Briefing Report
PROBLEMS RELATING TO FINE SUSPENDED PARTICIPATES
   U. S. Environmental Protection Agency
   National Environmental Research Center
Research Triangle Park, North Carolina 27711
                      1973

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                                                   600R73006
                                            00  NOT QUOTE OR CITE
                              Preface



     This  document was prepared by a Task  Force convened under the

direction  of  Dr. John F. Finklea, Director, National Environmental

Research Center, Research Triangle Park (NERC/RTP).  The objective

was to identify  the major problem areas associated with fine par-

ti culates  in  the atmosphere, and their effects on human health and

welfare, with a  view toward the need for control  under the provisions

of the Clean  Air Act, as amended.

     The following members served on the NERC/RTP Task Force:
          James R.  Smith                Andrew O'Keeffe
          John Nader                   Robert Chapman
          Jean French                   Paul  Altshuller
          J.H.B.  Garner                 Robert E.  Lee
          James  Dorsey                 James H. Abbott
          Elbert Tabor                 Glen  Fairchild
          Gary Foley                   William E.  Wilson
          A. B. Craig                   Justice Manning - OAQPS
          Jack Wagman                   John  Sigsby
          Douglas Fox                   James 0. Baugh
          Kenneth T. Knapp              Ronald L.  Bradow
          Robert M. Burton

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                NOTICE

This document is  a  preliminary  draft.  It
has not-  been formally  released  by EPA
and shoijM^Qt at this stape he  r'ormtri'ed
to represent Agency policy.   It is being
circulated  for  comment  on it?,  technical
accuracy and policy implications.

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                        TABLE OF CONTENTS   DO  NOT QUOTE OR C1
  PREFACE
  QIIMMADV.                                                              1
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  CONCLUSIONS ............ - .............. - --------------- — — ....... — 5
  RECOMMENDATIONS— —— ............ -- ..... ---- — — ...... — _ — 7

  I.   INTRODUCTION ..... - ............ - ----- -- — -------- — -------- --35

 II.   CHARACTERIZATION METHODOLOGY— ....... ------- — _ — _ -------- 36
  A.   Definitions ---- -----—, ---- - ...... , ------ ,---- ---- _..---, ------- - — 35
  B.   Particle Sizing Methods — ---ซ ---- ---_„-, ---- „„„„„__„„ ------ _ — 35
  1 .   Microscopic Methods .............. - ..... --__-„„_„-__-, ----- ------37
  2.   Aerodynamic Fractionating Devices- ..... -- — - — ----- — --____37
  3.   Optical Sizing Devices ---- < ---- < -------- - ---- --• ------ ----• ---- ----33
  4.   Particle Size Sampling -------- < — - ----- • ----- • ------ • ---- ----- — --39
  a.   Ambient Aii ------ ................. ----- - ...... - — --— - — -----39
  b.   Stationary Sources----- ----- - -------- - — ----. — ,-_-___-. — __ — 39
  c.   Mobile Sources. ------ - ............... ---- - ......... -• ---- - ------- 40
  C.   Chemical Composition ---- - — <--- ---- - ---------- < ------- • ---------- 40
  D.   Problem Areas ---- ----- ------- . ------ ....... - ---- _____„_„___. ___-A]

III.   ATMOSPHERIC INPUT— ...... „— -„ ........ ,.——.,—44
  A.   Stationary Source  Emissions and Control — ,--,---. — , ------ >-- ----- 44
  1 .   Emissions----- ...... - ----- - --------- • ----------- -- — ___— -------44
  a.   Present Status ...... -- ...... ---• ---------- — ---. — -,-„_--„ — 44
  b.   Planned R & D ---- - ----- • ...... — ........ ——_ ——-_—_„_, ---- 45
  2.   Control---- ..... ------- ........ - ..... — — — _ ---- 45
  a.   Primary Fine Particulates— ------- — ----- ---- --__---„--__. -.45
  b.   Secondary  Fine  Particulates— ----- ------ ,_..-,_„_„„„„, — „„ ------ --,43
  3.   Problem Areas ---- ----_--„-,-,---,,, ---- „>„„„„„„, r,^_^_r,_m^^r,,ป^,_mป^49

  B.   Mobile Source  Emissions and Control--------- — ._„_„, ^--_^_^,_--5]
  1 .   General Discussion--"-"------. ----- - ------ ^-r.~-~-,--~--~ ----- _____51
  2,   Problem Areas--- .......... - ...... ----- ------- -„-„-,-„.„„ ---- 53
  C,   Natural Sources--' ---- --• ----- - ------- -- — ----- ........ _...,_->,,55
  1 .   General Discussion--------- ---- __-_,.-„„--„„_„, ---- ^.ป.7.,ปซ^^r,^r.™.r,^.55
  2.   Problem Areas- ---- „„„„,._,.-, ------ „,,-,,-,-., ---- ^- -------- --- ---- ---56

 IV.   ATMOSPHERIC LOADING ....... - — -- ---- — ----- , ---- „„„„.,,._„., ——58
  A.   Introduction — „„„_.„---, ...... „„ ..... ~^ ----- l„„r.ป„^---.-,^„r.ป--„„„':>Q
  B,   Transport and  Prediction Modeling ---- „„-.„-.„,-,.,-...-„„,..-_.-__.,., — 53
  C.   Transformations ---- ---- — ---- ------ ...... ------- --. ----- --- ---- 60
  1.   Sul fates ......... - ........... • ----- - ---- --- ----- .— -,— ..... ----60
  2,   Nitrates ...... -- ........ - ........ „„„„„„_„_.,_..,,_„.,.-,. ----- „, ---- _ป5Q
  3.   Organic Parti culates ---- - — ••<-< ------ ---< ----- ----- ---- ----- ------ 59
  4.   Ammonia-. ----- • ------- „----_--_-, ---- , ----- „-„ ..... ^r~~~r.~~-.^-,~-~~-(:>Q
      5Dav>-H/-la ^n-yo  _______ซ.______--,___--__-._-.__--.__-,____ _          SI
   .   tar I. 1 1- I c o I /.c---"----™1-- ------------- -----  „- — -„„_„______,„„„_(-) |
  6.   Properties ------ ---- ...... --------„-, ---- ----- ------ ,-f._.,,,,,_,-___,.6i
  7.   Problem Areas ------ ------. ---- , ------ ------ ----------- „„.,., ---- ,---61

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                                                 DRAFT
                       TABLE OF CONTENT^ J.QJ Q^^ QR C|TE

                                                                     Page
IV.  CONTINUED
 D.  Natural  Removal  Processes		-		62
 1.  General	<	'	'—--62
 2.  Problem Areas---	•			63
 E.  Physical  and Chemical Characterization of Ambient  Air
        Particulate-------	<	>--	• -	- —-—.	63
 1.  Size  Distribution--	•	63
 2.  Composition and Concentration	:	66
 3.  Problem Areas<	——,	— .	.	66

 V.  EFFECTS—	—	—	71
 A.  Health	———	—,	——-——71
 1.  Experimental Studies (Man and  Animals)-------"-		,—--71
 a.  Introduction--*—-—••<	———>	.——,— ————————71
 b.  Dose-Response RElationships— —	<	>--—<	---	72
 c.  Physical  Factors	---—	•	-73
 d.  Host-Related Factors--------		-	—75
 e.  Retention Factors	78
 f.  Biological  Respirable Particles---	--<	79
 2.  Epidemiology-----	„„,„..„..„.,„_,	rP,r,^^r,^r,r,^,.F,r,r,r.^™^^r,T,^^_r,mr,80
 a.  Asthma  Study------------------------------------------T-	--80
 b.  CHESS  Studies	-	__..,,,.,.r..,,,_,,.,,._.,,.r,r...,.r,...,,,_8l
 3.  Relative  Toxicity-----'		-„-..,-	^--,—.----83
 4.  Problem Areas	<	.		„---„„„-„„„..,—.-—-84
 a.  Aerometry	--•	—--.—.	:-	—.^---84
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 B.  Effects  on  Visibility, Weather and Climate—.	--——86
 If  V I O I L) I I | U V ^1*™^p^r"w^^^"^^^wซซ*"""r'^M^^wf"r*r™^^'w^^^^^^,^i^i^^^^"i?^.^i^^^^^^^™^r"^^QQ
 2.  Weather  and Climate	--.	.--.—.	——- ——^^86
 C.  Ecology--	-•			,	—,	--—--——89

VI.  CONTROL  STRATEGIES	-	--90

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                   SUMMARY, CONCLUSIONS AND RECOMMENDATIONS *ฐ/
                                                                •~/(j
A.  SUMMARY
                                                                           Wfr
     There is no universally acceptable definition of fine particulate.       c
For the purpose of this report we have chosen an upper size in the range of
2-5 urn diameter.  Based upon the limited data available, a significant
portion of the particulate found in the atmosphere would be classified
as fine.  The total atmospheric loading consists of primary and
secondary particulates, as defined in Section II.
     The term fine particulate implies that the characteristic of
physical size is the  dominant factor relative to air pollution problems.
This is not  necessarily true with respect  to health effects.  Chemical
composition, and related  physical factors, may prove to be equally or
more significant.

        For the purpose of this report, we have classified the major source
   categories of fine particulates as:   (1) stationary, (2) mobile,
   and  (3)  natural.  Natural  sources include forest fires, wind-blown  dust,
   volcanic activity, and sea salts.   Natural  gaseous emissions of H2S,
   NO ,  NH3,  and hydrocarbons are transformed  in the atmosphere to sulfate,
   nitrate,  ammonium compounds,  and hydrocarbon aerosols.   We do not have
   reliable quantitative estimates of the contribution of  each of these
   source  categories to the total  atmospheric  loading.   There appears
   to be significant regional  differences in source contributions.  Emissions
   from  mobile  sources are primarily in the fine particulate category.
   In Los  Angeles  the major portion of the mart-made fine particulates  has been
                                  -1-

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attributed to mobile  sources—principally the passenger car.  On a national
basis, and in particular,  the eastern industrial regions, the stationary
sources probably contribute  the  larger portion.  Neither global nor local
concentrations'Of fine  particulates'in the atmosphere have been adequately
characterized.  Where particulate data have been characterized, by particle
size and chemical composition,  it appears that each chemical constituent
may have a discrete size distribution.
     The formation of secondary fine  particulates  in the atmosphere
represented major problem in assessing man-made  and natural contributions
to the total atmospheric loading.   Neither  the chemical mechanisms
nor the reaction rates involved in these  transformations are well known.
     Very little effort has been devoted  to understanding  the  removal
mechanisms for fine particulates in the atmosphere.  The principle
mechanisms are thought to be precipitation, dry  deposition, and  biological;
however, none of these are well understood.
     The toxicological properties  of  inhaled particles  are related  to
specific physical and chemical properties of the particles and host con-
ditions which affect response to exposure.   The  principal  path through  which an
airborne particle exerts an effect on health is  presumed to be through
inhalation and consequent effects  on  the  respiratory  system.   This
presumption is acceptable for a determination of short-term effects  of
irritant aerosols; however, it may be less  tenable in  the  consideration
of long-term exposure effects where such  responses as  carcinogenesis,
                                     -2-

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                                                       fi D ^ 3"T
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                                                       vvGfฃ  Q$ PITT
deposition,  the  body insult may actually be initiated  by an overburden
of particles of  a  specific chemical species whose effects are aggravated by
particle size.
     Fine particulate control technology is now at a early  state of
development, except under certain limited conditions where collection
systems have reached high mass efficiencies resulting  in the capture
of fine particles  along with large particle size material.

