogged if they are on the upper



leaf surface.   Depending on their chemical composition,  dusts can cause direct



injury to leaves and flowers.  Particles containing fluorides,  magnesium



oxides, and soot-containing particles have been shown to cause  vegetational



injury.



     Fine particulate matter (ambient aerosol) is the principal conveyer of



acid in the atmosphere.    The effects of acidic precipitation  on ecosystems



are briefly reviewed in Airborne Particles   and more extensively in the



numerous contributions to a Symposium on Acid Precipitation.    Acidic



precipitation, containing sulfuric, nitric, and hydrochloric acids, can
                                     62

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severely inhibit the growth and health of trees and other plants  both  by



direct contact and by acidification of the soil.   The effects  on  domestic



plants can have substantial agricultural    as well as natural  ecological



impact.



     Several analyses of the effects of acidic precipitation on specific


                                                       78
ecosystems have been presented.  For example, Schofield   estimated that fish



populations have been adversely affected by acidification in approximately 75



percent of the high-elevation Adirondack lakes.  Some of these lakes are now



so acidic that fish cannot survive.



     Toxic material in airborne particles can also injure terrestrial  animals.



An example is the fluoride poisoning which has been observed in cattle and


                                                                       79
horses grazing near point sources (such as aluminum processing plants).



Lead poisoning of wildlife, domestic animals, and aquatic organisms is


                                          29
reviewed in Air Quality Criteria for Lead.



6.2  EFFECTS ON MATERIALS



     The damaging effects of particulate matter on materials are extensively



reviewed in Airborne Particles.    These effects are due not only to the



attack of chemically active components such as sulfuric and nitric acids but



also to the action of adsorbed or dissolved gaseous pollutants, including



sulfur oxides, nitrogen oxides, hydrogen sulfide, ammonia, and ozone.   The



effects include corrosion of metals, deterioration and discoloration of paint,



erosion of stone and masonry, fading and embrittlement of plastics, fading and



weakening of textiles, and peeling of asphalt surfaces.  An estimate of 3.8



billion dollars as the annual cost of such damage is cited. This estimate did



not include costs associated with surface soiling.
                                     63

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                                                                     80
     Using an economic model of household behavior, Watson and Jaksch



estimated welfare gain from less soiling using empirical estimation of a



physical soiling function, a behavioral frequency-of-cleaning function, and



total current expenditures for cleaning derived from two earlier studies.   A



behavioral frequency-of-cleaning function and estimates of total cleaning



expenditure were obtained by analyzing data gathered for Philadelphia, including



data from a cross section survey of 1090 households.  Although the results are



limited by the empirical data, this preliminary analysis for 123 SMSA's* found



that the benefits of less soiling when the federal primary particulate standard



is attained would range from $537 to $3816 million per year in 1971 dollars.



When soiling benefits and health and materials benefits (obtained from other



studies) were combined and compared with control costs, Watson and Jaksch



found tentatively that the secondary annual particulate target (60 micrograms



per cubic meter) would provide the largest net benefit.



6.3  ATMOSPHERIC AND CLIMATIC EFFECTS



     Absorption and scattering of sunlight by aerosol particles cause decreased



visibility and decreased intensity of the sunlight which reaches the ground.



It has been estimated that such scattering and absorption are responsible for



a radiation loss of 20 percent in parts of the rural midwest, an effect of



potentially great agricultural impact.  Absorption and reflection of sunlight



by the aerosol and by particle-enhanced cloud cover may also be responsible,



to some degree, for the recent cooling trends in regional and global climate.


Although the significance of this effect on climate is still uncertain, it may



prove to be of importance.
^Standard Metropolitan Statistical Areas.
                                     64

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     Airborne particles influence cloud formation and rainfall  by serving as
condensation nuclei.   The effect is well documented in areas downwind from
urban and industrial  locations.   It is estimated that many urban centers cause
an increase in downwind precipitation of 5 to 15 percent.
     These effects of airborne particles on visibility,  insolation,  cloud
cover, global temperature, and precipitation are discussed and  documented in
detail in Airborne Particles.
6.4  AESTHETIC EFFECTS
     Aesthetic and nuisance effects of airborne particles  include such phenom-
ena as the general soiling of clothing, buildings, and other exposed surfaces,
the association of unpleasant odors with airborne particles,   the obscuration
of scenic vistas, the cultural loss incurred by degradation of  exposed archi-
tectural and historical artifacts, and the diminished opportunities  for pleasant
outdoor activity, including recreational enjoyment of natural ecosystems.
     Although the costs of these effects are not normally  quantifiable, it is
apparent that they are significant and are a major factor  in public  assessment
                                                     81
of the undesirability of airborne particle pollution.   The 1969 criteria
                                                      81
document, Air Quality Criteria for Particulate Matter,  presented the conclu-
sion that total suspended particulate (TSP) levels above 70 mg/m  (annual
geometric mean) evoke public awareness and/or concern.
6.5  Trends in Visibility
     Recent studies suggest that fine particulate sulfates may be a principal
cause of visibility reduction associated with air pollution in areas as
                       82                  83                   84
diverse as Los Angeles,   the eastern U.S.,   and the southwest.
                                     65