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B.  Conclusions
     In essence, the following conclusions reflect the problem areas
related to fine particulates in the atmosphere,
     (1)  The present data base, and current state of knowledge related
to the pollutant classification  fine particulate, is  inadequate
to serve as a basis for rational decisions regarding control strategies
under the provisions of the Clean Air Act.
     (2)  Available information suggests that certain chemical
elements and compounds included in the classification of fine particulate
may account for the major portion of the  air pollution stress on human
health and the environment.
     (3)  The total atmospheric loading of fine particulate results from the
emissions of primary  fine particulate and from the secondary fine particulate
formed by the complex transformation and  transport processes occurring
in the atmopshere  between other particulates and/or  gases.  Data are
inadequate to define  the relative contribution of primary and secondary
fine particulate to atmospheric  loading  on  a national  basis.

     (4)  Atmospheric visibility, certain weather processes, and certain
climatic conditions  can be  related directly  to fine  particulate  in  the
atmosphere.  Particle size  range of  greatest importance  for effect
on visibility  is 0.1  to 1.0  >mi,
      (5)   The  total  atmospheric loading of  fine  particulates  is
 related  to  source  inputs,  transformation, transport and removal  processes.
 These  processes and conditions are not understood well.

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                                            1  NOT QUOTE OR CITE
     (6)  At the present time,  the  man-made  contribution  to  the  total
atmospheric loading of fine  particulate  cannot be  quantitatively
separated from the natural  contribution.
     (7)  The control  of the man-made  contribution to  the total
atmospheric loading of fine  particulates  will  require  the control
of primary fine particulates and gaseous  precursor emissions.
     (8)  The total atmospheric loading  of fine particulate  and  its
effect upon human health and welfare are  dependent upon a complex
matrix of directly and indirectly related processes.   Any compre-
hensive study of this  problem cannot ignore  these  relationships.
     (9)  Solutions to the  problems related  to the control of  man-made
contributions to the atmospheric loading  of  fine particulate will
require an extensive data base which must be developed over  an extended
period of time.  Implementation of  partial control actions should
proceed in consonance  with  the accumulation  of this data  base.
                                 -6-

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C.  Recommendations

     Suspended fine particulate in the atmosphere represents not

only one of the most complex scientific and technical  aspects of

air pollution, but also one of the most important.  In fact, it

encompasses a large segment of the total atmospheric pollution

problem.  The solutions will require a closely integrated research

and development effort involving responsible federal agencies,

universities, and  industry.  The program must be oriented toward

specific goals, and will require extensive resources over an extended

period of time.  This requires a program planning effort which

exceeds the scope  of this document and the efforts of this task

force.  However, an attempt has been made to identify the major

problem areas, and hence provide the basis for a more extensive planning

exercise.

     The problem of suspended  fine particulates  is so complex that

it  is difficult to place in perspective without  the aid of systematic

paths of inquiry.  An effort has been made to depict these paths in

Figures S-l  - S-ll.    These represent the essential elements

of  a research and  development  program to achieve  the following goal:

                 "Determine and understand the contribution
                 of man-made sources to the total atmospheric
                 loading of fine particulate; assess its effect
                 upon human health and welfare;  develop needed
                 control technology; and define  and implement
                 control strategies when and where the result
                 of this research effort dictates that such
                 are necessary."


The proposed research and development program would include  five major

elements, as indicated in Figure 1.  These are:   (1) the atmospheric

input from      man-made and natural sources, both controlled and
                                    -7-

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                                              00 NOT QUOTE OR CITE
 uncontrolled;  (2) characterization  of  the  fine  participate  in
 the  atmopshere;  including physical and chemical properties, and
 transformation,  transport, and removal processes; (3) quantify the
 atmospheric  loading in space and time, (4) determine the health
 and  welfare  effects, and (5) develop specific control technology-
      The  atmospheric input element must address the contribution
 from man-made  stationary and mobile sources, and natural sources.
 Emissions from each of these sources must be characterized in terms
 of physical  and  chemical properties, both in the process stream
 and  at the source output.  The output must be quantified in terms
 of mass,  number, and chemical  composition as a function of size.  This element
 must consider  both primary fine particulate and gaseous: secondary presursor
 emissions.
      Fine  particulate in the atmosphere is  subject  to complex
 physical  and chemical  transformation,  transport, and removal  processes.
 These must be at least semi-quantitatively  assessed  and understood
 if the atmospheric loading  is  to  be  efficiently controlled.
     The atmospheric  loading  in space  and time reflects the  degree
 to which receptors are exposed, and  consequently the stresses upon
man and the environment.   It  represents the realistic input  essential
 for the assessment of  effects.  Adequate simulation  and prediction
models must be developed to quantitatively estimate  the atmospheric
 loading.  This will  require inputs,both in terms of  understanding and
 quantitative values,  from the program element involving transport,
 transformation, and removal  processes, as well as quantitative
 measurements from a routine data  collection network.
                                     -8-

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                                            nO MOT OUOTE Oft CITE
     In the final analysis, the assessment of health and welfare
effects must be based upon the concentrations, as well as physical properties
and chemical composition, of fine particulate observed in the atmosphere.
The program element concerned with atmospheric loading must provide
in the proper format the necessary quantitative and qualitative
input.  The effects program element must be concerned with acute
effects resulting from short-term exposure to maximum concentrations,
or highly toxic substances; and chronic effects from long-term exposure.
These studies will require information on size distribution (possibly both mass
and  number  density), chemical  composition,  physical  characteristics, and con-
ditions  of  exposure.   Chronic  studies  will  require  long  periods of record.
The  assessment  of human  health effects will  require  extensive  laboratory
and  epidemiological studies.   The problem of extrapolation from
laboratory  experiments with animals to human response should be given
a  high priority.   In designing and conducting the laboratory studies
consideration should be given  to  interrelating them with the needs
of epidemiological studies.  Close coordination and  feed-back between
the  effects effort and the control technology effort of  the atmospheric
input element will-be essential.
     The  environmental effects studies will  require  specific inputs
from the  atmospheric loading program elements-. Visibility studies will re-
quire quantitative  data on size distribution, chemical composition, physical
properties, and concentrations.  Ecological  studies  will depend heavily
upon information concerning removal processes.

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     The ultimate goal  of research on the heWlh) effefcWHbr-fWte  ^arti-
culates is, as for other pollutants,  the development of complete  and
accurate dose-response  relationships  for humans.   Fine particulate  research
is beset by problems common to all pollution research.  Among these are
incomplete aerometric technology and  the frequent necessity to make
inferences about human  response from  animal  studies.
     Fine particulates  research is especially complex, due to the
twin factors of particle size distribution and particle chemistry.
With gases, size distribution is not  a problem.   With :particles,  it is
crucial.  Without knowledge of particle size distribution, we cannot know
the principal site or sites of deposition, and thus cannot fully  understand
the particulate pollutant's mechanism of physiologic action.  Thus,
a prime goal of particle research must be to develop size-specific
dose-response relationships for particulates of concern.  Amdur has begun
this work with sulfates, and has demonstrated the importance of particle
size.

      The importance of knowing specific particle chemistries  in  addition
 to size distributions  must be stressed.   For example,  the finding  that
 different metallic sulfate compounds have different effects on airway
 resistance supports the contention that the sulfate's companion
 cation or cations are  important to the sulfate's toxicity.   Whether
 the cation of the sulfate is primary responsible for the observed
 effect must be determined.
                                 -10-

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     Perhaps the ultimate characterization of local  atmospheres,  and
thus of individual pollutant doses, will  come through  the  use of  personal
enviornmental monitors.  At present, it is very  difficult  to conceive of
a personal monitor that is both inconspicuous and capable  of making  size-
specific measurements of potentially toxic pollutants.   However,  if  the
list of pollutants can be narrowed to a few of greatest concern  (and
that may not be possible), such monitors may be  plausible.   They  would
certainly be helpful in the development of dose-response relationships.
       Health research  on  fine  particulates  must be  expanded  in two major
 ways.   First,  new health  indicators must  be examined  in experimental
 studies.   The  experimental  work to date  has dealt primarily  with one
 physiologic indicator, airway  resistance.   This indicator is  a functional
 one,  which has been used to reflect acute exposures.   Structural changes,
 which  underlie functional  changes, must  also be studied.  Perhaps more
 important, the impact  of chronic particulate exposure  on chronic and acute
 disease must be assessed.
       Second,  studies  of fine  particulates  must be  extended  to humans.
 Of course, ethical  constraints will not  permit  the  exposure  conditions to
 which  animals  are subjected.   However, carefully controlled  clinical
 studies involving chamber exposures will  have an important  place in fine
 particle research.   Such studies will  be most helpful  in  the systematic
 description of particle toxicity.   Conceivably, clinical  studies will
 narrow the long list of fine particulate substances to a  few of  major concern
 Clinical  studies  should also help in assessing  the  effects  of different par-
 ticle  size distributions.
                                  -11-

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      Epidemic!ogic studies  will  be necessary to  assess  the chronic  and
acute effects of fine particulates  in  ambient atmospheres.  Such  studies
may be particularly useful  in elucidating  the effects  of long-term exposures.
Also, it has proven extremely difficult to find field  settings in which ,a single
pollutant or pollutant class 1s  present in the absence of other pollutants.
Thus, field studies may prove at least as  useful  in  assessing pollutant
interactions as in assessing the effects of individual particulates.
    The effects of particulates alone, or even of individual  particulate substances
could be assessed in epidemiologic  studies if a series of biological indicators,
specific for particulate exposures, were developed.   It is quite  conceivable,  for
 instance,  that  certain cytologic changes in the resptratory tract might
 reflect exposures  to  particulates and to no other pollutants.  Certain
 changes in enzymes, other proteins, and cells away from the respiratory
 tract might also reflect such exposures.  The use of epidemiologic indi-
 cators specific for particulates (and for other pollutants) would clarify
 and  complement  toxicologic and clinical studies in the field of fine
 particulate research.  Complete epidemiologic and clinical data will
 relieve us from the risky task of developing air quality standards
 largely from animal data.
      Given adequate information regarding health and welfare effects,
 the  problem of  specifying control technology, and the definition and
 implementation  of  control strategies, would depend upon the status
 of technology,  and cost-benefit relationships.  Control technology must
 be developed, to control both primary fine particulate and gaseous secondary
                                  -12-