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Widespread atmospheric hazes observed throughout the eastern U.S.  are apparently


                                                          83
increasing with regional SO  emissions.   Trijonis and Yuan   analyzed visibility/
                           A


pollution relationships at 12 northeastern sites.  They found that visibility



is not substantially better in non-urban areas than in metropolitan areas of



the northeast, averaging only 9 to 12 miles.   From the middle 1950's to the



early 1970's, visibility exhibited only slight downward trends in  large



metropolition areas but decreased on the order of 10 to 40 percent at



surburban and nonurban locations.   Over the same period, visual  range declined



remarkably during the third calender quarter relative to other seasons, making



the summer months the worst season for visibility.   Examination  of meteoro-



logical trends at some sites indicates a slight decrease in maximum daily



average temperature and a slight increase in humidity, but these are not



sufficient to account for the visibility trends.   Additional work  is needed to



determine whether the visibility changes influenced the climate  trends.
                                     66

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7.   REFERENCES

1.    Whitby K. T., R. B. Husar, and B. Y. H. Liu.  The aerosol size distribution
     of Los Angeles smog.  Jji:  Aerosols and Atmospheric Chemistry.  G. M.
     Hidy, ed., Academic Press, New York, 1972.  pp. 237-264.

2.    Bockian, A. H., and M. A. Hostak.  A comparison of filterable mass and
     light scattering of photochemically produced aerosols.  J. Colloid Inter-
     face Sci. 39:90-93, 1972.

3.    Lee, R. E., Jr., and J. Wagman.  A sampling anomaly in the determination
     of atmospheric sulfate concentration.  J. Am. Ind. Hyg. Assoc. 27:266-271,
     1966.

4.    Spicer, C. W., and P. M. Schumacher.   Interferences in sampling atmospheric
     particulate nitrate.  Atmos. Environ.  11-873-876, 1977.

5.    Wells, R. M.  Total Suspended Particulates:  Review and Analysis.
     EPA-600/2-76-092, U.S. Environmental Protection Agency, Research  Triangle
     Park, NC, April 1976.

6.    Office of Air Quality Planning and Standards.  National Air Quality  and
     Emissions Trends Report, 1976.   EPA-450/1-76-002, U.S. Environmental
     Protection Agency, Research Triangle Park, NC, December 1977.

7.    Fair, D. H.,  R. C. Rhodes, E. G. Evans, J. C. Puzak,  F. E. Butler, a.nd
     J. E. Frazer.  Air Quality Data  for Nonmetallic Inorganic Ions:   NH., NOV
     SO.  1975  from the National Air  Surveillance Networks.  EPA-600/4-78-035;
     U.S. Environmental Protection Agency,  Research Triangle Park, NC, June,
     1978.

8.    Rhodes, R. C., D. H. Fair, J. E. Frazer,  S. J. Long,  W. A. Loseke,
     V. A. Wheeler, and J. F. Walling.  Air Quality Data for Metals 1975  from
     the National  Air Surveillance Networks.   EPA-600/4-78-059, U.S. Environ-
     mental Protection Agency, Research Triangle Park, NC, October, 1978.

9.    Junge, C., and G. Scheich.  Determination of the acid content of  aerosol
     particles.  Atmos. Environ. 5:165-175, 1971.

10.  Lee, R. E., Jr., and S. Goranson.  National Air Surveillance Cascade
     Impactor Network.  III.  Variations in size of airborne particulate
     matter over a three-year period.  Environ. Sci. Techno!. 10:1022-1027,
     1976.                                                    ~

11.  Patterson, R. K., and J. Wagman.  Mass and composition of an urban aerosol
     as a function of particle size for several visibility levels.  J. Aerosol
     Sci. 8:269-279, 1977.

12.  Durham, J. L., W. E. Wilson, T.  G. Ellestad, K. Willeke, and K. T. Whitby.
     Comparison of volume and mass distributions for Denver aerosols.  Atmos.
     Environ. 9:717-722, 1975.
                                     67

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13.  Rahn, K. A., R. Dams, J. A. Robbins, and J. W. Winchester.   Diurnal
     variations of aerosol trace element concentrations as  determined  by
     nondestructive neutron activation analysis.  Atmos.  Environ.  5:413-422,
     1971.

14.  Akselsson, R., J. W. Nelson, and J. W. Winchester.   Proton  scattering  for
     analysis of atmospheric particulate matter.  Bull. Am.  Phys.  Soc.  2:484,
     1975.

15.  Hardy, K. A., R. Akselsson, J. W. Nelson, and J. W.  Winchester.   Elemental
     Constituents of Miami aerosol as a function of particle size.   Environ.
     Sci. Technol. 10:176-182, 1976.

16.  Gladney, E. S., W. H. Zoller, A. G. Jones, and G. E. Gordon.  Composition
     and size distributions of atmospheric particulate matter in Boston area.
     Environ. Sci. Technol. 8:551-557, 1974.

17.  Lundgren, D. A., and H. J. Paulus.  The mass distribution of large
     atmospheric particles.  J. Air Pollut. Control. Assoc.  25:1227-1231,
     1975.

18.  Lee, R.  E., Jr., R. K. Patterson, and J. Wagman.  Particle  size
     distribution of metal components in urban air.  Environ. Sci. Technol.
     2:288-290, 1968.

19.  Lee, R.  E., Jr., S. Goranson, R. E. Enrione, and G.  B.  Morgan.  National
     Air Surveillance Cascade Impactor Network.  II.  Size  distribution
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     1972.

20.  Dzubay,  T. G.,  R. K. Stevens, and C. M. Peterson.  Application  of the
     dichotomous sampler to the characterization of ambient aerosols.   In:
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21.  Commins, B. T., and R. F. Waller.  Observations from a 10-year  study of
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22.  Lee, R.  E., Jr., J. S. Caldwell, and G. B. Morgan.   The evaluation of
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24.  Robinson, E., and R. C. Robbins.  Sources, Abundance,  and Fate  of Gaseous
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                                     68

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25.   Hidy, G.  M.,  and J. R. Brock.  An assessment of the global sources of
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28.   Office of Air Quality Planning and Standards.  National Air Quality,
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29.   Health Effects Research Laboratory.  Air Quality Criteria for Lead.
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49.  Dehnen, W., N. Pitz, and R. Tomingas.  The mutagenicity of airborne
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63.  Environmental Criteria and Assessment Office.  Health Assessment Document
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76.   L.  S.  Dochinger, and T. A. Seliga, eds.  Proceedings of the First
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                                     75

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                                   TECHNICAL REPORT DATA
                            (Please read Instructions on the reverse before completing)
 1. REPORT NO.
  EPA-600/9-70-Q06	
 4. TITLE AND SUBTITLE
, SUSPENDED  PARTICULATE MATTER:
 A Report to  Congress
7. AUTHOR(S)
 Dr. Lucile Adamson,  Howard Univ., Washington,  D.C.
 Dr. Robert Bruce
                                                           8. PERFORMING ORGANIZATION REPORT NO
9. PERFORMING ORGANIZATION NAME AND ADDRESS
 Environmental  Criteria and Assessment Office
 Office of  Research  and Development
 U.S. Environmental  Protection Agency
 Research Triangle Park,  N.C.  27711	
                                                           3. RECIPIENT'S ACCESSION NO.
             5. REPORT DATfc

                 June 1979
             6. PERFORMING ORGANIZATION CODE
                                                           10. PROGRAM ELEMENT NO.
                1HA882
              11. CONTRACT/GRANT NO.
12. SPONSORING AGENCY NAME AND ADDRESS
 Office of Research  and Development
 U.S. Environmental  Protection Agency
 Washington, D.C. 20460
                                                           13. TYPE OF REPORT AND PERIOD COVERED
                TYPE Q
                Final

             14. SPONSORING AGENCY CODE
                                                              EPA-600/CO
15. SUPPLEMENTARY NOTES
      fliis report is  in  response to Section 403(a)(1) of the Clean  Air Act as Amended
 August 1977.  The  report  covers:   1) a review of the physical and  chemical  characteris-
 tics of airborne particles  (source, composition, and sampling site as related to size);
 2) a review of the effects  of particulate matter on public welfare (ecological,  materi-
 als, atmospheric,  aesthetic);  3)  the status of human exposure to airborne particles as
 related to source; and  4) a review of the effects of airborne particles  on  human health
 (lung deposition,  chemical  composition, interactions, and potentiating conditions).
      Although there  is  a wide  divergence of opinion among experts  and scientific groups
 with respect to the  issues  of  particulates (cf. Appendix A), the following  can be
 concluded from the available information:
      1.  High levels of airborne  particles have been associated with  episodes of high
 pollution during the past,  especially in the United Kingdom and the United  States.
      2.  Although  pollution levels have declined in many U.S. localities  in recent
 decades,  there is still need for  improvement in several of our cities.
      3.  Additional  research is needed to improve the scientific basis for  future
 airborne  particle standards as  outlined by EPA (cf.  Dr. Cortes 1 in the Culver Pilot
 Study of  Particulate Matter).
17.
                                KEY WORDS AND DOCUMENT ANALYSIS
                  DESCRIPTORS
b.IDENTIFIERS/OPEN ENDED TERMS  C.  COSATI Field/Group
aerosols   ecology    public health  smog
airborne wastes  emission        smoke
air pollution  fibers   soot
ashes    fly ash  respiratory system
carcinogens    inorganic acids  visibility
combustion products   metals     smelting
corrosion   mist
       nr
   ;irllPiHiIPpIrticu1a4s
 m\
                                                                            04A
                                                                            04B
                                                                            06A
                                      13B
metallurgical processes
                                                                            07B
                                                                            07C
18. DISTRIBUTION STATEMENT

  RELEASE  TO PUBLIC
19. SECURITY CLASS (This Report/

 UNCLASSIFIED
                           21. NO. OF PAGES
                                                                            76
                                              20. SECURITY CLASS I This page)

                                               UNCLASSIFIED
                                                                        22. PRICE
EPA Form 2220-1 (Rev. 4-771
                                    'S CBSO'_E-E
                                            76

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