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                                              DO [MOT QUOTE  OR CITE
particulate precursors.   The problem of physical  and  chemical
characterizitoon of emission sources is particularly  important.
Improved techniques must be developed to determine the  contribution
of man-made sources to the total  atmospheric  loading.   The  problem of
relative importance of secondary pollutants resulting from  precursor
emissions from stationary and mobile sources  must be  resolved. Solution
of these problems will require improved measurement and analysis
techniques.
     A summary of current research activities related to fine  particulate
is given in Table S-l.  These efforts are contributing  materially to our
information base, however, much remains to be done.   Specific  recommended
new research projects are listed in Table S-2.  These projects reflect
the needs of the proposed research program;  however,  they do  not
represent the entire  scope.  In essence, they represent the capabilities
of the NERC/RTP,
     Finally, in our  emphasis of "fine particulates", we must not
forget the importance of  larger particles as  objects  of study.  Such
particles may promote disorders in the nose,  nasopharynx, sinuses,
or gastro-intestinal  tract.
                                 -13-

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                              FINE PARTICIPATE
                           AREA AIR POLLUTION CYCLE
                                  Figure 5-1
                                                            CUE
STATIONARY.
EMISSIONS
   &
CONTROL
™J5to

MOBILE
EMISSIONS
&
CONTROL
\ \
\
\
\
                                 CONTROL
                                 STRATEGIES
 NATURAL
 SOURCES
ATMOSPHERIC
INPUT-
PHYSICAL AND
CHEMICAL
CHARACTERIZATION
                                               TRANS-
                                               FORWION
                                           -*H
                              TRANSPORT!
\ fc NON-ATMOSPHERIC,
 V [ POLLUTION
  ][ EFFECTS
                              NATURAL
                              REMOVAL
                              PROCESSES
                                                               r
; ATMOSPHERIC
; LOADING -
PHYSICALS
| CHEMICAL
jCHARACTER-
IZATION
HEALTH
  &
WELFARE;
EFFECTS!
                                                    I

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                            STATIONARY EMISSIONS AND CONTROL
                                   FINE PARTICULATE
                                    Figure 5-2
                                                            DRAFT
                                                    !')0 NOT QUOTE OR CITE
PHYSICAL &

PROPERTIES OF

STREAM
                   CONTROL
                   DEVICES
5*
PROCESS

CATION
                   RAW
                   MATERIALS
                   CLEANUP
\


PARTICLES

                                     GASEOUS
                                     PRECURSORS!
                                        SIZE
                                        DISTRI-
                                        BUTION
                                                     CONCENTRATION
COMPO-
SITION
                                       COMPO-
                                       SITION
                                                      CONTROL
                                                      STRATEGIES!
                                                                           MASS
                                                         NUMBER
                                                         DENSITY
ATMOSPHERIC
INPUT-
PHYSICAL &
CHEMICAL
CHARACTERIZATION

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cr>
i
FUELS
FUEL
ADDITIVES
            T
                                          MOBILE EMISSIONS AND CONTROL
                                              FINE PARTICULATES
                                                   Figure 5=3
                         PHYSICALS  ,
                         CHEMICAL   I
                         CHARACTERI-
                         ZATION
                         WITHIN      I
                         SYSTEM     !
                OPERATING
                CONDITIONS-
                CYCLIC
                                     CONTROL
                                     DEVICES
NEW
POWER  i
SYSTEMS
                                                          PARTICU-
                                                          LATE
                                                                                    SIZE
                                                                               *H  DISTRI-
                                                                                    BUTION
                                     CONCEN-
                                     TRATION!
                                                              EMISSIONS!
                                      COMPO-
                                      SITION
                    GASEOUS
                    PRECURSORS
CONCEN-
TRATION i
                                                              CONTROL
                                                              STRATEGIES
                                                ATMOSPHERIC
                                                   INPUT

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                                  NATURAL SOURCES
                                  FINE PARTICULATE
                                     Figure 5-4
                                                                   DRAFT
                                                            DO NOT QUOTE OR CITE
  PRIMARY
  GASEOUS
 SECONDARY
PARTICULATE
 PRECURSORS
•*ป•
                     SOILDUST
                    VOLCANOS
                     FOREST
                     WILDFIRE
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                                       ATMOSPHERIC INPUT
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-------
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-------
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-------
                                         REMOVAL PROCESSES
                                         FINE PARTICIPATE
                                             Figure 5-8
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                                                                            DO NOT QUOTE OR CITE
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-------
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                                                  Figure 5-9
                            TECHNIQUE DEVELOP-;
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                                                                             DO NOT QUOTE OR CITE
                 CONCEN-
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                                                                        COMPO-
                                                                        SITION
                                                                                     ATMOS-
                                                                                      PHERIC
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-------
                                                  EFFECTS
                                              FINE PARTICIPATE
                                                  Figure 5-10
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  AND
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                         HUMAN
                         HEALTH'
                        MATERIALS
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                                        ANIMAL
                                       PRECIPITATION (ACID RAIN)
                                         VISIBILITY REDUCTION
                                         RADIATION BALANCE
EFFECTS
CRITERIA
CONTROL
STRATEGIES

-------
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  SHORT-
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  LONG-
  TERM
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                                                   Figure 5-11
                     SINGLE
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                       OR
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                 MULTIPLE
                       OR      i
                     COMPOUNDS!
                 METEOR-
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                 REACTIONS
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ACUTE
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                                                                             CHRONIC i
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                                                                                 iฃ*
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                                            DRAFT
                                     DO NOT QUOTE OR CITE
                   Table S-l

SUMMARY OF CURRENT RESEARCH RELATED TO FINE PARTICULATES
                        -25-

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                                                QMJE OR CITE
                       Table  S-l
SUMMARY OF CURRENT RESEARCH  RELATED  TO  FINE  PARTICULATES
                                                    Est*
                               Estimated  Date       Costs
                             of Completion  (Yrs)   ($1000)
      Task Description

1.  ROAP 21AYB - Produce mono-              4
graphs describing human  health
effects of long- and short-term
exposure of population  subgroups
to respirable particulates.
Health effects will  be  identi-
fied in CHESS neighborhoods  and
in selected high risk subgroups.
Human exposure chambers  will  be
used to provide dose response
information on the clinical  and
physiologic effects  of  controlled
human exposures to sulfates  and
nitrates.

2.  ROAP 21AYF (Partially related          5
to fine particulate)- Isolated
test systems will be developed
and employed in conjunction  with
relevant whole animal studies
to assess toxic effects  of
environmental pollutants at  the
cellular and subcellular level
pollutants include airborne
particulate and fly ash.  Con-
tinuing studies to evaluate  the
interaction of inhaled  carcinogens
with nose mechanisms and pul-
monary defense systems.   Determine
the relative biological  effects
of specific sulfates.  Studies  to
determine the role of selected
fine particulates found in the
atmosphere as co-factors in  pul-
monary carcinogenesis when com-
bined with known atmospheric
polycyclic hydrocarbons.

*Represents that portion of ROAP cost prorated for fine
 particulates.
                                                    1,200
NERC/RTP
  Lab

  HSL
                                                              EBL
                               -26-

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                                              00  NOT QUOTE OR CITE
                      Table S-l  (Continued)
      SUMMARY OF CURRENT RESEARCH RELATED TO  FINE  PARTICULATES

                                                         Est*
                                     Estimated  Date      Costs    NERC/RTP
      Task Description             of Completion  (Yrs)   ($1000)      Lab

3.  ROAP A26AAE - (Partially              3            ] >'951        EBL
related to fine particulate)
Estimate no-effect level using
mouse pulmonary infectivity model
(a) of appropriate Pt. group
metal compounds administered
singly (b) of base metal compounds
administered in appropriate com-
binations.  Compare relative
toxicities against Pb compounds
using vn_ vitro macrophage system
(a) of Pt - group compounds (b)
of base metal compounds.  Compare
pulmonary carcinogenicity of Pt
group metal compounds and of Pb
compounds in association with
polynuclear aromatics using
ir\_ vivo hometer system.

4.  ROAP 21AZM - The effects of           6             1,249        CPL
aerosol composition on visibility.
Measure the optical properties of
primary and secondary aerosols.
Develop quantitative relationships
between visibility loss and aerosol
characteristics such as concen-
tration, size, shape, and chemical
composition.  Determine effect of
changes in relative humidity on  •
particle size and optical properties.
Study conversion of NO  , SO , and
organic vapors to particulars.

5.  ROAP 21AKB - Determination of the     6             5,321        CPL
character and origin of aerosols.
Determine the physical and chemical
character and properties of source,
ambient, and natural aerosols.
Determine the contribution of the
various sources to the ambient
atmospheric aerosol loading.
Determine generation rates and
removal rates for important sources
and sinks.  Measure effects of various
aerosols on atmospheric chemical

                                -27-

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                                                       Dfi/IFT
                                         ,     DO WOT QUOTE  OR CITE
                     Table  S-l  (Continued)                          on L

      SUMMARY OF CURRENT  RESEARCH  RELATED TO FINE PARTICULATES

                                                         Est*
                                     Estimated Date      Costs     NERC/RTP
      Task Description             .of Completion (Yrs)  ($1000)       Lab
reactions.   Determine rates  and
mechanisms  for conversions of  gases
to aerosols, growth and  coagu-
lation of aerosols, and  aerosol
removal mechanisms.
6.  RQAP 56AAJ (Partially related             5             1,425       CPL
to fine particulates)  -  Regional
air pollution  study air  quality
characterization.   Characterization
of aerosol  pollution in  St.  Louis
to develop data base for develop-
ment and validation of models  of
visibility loss and aerosol  forma-
tion, growth,  and  removal.   Determine
sources of visibility reduction;
determine aerosol  chemical  composition,
size distribution, and sources;
determine gas-aerosol  interactions.

7.  ROAP 26AAM - Development of               5             1,200        CPL
instrumental and analytical  method
for the measurement of particulates
from stationary sources.  Much
of the effort  relates to particle
size measurements.  This includes
both the development of  stationary  source
sampling systems that maintain sample
integrity for  size measurement and  size
measuring system.   Several  instruments
for size measurement have been developed
including an automated device  that
combines with  an  seperator  with beta
absorption  measurements.

8-  ROAP 26AAN - Methods development         5              300       CPL
for the determination of chemical
composition of particulate by  size
fractions from stationary sources.
                                  -28-

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                     QUOTE  OR CITE
                  Table S-l  (Continued)          "u NOT

    SUMMARY OF CURRENT RESEARCH RELATED  TO  FINE  PARTICULATES

                                                          Est*
                                     Estimated  Date       Costs    NERC/RTP
    Task Description               of Completion (Yrs)   ($1000)      Lab

9.  ROAP 21ADL - Development through       6             11,042      CSL
pilot scale of at least three broadly
applicable methods or devices for
control of fine particle (less than
3.0u) emissions.  Pilot ?cale demon-
stration of systems on several typical
priority hazardous particle sources.
Documentation of the relative technical
and economic feasibilities of various
systems.  Development of at least one
practical, manual particle-sizing method
and one continuous method for fractional
efficiency determination and control
device performance evaluation.

10.  ROAP 21ADJ - Demonstration and       3                 983      CSL
comprehensive characterization of the
particulate control capability and limi-
tations of the best available full-scale,
utility applications of Fabric Filters,
electrostatic precipitators (ESP's),
and scrubbers by means of thoroughly-planned
and executed demonstration test programs
to examine major variables for at least
three major control devices.  Evaluation
of the particulate control capabilities
of a representative range of commercially
available variations and types of the
three major classes of conventional par-
ti cul ate equipment: fabric filters, ESP's,
and scrubbers on several major sources.

11.  RQAP 21 ADM - Evaluation and docu-     6               2,941     CSL
mentation of the relative capabilities and
limitations of fine particulate control
devices.  This information will permit
selection by equipment users of collection
systems that are technically and economically
optimum for specific applications.
-29-

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                                                   '  -'       • DRAFT
                                                      DO NOT QUOTE OR CSTE
                           Table  S-l  (Continued)

           SUMMARY OF CURRENT  RESEARCH  RELATED TO  FINE PARTICULATES

                                                             1st*
                                        Estimated  Date       Costs    NERC/RTP
             Task Description         of Completion (Yrs)   ($1000)      Lab

12.  ROAP 21ADK - Current, compre-            6               1433       CSL
hensive, and accurate engineering
analysis of all particulate emission
control techniques will  result.   These
analyses will be in the  form of indi-
vidual evaluations of particulate pro-
cesses and comparative analyses  of all
processes of a similar type.  The evalu-
ations will be made using common  method-
ologies to facilitate comparisons.   The
comparative analyses will permit rational
and timely management decisions based on
solid, technical groups; this  will  permit
optimum allocation of resources within
the air pollution control technology area.

13.  RQAP 26ACV - Development  of technology  6               4000       CPL
to measure the emissions from  mobile sources.
Determination and characterization of emissions
both gaseous (precursors) and  particulate.
Development of sampling and analytical  tech-
niques to provide regulating capability and
to provide the basis for effects research.

14.  ROAP 26AAE - Characterization and        6               3000       CPL
protocol development related to emissions
from mobile sources from fuel  and fuel
additives.  Definition of chemical  species
and mechanisms which result from the use of
additives.  Particulates are determined as
appropriate in support of Section 211 of
the Clean Air Act.

 15.   ROAP  21 ADO  - JjodeJlnfl.                    3              120      ML
 Methodologies  developed  for calculation
 for diffusion  of  reactive  pollutant  are
 applicable  to  modeling  secondary pollutant
 generation  and certain mechanisms  have  already
 been  applied to  aerosol  generation.  Scavenging
 and general  removal  processes of fine  particulates
 are studied  in the  laboratory and  in the ambient
 atmosphere.
                                  -30-

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                                                       DO NOT  QUOTE OR CITE
                          Table S-l (Continued)

           SUMMARY  OF  CURRENT RESEARCH RELATED TO FINE PARTICULATES

                                                            Est*
                                       Estimated Date      Costs    NERC/RTP
             Task Description         of Completion (Yrs)   ($1000)    Lab

16.  ROAP 26AAS - Geophysical
Background classification  and monitoring      5                35        ML
of atmospheric turbidity.   Lidar
development and studies.   Evfects  of
aerosols on the radiation  balance.

17.  The following ROAPs  contain one or       5             1,250,    CSL
more tasks which are related to fine
particulate control R&D:   21AFF, 21ADC,
21AUY, 21AFA, 21AQR, 21AFE,  21AVA,  21AFH,
21ARO, and 21BAO.
                                 -30a-

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        Table S-2



SUMMARY OF RECOMMENDED NEW RESEARCH
         -3 1-

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                            Table S-2      QQ  MOT QUOTE OR  CiTE

                    SUMMARY OF RECOMMENDED NEW RESEARCH


                                               Estimated time       Est Costs/yr
      Task Description                        for Completion (Yrs)    ($1,000)

1.  Conduct biological experiments using dynamic        5                500
atmospheres with fine particulate and gases similar
to urban atmospheres for exposure of various
species of animals.  Acute, subacute, and chronic
exposures will be used to determine the significance
of factors such as particle sizes chemical
composition, concentration, and associated physical
properties or canditrans on particle deposition
retention, translocation, pulmonary clearance
rates, and other parameters related to pulmonary
defense,

2.  Identify human biochemical and metabolic            5                200
changes associated with atmospheric levels of
fine particulates.

3.  Conduct community health and environmental          10              1,500
surveillance studies designed specifically to
investigate the health effects resulting from
short and long-term exposure, to fine
particulates  in the atmosphere.  The studies
will consider particle size, chemical
composition, and concentration; as well as
meteorological and population variables,

4.  Characterize and determine the relative             5                500
toxicity as single elements or compounds and
in combination, of primary and secondary
fine particulates from stationary, mobile
and natural sources.

5.  Develop, test, and evaluate sampling,               3               600
measurement and analytical  techniques for
monitoring and physical  and chemical
characterization of atmospheric fine
particulates.

6.  Development and testing of improved                 5               300
fine particulate models.

7.  Determine the fate of fine particles                5               500
in the atmosphere.

8.  Characterization of visibility as an                2               225
indicator of particulate loading, study of
visibility trends, and determination of large-
scale particulate loading distribution and
trends from atmospheric  turbidity
measurements.                    -32-

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                                    DO MOT QUOTE OR CSTE
                                               Estimated time       Est Costs/yr
      Task Description                        for  Completion  (Yrs)   ($1000)

9.  Measurement of fine particles  using                 5               250
satelliteborne instruments.

10.  Update MRI fine particulate source                 2               300
inventory report using recently developed
particle sizing techniques.

11.  Characterization of fine particulates              5               200
from selected industrial sources.

12.  Field testing of selected industrial               5               300
combustion sources for potentially hazardous
pollutants.

13.  Improved ESP collection of fine particulates       5               400
by (1) developing specdal ESP charging section to
take advantage of diffusion charging of  fine
particulate; and (2) modification of high
resistivity dusts using chemical additives.

14.  Construction and operation of a versatile         5               150
fabric filter system test stand for fine particulate
R&D studies.

15.  Construction & operation of a multipurpose fine    5               150
particulate scrubber test stand for fine particulate
R&D studies.

16.  Construction & Operation of versatile mobile       5               300
pilot scale ESP.

17.  Improved fabrics & fabric finishes  for fine       4               150
particulate control.

18.  Develop and evaluate devices, and establish       5               500
measurement protocol, for determining mass,
fractional efficiency, aerodynamic size, and
chemical composition of fine particulate from
stationary sources.

19.  Relationship of sulfate formation to fuel         1               150
sulfur in controlled non-catalyst cars,  modeling.

20.  Sulfate formation in other mobile source com-     4               125
bustion systems, modeling included.

21.  Study of nitrate formation in mobile source       4               190
combustion and post combustion systems.
                               -33-

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                                              Estimated time       Est Cost/yr
    Task Description                          for Completion (Yrs)  _J$1000)	

22.   Expand program on emissions from                   6               125
novel automotive engines.

23.   Develop,  test, and  evaluate sampling,              5               500
measurement, and analytical  techniques
for monitoring and characterization of
fine particulates from mobile  sources.

24.   Study relating health  effects and                  4               125
mobile source emissions.

25.   Define effects of  "smoke  suppressants"             5               180
on mobile source emissions.

26.   Impact of reduction catalysts on emissions.        3                70

27-   Aerosol-gas Interactions  Studies                   3               500
     a.  develop quantitative  theory
     b.  laboratory  studies with collected aerosols
     c.  chamber studies with  dispersed  aerosols
     d.  quantify role  of aerosols in transporting
         nixious material  to pulmonary system
     e.  determine effect of high  humidity in
         pulmonary system on deposition  of hygroscopic
         and deliquescent aerosols.

28.  Characterization of Atmospheric  Fine Particulate   3              1,000
     a.  nationwide  research network  to  determine
         mass and composition  as a function  of  size.
     b.  relate atmospheric aerosol loading  to
         emission sources.

29.  Determination of long-term trends  in aerosol       5              25000
loading and aerosol  sources including $5,000,000
installation cost, $1,000,000/yr operating costs

30.  Visibility Studies                                3                250

     a.  Develop light scattering  theory for non-
         ideal particles.
     b.  determine relationships between visibility,
         light-scattering, and sub-micron  aerosol
         mass.
     c.  determine light absorption  of  atmospheric
         fine particulates.
                                _34-

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                                                 uimi I
                                        00 NOT QUOTE OR  CITE
    Task Description

31.  Transformations  Studies
     a.   Studies in plumes
     b.   Sulfate mechanisms
     c.   Nitrate mechanisms
     d.   Organic mechanisms
32.  Natural  Source Studies
     a.  Sulfur cycle
     b.  Nitrogen cycle
     c.  Carbon cycle

33.  Development of technology  for  secondary
     fine particulate reduction  by  improved
     control  of gaseous precursors  (SOX, NQX,
     ammonia, hydrocarbons,  etc.)

34.  Improved control of fine particulate
     emissions from stationary  sources by cleaning of
     raw materials and/or fuels.

35.  Improved control of fine particulate emissions
     from stationary sources by process modifications.
 Estimated time       Est Costs/yr
for Completion  (Yrs)    ($1000)

          3             1 ,000
                         325
                       2,000
                       1 ,000
                       1 ,000
                           -34a-

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                         I.  INTRODUCTION  -D jUO]
     The objective of this Task Force is to identify problem "areas'
major concern to EPA relative to primary and secondary fine particulates
in the atmosphere.  There is an increasing body of evidence which
suggest that those particulates found in the atmosphere in the size
range less than 5 ym contribute significantly to the adverse effects of
air pollution on human health and welfare.
     The category of fine particulates encompasses the most complex
scientific, technical, and economic problems associated with air pollution
Not only are there fundamental questions which have not yet been
answered, but in certain areas our knowledge is so limited that questions
cannot be properly formulated.  No attempts have been made here to
present an in-depth scientific treatment of fine particles as specific
chemical elements or compounds.  Rather scientific discussion is limited
to that extent considered necessary to identify the major problem areas
which may impact on the need for Agency decisions.  In the final
analysis, a pollutant category of fine particulates, as opposed to a
classification by chemical species, may prove to be too arbitrary and
hence impractical from the standpoint of effects criteria.  Currently
available data indicate that consideration of particle size alone
in health effects research would be inadequate.  Chemical composition
and other associated physical properties appear to be equally important.
From the standpoint of control technology—and to a certain extent
the effects upon visibility, weather, and climate--the size
classification of fine particulate appears to have distinct
advantages.  This problem of pollutant classification is considered in
the report but not resolved.  Further research will be required.
                              -35-

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                                                             ABC
                                       DRAFT
                               DO  *;cT QUOTE or.:

                  II.   CHARACTERIZATION METHODOLOGY

A.  Definitions
         The following  definitions  have been  used arbitrarly through-
out this report:
    1,  Fine particulate matter is  defined as "material that exists as
        a solid or liquid below the size  of 2 to  5 urn  in diameter," as
        measured by aerodynamic and/or  optical  techniques.   For design
        purposes, a cut-off of 3.5  ym diameter  is considered acceptable.
    2.   Primary fine particulate is defined as all  "fine particulate which
        has  not been modified by atmospheric transformation
        processes."  (Change of physical state is  not considered a trans-
        formation process.)
    3,   Secondary fine  particulate  is defined as "fine particulate  that
        is formed or modified
        by atmospheric  transformation processes."
    4.   Physical  particle  size  is the shape and the dimensions of the
        particle.
    5.   Aerodynamic  particle size is defined as the size of a sphere of
        unit density which  has  identical aerodynamic behavior as the
        particle  in  question.   Particles having the same aerodynamic
        particle  size may  have  differing shapes and dimensions.
B.  Particle Sizing  Methods
     Techniques for  determining  the size distribution of aerosols can
be classified broadly as those  based on the physical particle size and
those depending on the  aerodynamic  particle size.   Microscopic and other
                                -36-

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                                             NOT QUOTE OR CITE
optical methods determine the physical  particle size while  the inertial
devices such as impactors, cyclone separators,  diffusion  batteries, and
centrifugal devices determine the aerodynamic particle  size.   Electrical
devices,while  more complex in the principle of separation,  respond to a
combination of aerodynamic and physical size,
1.   Microscopic Methods
     The particulate matter is collected on glass  slides  or  membrane
filters.  The individual particles are viewed with a microscope
and subsequently sized with a reticule and counted.   The  lower limit
of resolution is about 0.5 ym in diamter, unless an  electron microscope
is used.
2.   Aerodynamic Fractionating Devices
     These devices fractionate particles by virtue of their  aerodynamic
dimension, electrical charge, or mass, and with some devices retain the
aerosol material for physical, chemical or microscopic  analysis.   The cyclone-
type sampler  is an aerodynamic fractionating device in which vortex of air
increases  the centrifugal force or, the entrained particles  which throws  them out
of the gas stream, at which point they either stick to  the  walls or drop
into a container.  This type of sampler is somewhat limited in that as the airflow
is increased to impart a greater centrifugal force to the entrained
particle,  the increased airflow also .-causes turbulence, which interferes
with the centrifugal force of the particle.
     Rotating centrifugal devices have been developed to collect particles
smaller than those collected by cyclones and separate them according  to
size.  Particle collection in rotating devices is limited by geometry and
airflow.   To get around these limitations, devices have.been designed
that increase centrifugal force of the entrained particles while permitting

                                   -37-

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                                                 DO NOT QUOTE ฉR -CITE
airflow within the.instrument to  remain  low enough  for  laminar  flow.
     Cascade impactors are used for determining  weight, number,  and  chemical
composition distributions.  Several  stages  are used in  series,  each with  a
different air inlet geometry, resulting  in  progressively increasing air
velocities with descending stages.   Particles with  a large  aerodynamic
mass are impacted and retained on the  upper stages  where the  particle
velocities are low,  while those with small  aerodynamic  mass are impacted
on the lower stages where the particle velocities are higher.
     Electrostatic fractionators  separate by means  of passing charged
particles through a strong electric field.   The  collection  efficiency
increases with smaller particle sizes  because of their  greater  mobility.
This makes the fractionator quite valuable  for the  collection of submicro-
meter-size particles in the range of 0.005  to 0.5 ym.  The  flow rates are
insufficient to collect an adequate amount  of material  for  chemical or
gravimetric analyses.
     Diffusion batteries,coupled with an  appropriate particle
counter>are used to measure particle size distribution in the
0.005 to 0.1 ym range.  In a diffusion tube, smaller particles
migrate to the wall through Brownian motion and larger particles
traverse through the tube.  By changing tube diameter, tube
length, and gas flow rate, the minimum size of particle penetrating
the tube can be varied and the number penetrating counted.  The
data can then be converted to a number size distribution.
3.  In-situ Optical Sizing Devices
     Several types of devices for physical particle sizing have been developed
based on light scattering,  However, the only ones that can be classed as
particle size instruments for airborne aerosols are "single particle
                                  -38-

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counters."  With these devices, the particles pass through a light
beam one at a time and the size of the particle is determined
by the amount of light scattered.  Other approaches are proposed
or have been used on a research basis such as multiwave length  light
scattering, angular scattering device, laser backscattering, and
polarization light scattering techniques, but instruments  based on these
principles are not generally available.
     Devices such as the integrating nephelometer that measures only
the total scattering o
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    conditions are not too severe.  Comparison of results measured before
    and after a particulate control device makes possible the estimation of
    the fractionating efficiency of tne control device.
        c.  Mobile Source.    A dilution tunnel is used to simulate the
    atmospheric dilution, that naturally occurs, and to lower exhaust temp-
    eratures and dew points at high engine speeds.  This allows formation of
    particulate by condensation before sampling.  Dilutions are normally
    10-20  to 1 (to maintain as high concentrations as possible for the sake of
    analytical measurements) rather than the roughly 1000 to 1 in the ambient
    atmosphere.  The sample to be sized is taken from the dilution tunnel.
        This technique  is particularly important on emissions from vehicles
    operating on fuel that does not contain metallic additives.  It has been
    widely applied to automotive exhaust emissions and is currently being
    extended to other mobile sources.
         Cyclic operations are necessary to duplicate normal emission patterns
    since  the  rate of emission is extremely dependent on operating mode.
    Fixed  cycles are required  in order to allow duplication of results
    and facilitate inter-laboratory comparison.

C.  Chemical Composition
         Compositional analysis is performed by a wide variety of techniques.
    X-ray  fluorescence,  atomic absorption  spectroscopy, optical emission
    spectroscopy, and wet chemical methods have been used for elemental
    analyses.  Liquid chromatography, infrared and ultraviolet spectrometry,
    gas chromatography,  mass spectrometry, fluorescence, and wet chemical
    techniques have all  been used for detection and measurement of organic
    components.   In most cases, two or more techniques are  used in concert
    because of the large number of compounds present.
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o.  Prob^reas                      DO NOT QUOTf OR fSTF
     The following are problem areas and/or needs  requiring  further
studies in the measurement area:
     !•  Calibration of size classifying devices  has  always  been difficult.
Ideally, such devices should be calibrated by atmospheric particulate
matter of heterogeneous composition and known size; such material is not
yet available,   and  is an important research need. Consequently.
laboratory aerosols consisting of polystyrene latex spheres, methylene
blue solutions or other liquid aerosols, or other homogeneous materials
have been used.  These synthetic aerosols are very much  unlike atmospheric
particulate matter and probably do not exhibit the same  aerodynamic,
optical, or other properties of atmospheric particulate  matter.
     2.  Cross-comparison of different in-stack cascade  impactors has
been made by one contractor at a given site.  Under carefully controlled
conditions, reproducibility between types of impactors was  reasonably
good.  However,  few  runs have been made and analyzed  to  compare:
       a.  different operators using the same impactor on the same source;
       b-  duplicate  impactors on the same source used by the same
          operator;
       c.  the same impactor used in different locations  in  a given stack
          or duct.
     3.  Cross-comparison of optical, aerodynamic, and  electrical sizing
devices has not  been adequately done. Controlled experimental  facilities  are  nc
available.
     4.  Cascade impactors are subject to error because  of  particle  bounce-
off, re-entrainment, wall losses, and particle size changes either due  to
chemical reaction or moisture content changes.
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 5.   All extractive techniques used for source sampling  have  the  oroblern of
 getting  a  truly representative sampling through the sampling interface
 to  the  collection device.   Wall  losses,  aaalomeration,   particle fractionation
 and preferential  loss of one size of another are some of the problems
 encountered with  the sampling interface.
 6.   Conventional  impactors  isolate extremely small samples making
 anything other than selected elemental and/or microscopic analyses
 difficult.  Four  newly developed, larger size cascade impactors are
 available  for ambient air  sampling which collect sufficient material
 for gravimetric and chemical analyses.  These impactors have not been
 adapted  for in-stack use.
 7.   Impactors operate over  a fairly narrow range of flow rates and are
 difficult  to use  in gas streams with heavy loading because of rapid
 overloading of one or more  stages or with very light loading because
 of  the  long testing times nesessary to take an adequate sample for
 weighing.
 8.   Optical and some electrical sizing devices take large dilution
 with pure  air to  reduce particle loading to a measurable level.
 9.   No  particle size distribution  tests  have  been standardized with
 any of  the sizing devices available.   Each group with a need  tends to
 go  its  own way.
10.   Manual devices are time consuming  to operate  and are not  able
 to  measure short-term changes in control systems  operation.   There is
 an  urgent  need for devices  that can provide size  distribution data on a  near
 real-time  basis.
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11.  Filtration techniques must be accurately defined and evaluated.
Absorption, condensation, and evaporation  of volatile materials cause
serious errors.  Surface reactions may  also  be very  important.
12.  What is a "particulate" must be defined in  each instance.  No
definition is all inclusive.  Specific  analysis  often ignores the
distinctions between particulates and gases. Conversely, adverse health
effects are more dependent upon composition  than physical state.
13.  Convenient measurement techniques  are required  for  all mobile
sources.  Current techniques are cumbersome  and  expensive,  both in  time
and equipment.
14.  Mass measurement techniques, at least as  applied to mobile
sources, need  to be improved to provide increased sensitivity and
convenience.
                               -43-

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                         T
                          III.  ATMOSPHERIC INPUT



A.  STATIONARY SOURCE EMISSIONS AND CONTROL


                                                       DPA-
1.  Emissions                                 r._      '--" s 5,;J•{:  I


    :	~  t                              t;'J NOT QUOTE OR CITE
a.  Present Status^-



     Data on the emissions from stationary sources are needed  for two



purposes — to determine the atmospheric input from these sources and



to permit the proper application d'f control technology to reduce the



emissions.  Both particulate emissions and gaseous emissions,  (SOX,



NO , hydrocarbons, etc.) from which secondary particulate form,  are
  A


important.



     Estimated or measured emissions of SO  and NO  from each  point source
                                          X       A


in the nation, which emit more than 25 tons/year of either of  these pollutant



categories, are available from the National Emissions Data System (NEDS).



Mass emissions of hydrocarbons and particulates are also given in this data



base, but no attempt is made to identify the chemical composition of the



pollutants nor the size distribution of the particulates.



     In  1971, Midwest Research Institute (MRI) completed for EPA a three



volume "Particulate Pollutant Systems Study."  Volume II, "Fine Particle



Emissions", gives an estimate of 1970 emissions from stationary sources



as about four million tons of material with particle sizes of less than



3 urn diameter of which about one million tons consisted of material



with particle size smaller than 1 pm diameter.  These estimates



were based on major extrapolations, because of the lack of actual  data



in the  fine  particulate  range.   During the  past year,  techniques  have been



utilized  which are capable of  measuring  particle  size  distributions  down



to 0.2  ym using  inertia!  impactors,  and  to  about  0.01  urn  with  diffusion



batteries.   In recent months,  nearly fifty  sets  of particle  size
-44-

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                                             DO NOT  QUOTE OR CITL
measurements have been made down to 0,2 ym and  several  to 0.01 ym.  MRI is
currently upgrading the particle size distribution  data.  An automatic
stationary source particle sizing device that couples  the beta gauge and an
inertial impactor has been developed and is in  the  final phase of testing.

b.  Planned R&D
     It is imperative that a better data base for fine  particulate emissions
from stationary sources be developed.  This will be  done by utilizing particle
size distribution data, developed in recent months  (fine particulate range),
that which will be obtained from currently planned  and  funded programs, and
that which must be obtained to fill in the gaps  and  will take additional
funding.  A complete update of the MRI Fine Particulate Emissions report will
take about 2 years to complete.  However, accuracy  of  our data base will
continue to improve throughout the 2 years.
2.  Control
     To insure that those atmospheric fine particles which may be
determined to have serious health or welfare effects can be controlled an
                                    -45-

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active control  technology development  program  must  be pursued  which
aims at primary fine participate and the gaseous precursors  of secondary
fine particulate.
         a.   Primary Fine Particulates
             (1)  Present Capability
                  Fine particulate control  technoloav
is now at a very early stage of development.   Exceptions  exist where
collection systems have reached very high mass efficiencies  resulting in
capture of fine particulates along with large  particle size  material.  Recent
tests have shown that under certain  limited conditions, an ESP or a  baghouse
can control  fine particulate flyash.  One high efficiency ESP  (99%+  overall
efficiency) was found to be more than  90% efficient in the mass removal  of
all particulate fractions down to about 0.01   urn.     Unfortunately, much
of the coal  burned in this country produces flyashes having  electrical
properties which fall outside the range where  ESP capture is most effective.
Either modification of the ESP or the  flyash (or both) will  be necessary
to capture the fine particulate.  In addition, fine dusts from many  sources
not associated with fossil fuel burning are difficult to  collect electro-
statically.
     A baghouse has recently been installed on a coal-fired  utility  boiler
and has been shown to effectively control fine particulate,  at least down
to 0.2ym.  However, the development  of special operating  techniques  and
improved filter fabrics will probably  be necessary  to significantly  broaden
the applicability of baghouses for fine particulate control.
     High energy scrubbers also are  capable of fine particulate control  on
certain sources, but suffer from the disadvantage which their  name implies
(high energy consumption).
                                    -46-

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                                       r\f\ ซซซ"ป•ป•'•
              (2)  Current R&D Activitfe?  '-JOT
                   Particulate control technology consists of add-on
 collection devices, fuel or raw material cleaning and process modifications.
 Basic technology for collection devices can be developed independent of the
 sources.  The latter two technologies and the specific aoolication of collection
devices must be developed for the applicable industry.  Therefore, two programs
for particulate control technology are possible - R&D on collection devices and
R&D aimed at reduction of oarticulate emissions from ป*ch source ^P6-
      Currently both programs have been established.  The particulate control
 device program has the following objectives:
      4.  To establish a data and technology base to assist manage-
          ment in decision making on fine particulate R&D.
      b.  To  assess      the collection capability of conventional
          control devices using standard sources of fine particulate
          emissions.
      c>  jo  assess      the collectability of dusts from the
          major sources of fine particulate using standardized
          collection devices.
      d.  To identify, evaluate and develop new concepts and novel
          devices which  show promise for control of fine particulate.
      e.   To demonstrate the use of high efficiency collection
          devices on major sources.
 The source oriented program has the goal of selecting and demonstrating
 the most promising control technology for combustion sources, the metallurgical
 industry, the chemical  and petroleum, industries, open sources, etc.  Emphasis
 in these programs  is to control all emissions from the source including
                                      -47-

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                                                            r






particulate emissions  with  emphasis  on  potentially  hazardous pollutants.



        b.   Secondary  Fine  Particulates




            (1)   S0.x



                 Sulfates found  in  secondary  fine particulate,  appear to




come primarily from/atmospheric  oxidation  of  S02 to S03.   Reduction  of



sulfates to an acceptable  level  will  probably require  reduction of SOX




emissions by 90-99%.



     The current EPA program is  targeted  at moderate (30-70%)  reductions of




ambient concentrations of  S02 in urban  areas.  This will  be accomplished



by using stack gas cleaning on large point sources  (75-90% abatement) and



cleaner fuels on most other sources (20-60% abatement).   To achieve 95%



reductions  of ambient concentrations of SO,,  in urban areas, large point



sources will require high  efficiency stack gas cleaning  (90-99%) and other



sources will require increased use  of clean  fuels.



            (2)   NO^



                 Nitrates  in the atmosphere  are generally formed from NO
                                                                        X


emissions.   Adequate control of atmospheric  nitrates may require reducing



NO  emissions by 90% or better.
  X


     NO  control by combustion modification  (present program)  can achieve
       A


reductions  of 50% to about  80%.   Reduction of NO  by better than 80% will
                                                X


require major combustion process modifications.  Fluid bed combustion and



catalytic combustion may have high  potential  here.



            (3)   Hydrocarbons




                 Although  significant reduction in  the emissions of reactive



hydrocarbons from many  stationary sources 1s  possible vfi.th. application  ฐf  existing
                                    -48-

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    technology, there are numerous industrial sources where adequate  control
    has not been demonstrated.
            (4)   Other
                 Other gaseous pollutants,such as ammonia,  can increase
the reaction rate  for formation of secondary  fine particulates.  These
pollutants must be identified, the sources  and levels  established, and
control techniques developed and applied.

     3.  Problem Areas
         a.  In order for the agency  to make  decisions with respect to the
             control  of fine particulate  matter, it  is necessary to establish
             immediately a better data base on the physical and chemical
             characterization of fine particulate emissions from stationary
             sources.
         b.  To establish what important  gaps in the  technology base must
             be filled, a rapid characterization of  the collection efficiency
             of conventional particulate  control devices is necessary.
         c.  In order to identify difficult control  problems, the character-
             ization of the collectability  of various  industrial dusts
             must be accomplished.
         d.  New concepts and devices for collecting  fine  particulate
             matter must be identified, characterized  and  developed.
         e.  The best applicable technology for  control of fine particulates
             must be demonstrated at  the  earliest possible date on an
             industry~by-industry basis.
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f.    Strategy arrd methods  for  the control of gaseous precursors of

      secondary fine particulate matter emitted by stationary sources

      (SOX, NOX, hydrocarbons,  NH3, etc.) must be developed.  Before

      the magnitude of the  necessary effort,here can be determined,

      we must know the level  of control required.
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B.  Mobile Source Emissions  and  Control
1-  fiftnerftibneCsourcSs  contribute  only  about 3% of the total particulate
    emissions in the U.  S.   However,  this  is all in the fine particulate range
    and may constitute a significant  fraction of total primary fine particulate
    emissions.  Moreover, atmospheric transformation of the gaseous emissions
    from mobile sources  accounts for  a major fraction of secondary fine
    particulate matter in some urban  areas.
         The major contributor to particulate emissions from mobile sources
    is the passenger car (45.8%) due  mainly to  the large number (87 million)
    in daily operation and not to a higher emission rate (0.3g/mi) than other
    forms of mobile sources.  Trucks  and buses  account for another 15% and the
    rest  is split up among the wide variety of  other  sources:  aircraft,
    locomotives, lawn mowers, earth movers, etc.   Emissions  from all mobile
    sources amounts to 600,000 tons/year.
          In a study for EPA by the Dow Chemical Company, it  was found that
    particulate matter in automotive exhaust  had  a MMED of  <0.1ym  and
    the size  range observed in a series  of tests  was  3.2y to <0.1ym.   Nearly
    all studies to date on the particle  size  distribution of automotive
    exhaust indicate that 90% or more of the  mass emitted consists of particles
    with  diameters below 1 micron and thus the  total  particulate emissions may
    be considered as fine.
          A significant fraction of atmospheric  aerosol  results from atmospheric
    oxidation of S02 and NOX to sulfate and nitrate  and  from oxidation  and

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                                        K) HOT QUOTE OR CiTE
polymerization of gaseous  organic  compounds  to  carbonaceous  residues.
In areas where automobiles are  important sources of these gases,  part of the
secondary pollutants  will  also  belargely   mobile-source derived.  Nitrates and
sulfates account for  about half the  fine particulate material present in
the L. A. atmosphere  and may be derived largely from  automotive sources.
Estimated emissions rates  for gasoline-powered  vehicles  burning fuel
containing usual quantities of  tetraethyl  lead  (2.5 gm.  Pb./gal.)  are in
the order of 0.08 to  0.25  grams/mile in a  typical consumer driving pattern.
     Lead-free gasoline will  be required in  cars equipped with  hydrocarbon-
control catalysts since lead emissions  quickly  deactivate catalyst.   With these
lead-free fuels and catalysts,  particulate emissions will be in the 0.02 to
0.05 gram/mile range  and may be dominated  by nitrates  and sulfates.
     Diesel smoke has been controlled by many modifications  to  combustion
systems, reduction in fuel injector  volumes  and addition of  turbocharging.
However, attempts at NOX control  have introduced a design trade-off with
smoke control and turbocharged  power output.
     Emissions from aircraft turbines are  significant  in some areas.
Estimates of Los Angeles turbine particulate emissions are 1/3  to  1/5 of
automobile-generated particles.  In  areas  near  approach  and  take-off  corridors,
aircraft particulates dominate  the atmospheric  aerosol.  Particulate
emissions range from 0.1 to 2%  of the fuel  burned, depending on engine type
and operating mode.
                                -52-

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2. Problem Areas                                 '  " NฐT  CM ft OR CUE
       There 1s a need for more effort and data on the particulate emissions
  from mobile sources.  Some of the specific types of .data needed are more
  and better size distribution data, as well as chemical composition of
  particulates, and better mass emission data for the lesser known sources.
       Fine particulates from mobile sources have not been specifically
  regulated except as visible smoke from heavy duty engines.
       Some specific problem areas include:
       1.  Reliability of particulate data is in question because of
  difficulty in collecting volatile components which behave as particulate
  matter.
       2.  There is  not at the present time an absolute filter for automotive
  exhaust particulate and thus nothing for use in determining true emission
  rates.   Reported  results can be low but not high.
       3.  Adequate  instrumental methods are lacking for determination of
  particle sizes below  0.1 ym, which accounts for a significant portion  of
  automotive particulate emissions.
       4.  A better  definition of the composition of particulate matter from
  engines will be necessary in order to take into consideration the variable
  volatility of many high-molecular weight organics present in the exhaust.
       5.  Better instruments are needed with more availability
  for conducting wider surveys of the automobile population for better
  monitoring of emission trends.
       6.  Better methods are needed to reproduce driving conditions to remove
  that variable from the analysis mobile source emissions data.
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     7.   Smoke  is  currently regulated as a nuisance.  Since it may be
largely  carbonaceous participate matter, which could include polynuclear
aromatics,  its  composition must be        ascertained.
     8.   Better emission  factors are needed for all classes of mobile
sources.  The emphasis  should be on composition as well as mass and size.
Most sizes  are  very small and undoubtedly are sites for further nucleation,
agglomeration,  etc.
     9.   Inorganic precursors to secondary aerosol formation must be
determined.  Their composition as emitted will play a significant role.
Differentiation between sulfate and sulfur dioxide, nitric oxide and
nitrate, elemental metallic and soluble salts, are all examples of the
problem.
     10.  Gaseous  emissions must be elucidated and their emission factors
determined since many of  these are precursors to secondary aerosol.
     II.  The effect of control devices for regulated emissions must be
determined.  Thus  catalysts for control of total hydrocarbon and carbon
monoxide are likely to  increase the conversion of S02 to sulfate.

     12.  The environmental impact of all control strategies must be
determined.
     13.  Studies  are needed to determine the effects of fuel additives
on particulate  emissions. (For example, the use of a manganese-containing
smoke suppressant  increased the mass of particulate emissions while
reducing other  visible  smoke. )
                                   -54-

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     14.   Novel  engine  designs, such as Wankel rotary, stratified  charge,
and gas turbine  must be evaluated for changes in composition and mass
of emissions. (For example,  the rotary engine uses oil more intimately
mixed with the combustion  process, which can potentially produce different
type emissions including carcinogenic organic compounds. )
                                -55-

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                                                    as-
C.  NATURAL SOURCES                     00  ,V"ปT rM^v    -
                                        —  KUI  QoufUR  CITE
] .  General Discussion
     Much of the fine parti cul ate  matter in  the  atmosphere  results  from
emissions by natural  processes.  These processes yield  both primary
partlculates, such as those from volcanism or forest  "fires, and
secondary particles,  such as those from conversion  of gaseous sul fur-
or nitrogen compounds.  The most important natural  sources  for direct
emissions of fine particles include forest fires, wind-blown  dusts
volcanic activity, and sea salt.
     Natural gaseous  emissions of  H2S, NOX,  NH3  and hydrocarbons  are
transformed within the atmosphere  to sulfate, nitrate,  ammonium
and hydrocarbon aerosols.  Specific sources  of these  gases  include
plant exudations, biological activity and volcanic  activity.
     Data on the emissions and rate of formation of natural aerosols
are rather meager, and there is not complete agreement  among
different  information sources,  Although some data  are  available  for
particular volcanic events or dust storms, little detailed  information
exists on  the time and space variability of  the  secondary formations.
On the global scale,  some crude estimates of natural  emissions have been
made.  These estimates show that the  worldwide  contribution  from  natural  sources
to atmospheric  paniculate in  the  size range less than  20 pm  in diameter
is about 1-2 x  10^ metric tons per year.
2.  Probl em Areas
     Additional  quantitative and qualitative data are needed  in the following
areas:
     a.   Origin.^of natural aerosols.
     b.   Inventory of primary and  secondary  fine parti cul ate  from
                                " -56-

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     natural  sources.  This should include size distribution,
     concentrations, and chemical  composition.
c.   The temporal and spatial variability of fine particulate
     from natural sources.
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                IV.   ATMOSPHERIC  LOADING
A.  INTRODUCTION
    The atmospheric  loading  of fine  particulates is determined by
the rate of atmospheric input of  primary particulate pollutants
and gases, the rate  of transformation  of pollutant gases into
particles, the transport of  primary  and secondary pollutants through
the atmosphere, and  the removal processes which are a function of
particle size and composition.
B.  TRANSPORT AND PREDICTION MODELING
    The transport and resulting concentration of pollutants can be
predicted by meteorological  or diffusion models.  The modeling of
fine particulate concentrations can  be separated into two  categories
based upon the sources of the particulates.  To the extent that
the fine particulates may be considered inert, all the  existing
modeling techniques  for hourly, daily  and  longer term average con-
centrations are applicable.   The  largest difficulties in modeling
inert particulates are in determining  the  emission locations and
strengths.  It is more difficult  to model  pollutants from  mobile
sources than stationary sources.   The  mobile source is  so  close to
the ground that in most cases it  does  not  emit into a representative
wind field.

    Research is needed to determine mechanisms for dealing with mobile
source emissions in a general manner.  One expects, for example,  that
                               -58-

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the distribution of fine participates issuing from mobile sources
would be expected to have a very large degree of spatial  variability
on a very fine scale across a city.
    Much more difficult however is the modeling of fine particulates
which are secondary pollutants.  In order to accomplish this,  it is
necessary to fully understand the mechanisms of secondary particulate  genera-
tion.  Once these mechanisms are delineated it is possible to  model
their-, generation and transport. The state of understanding regarding
particulate formation however is not advanced to the point of  being
included in any transport and transformation models now available.
    An additional consideration regarding fine particulates is  their
interaction with the humidity field of the atmosphere.  Through this
interaction it is possible to affect the radiation budget as well
as the local precipitation.  Due to the significant interaction of
the fine particulates with water vapor it will be necessary to model
the water vapor field over a city-  There is currently no work in
this important area, although consideration is being given to  including
moisture processes in some dynamical models.  Again however the ques-
tion of how to treat these matters in a routine fashion with a general
approach will require some significant research.
    Finally the removal of fine particulates will be a problem of
relevance to the modeling.  The questions of how particulates  get
removed and whether these removal rates are dependent on  land use,
surface foliage, and other factors must be investigated.
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c.   TRANSFORMAT.ONS                            DO NOT QUOTE. OR CITE
     A significant component of the sub-micrometer particulate  is secondary
particulate formed in  the atmosphere by chemical reactions which convert
gases into solid or  liquid  particulates.
1.   Sulfates
     Sulfate, in the form of sulfuric acid  (H SO.), ammonium bisulfate
(NH4HS04), or ammonium sulfate KNH^JgSO^J, is formed from both natural
and man-made emissions of sulfur  compounds.  There are a number of
postulated mechanisms  for the conversion of"S02 to sulfate.  The only
one which has received extensive  study, the direct photochemical oxidation,
has been shown to be of little significance in urban situations.
2.   Nitrates
     The ultimate fate of gaseous NOx is presumed to be gaseous or
particulate nitrate.  Both  organic and  inorganic nitrates are found.
Nitric acid  (HN03)  is thought to  be an  end  product.  However, the
reaction forming HN03 occurs on or in particulates.  The  total  nitrogen
oxides, gaseous and  particulates, present after significant photo-
chemical reactions,  accounts for  only a fraction, 20-40%, of the
nitrogen oxides emitted or  present at the start of the  reaction.
3.  Organic  Particulates
     Unsaturated organic vapors,  olefins and aromatics, react in  photo-
chemical smog to giye an enormous variety of oxygenated organic matter.
Some primary organic particulates also  is  emitted  by stationary and mobile sources
4.  Ammonia
     Ammonia plays an important  role  in the formation  of  sulfate  and
nitrate particulate  by neutralizing the acid species  formed.
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5.  Particle Size
    Smog chamber and atmospheric studies indicate that secondary
participates exist almost exclusively in the sub-micron size range.
This size range penetrates into the lung, and is also responsible
for visibility reduction.
6.  Properties
    Secondary particulates are generally hygroscopic or deliquescent.
At low relative humidities, they may have a coating of adsorbed
water.  At higher relative humidities, they may grow in size and
become solution droplets.  Solution droplets or particulate with  a
liquid surface may play a key role in determining the rates and
mechanisms of gas-phase pollutant transformations.   For example,
the conversion of NOX to HNC>3 is probably controlled by surface
reactions.  It is also possible that the primary lung dosage of
gaseous pollutants, especially $62, may be due to transport to the
lungs on or in particulates.
7.  Problem Areas
a.  Mechanisms and Rate Constants
    Quantitative relationships between sulfate, nitrate, ammonium,
and organic particulates formed by gas to particle conversions and  their
gaseous precursors are critical to development of models and a
meaningful control strategy for this group of fine particulate.
Mechanisms and rate constants must be determined through smog chamber
and atmospheric studies.
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b.  Water Vapor Effects
    The effect of relative humidity and absolute water vapor content
is known to be important for sulfates.   However, there are no similar
results for nitrate, lead, or organic .particulates to use in drawing
conclusions on the relative importance of water vapor on particle
properties.  The state of such particles is of importance not only
for visibility but also lung penetration and biological  effects.
c.  Lung Deposition
    Present lung deposition curves are based on inert particles.
Secondary particles, however, tend to be hydroscopic or deliquescent.
They will grow in the high relative humidity of the lung.  The
fraction deposited will be higher and the point of deposition may
be different than would be predicted by present lung deposition curves.
d.  Gas -Part'leul aฃfe T^ctlpns_
    Secondary par'tTeuTates, especially those with, wet surfaces or liquid
droplets, will promote gas-particulate reactions and dissolve various n*s
phase pollutants.  These gas-particulate reactions are thought to plav an
important role in atmospheric transformation processes; but because
of the difficulties involved in studying such reactions, little quan-
titative data has been obtained.
 D.   NATURAL REMOVAL PROCESSES
 1.   General
    Particles are removed from the atmosphere by fall-out, rain-out,
wash-out, and impaction on or diffusion to surfaces.  Of these, only
rain-out appears to be effective with fine particles.
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The theoretical base for understanding  the  joint  processes of coagulation
and condensation as particles  grow into the fine  mode  is just being
developed.  At the present time, removal  rates  for fine particles
cannot be predicted.
2.  Problem Areas
a.  Agglomeration
     Changes in particle size  under real  atmospheric conditions in
urban atmospheres is unclear.   Coagulation, condensation, and gas-
particle reaction all play a role in determining  the size-composition
distribution.
b.  Removal Rates
     The rates of removal of particles  on a regional scale is not at
                                                                  ~2
all well quantitated.  Analysis of non-urban versus urban S02 to SO 4
ratios indicates a slow rate of removal in  the  Northeast region of
the U. S.  Long range transport into Canada and the North Atlantic
                                        2
for some particulate species such as SO ฃ  is  indicated.  We
know essentially nothing about removal  of organic particulates on any
scale of distance.
E•  Physical and Chemical Characterization  of Ambient  Air Particulates
1.  Size-Distribution
     Early studies of ambient  particulate used'five-stage impactors and
found that the size distribution could  be adequately accounted for
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                                                                  E
by a log-normal distribution.   However,  in recent years counting
techniques and eight-stage impactor studies have demonstrated a
bimodal  size distribution  in some  locations.
    Most particulate scientists  agree  that the  atmospheric  particulate  is
 multi-modal  with a  variety of particulates  from different  sources  and
with  different properties.  However, it is a convenient hypothesis
 to consider  the  atmospheric particulate   as composed of two  distinct size
 classes of particulates.   In  addition to  being  a  useful concept for
 organizing data  and theories, it  has  both an experimental  and a
 theoretical  basis.
      There are two  basic  mechanisms for creating  new particles  in  the  atmosphere
 nucleation and gas-particle conversion produce  very small  particles
which  grow by  coagulation  and condensation.  As these small  particles
 become  larger, the  growth  processes slow  down and virtually  cease
 as the  diameter  approaches one  micron.  Comminution or mechanical
 processes  such as breaking condensed matter into  smaller particles by
 grinding,  rubbing,   etc.,  produce particles with  a mass
 mean  diameter  much  greater than one micron.  The  resulting atmos-
 pheric  distribution in  terms  of number, surface,  and volume  is  shown
 schematically  in FigureIV-1.The lower mode may  be called the optical
 mode  since it  covers the  size range most  effective in  scattering light,
 or the  accumulation mode  since  smaller particles  grow  into this size
 range.   Particles in the  lower  mode are also within the respirable
 size  range.
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                        SMOG 8IKE DISTRIBUTION
              .OOl
                      .01
                                                      100
Figure IV-1.   Number,  surface grea, and volume distributions of a
hypothetical  smog.   The  linear ordinate normalized  by  total number,
area, or volume  is  used  so that the apparent area under the curves
is proportional  to  the quantity in that size range.
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                                                         n'tniT f<.'-  rsiP
                                                         I,) JUSt Ut'i  t'l ( H
2-  Compos 1t1Ton and Concentration
     Although the concentration  distribution  between  fine and  coarse  particles
in the ambient air has not been adequately measured,  considerable information
about the composition of the fine particulate mode can be obtained.
by observing composition as a function  of impactor stage.  The major
body of data comes from the National  Air Surveillance Cascade
Impactor Network.  Other data have been obtained  by research groups.
These data indicate that among the metals,  Pb and V
are found primarily in the fine  particulate mode; Fe, Mg, Mri,  Ba, Cd,
and Cr are found primarily in the coarse particle mode.   SO^,  N0=, Carbon,
Cl, NHj, and organic particulate are found in the fine particle mode and
P0| in the large particle mode.   Zn,  Cu, Ni,  and  Sn do not fall  firmly
in either mode.  However, the data are  sparse, and limited to'a few
locations.
     Studies  in  which complete analyses of atmospheric particles have
been made  (in  a  limited  number of locations)   indicate that fine  particles
comprise  25-60%  of  the  total  suspended  particulate matter and that from 60
to 80%  of  the  fine  particles  are  secondary.
3.  Problem Areas
a.  Sampling
     We do not know how to collect a  representative atmospheric sample.
Solid particles are a minor problem.   However, liquid droplets may
pass through a filter, they may evaporate as  the  concentration in the
vapor changes, or the process of interacting  with a surface may cause
them to evaporate.
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     The extent of conversion of S02 to sulfate on filter  media  has
been reported for some individual situations but not systematically  inves-
tigated.  Conversion on filters used routinely versus those  on optimum
filter substrates need to be determined.  Similar problems may exist
for nitrates but no investigations have been conducted.  Organic
particulates can be lost ^eadily from filters.  This problem has been
under investigation for particulates produced from combustion of non-
leaded gasolines in motor vehicles.  The metastable characteristics
of atmospheric organic particulates were reported many years ago but never
subsequently investigated from the standpoint of quantitating mass
or compositional changes.  When  this problem is combined with the
inefficiency of the routine benzene extracts for polar organic
particulates,  it appears that organic particulate concentrations
in the atmosphere may be grossly underestimated.
     Atmospheric particulate samples must be collected in  the presence
of gases which tend to be absorbed on most filter papers.   New  filter
media and collection methods need to be developed.  These  must  be
appropriate for use with current and anticipated analytical  methods.
These sampling techniques must be properly calibrated and  verified.
b.  Measurement Techniques:
     Current programs for the development of X-ray fluorescence and improved
collection devices  should make it possible to  rapidly and inexpensively obtain the
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elemental analysis of large  numbers  of  samples by particle size for
short time intervals.  However,  for  the lighter elements, C, 0, N, and
S problems still exist.  Also,  the elements  associated with soil
background, Si, Al, K, Ca, etc., have not  been routinely analyzed so
results for many of these elements are  available from only a small
number of particulate samples.   Elemental  analysis, however, is in
good condition compared to compound  analysis.  We need to know
whether the sulfur is present as H2S04, NH4HS04, (NH4)2S04, Na2S04,
or other compounds.  Similar considerations  exist for nitrate  an(j for metallic
elements  present.  Organic compounds  present an even more formidable problem.
c.  Particles are not Homogeneous
    Analysis of particle sized fractions provides no information on
the composition or structure of individual  type of  particles.  The
surface layers of particles, their solubility  in mucous, etc., may
be of particular significance.   However, there is very little pub-
lished literature on such particle properties, and  detailed investi-
gation of these properties requires  specialized equipment such as
scanning electron microscopes,  electron probes, ESCA, and ion micro-
probes .
d.  Time Resolution
    Size-number distributions (and the  calculated size-volume
distributions) can be determined with  a time resolution  of two minutes.
Size-mass distributions require 24 hours.   Size-composition distributions,
for certain elements, can be obtained with a resolution  of a few hours.
Short time resolution is needed to study  particulate dynamics-formation
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growth, removal.  However, mass and composition measurements are
required to determine sources and health effects.  There is at present
no way to correlate the three types of measurements.
e.  Data Base
     Obviously, more and better data are needed, for compounds as well
as for elements, in more locations under a greater variety of conditions.
Measurements of number density, mass, chemical composition, and concentration
need to be performed on the same air mass.
f.  Differentiating Primary and Secondary Sources &_ Natural, Mobile
    and Stationary Sources
     It is critical to find techniques for differentiating primary and
secondary particulates, and for determining the percent contribution
when several sources contribute to one type of particulate.
Sulfate and nitrate are largely secondary; but the SCL and NO  may
                                                     c.       X
come from power plants, home heating units, auto exhaust, or natural
processes in non-urban areas.  Organic particulate has several primary
and secondary sources.  The contribution of stationary sources to
primary fine particulate matter in the ambient atmosphere need to be
determined in a larger variety of urban areas.  Stationary  sources and
mobile make a major contribution to secondary fine particulate matter
through atmospheric conversion of S0~ to sulfates, N0x to nitrates,
and organic vapors to particulate organic material.  This secondary particulate
will all be in the fine particulate size range.  We must differentiate
between sulfate and nitrate from auto exhaust, stationary sources, and
natural sources.  We must differentiate between primary and secondary
organic material from auto exhaust and stationary sources,  and secondary
organic material from terpenes, solvents, and other organic vapors,

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The relative contributions of the various sources to the various  classes
of particulate matter must be determined from atmospheric measurements
as well  as  from emission factors,  and attempt should be made to correlate
the two.
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                          V.  EFFECTS                   "  ""
A.  HEALTH
1.  Experimental Studies (Man and Animal)
a.  Introduction
     At this point in time, the theoretical definition of suspended fine
particles as they relate to health must necessarily be broad and somewhat
arbitrary.  The deposition of particles anywhere in the respiratory
tract, from the nose to the alveoli, may engender significant harmful
effects on health.  There is some reason to believe,,however, that
particles deposited below the trachea may be more dangerous than
those deposited in the nasal cavity.  Whether particles must reach
the alveoli to exert harmful effects is a more controversial issue.
It is plausible that particles deposited in the bronchi or bronchioles
are more  important in producing bronchitis than those deposited in
the alveoli.  At  present, there seems to be little utility in confining
the category of suspended fine particles only to those particles which
reach the alveoli.
     The  Task Group on Lung Dynamics has calculated that up to 10 percent
of inhaled particles of diameter  2-5 ym are deposited in the tracheobronchial
compartment, and  that up to 30 percent are deposited  in the alveolar
compartment,  The vast majority of  particles of diameter above 5 ym
are deposited in  the nasal cavity.  Thus,  a size range of fine particulate  up
tป 2-5 ym diameter, measured aerodynamically, is of principal interest
from the  standpoint of health effects.
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                                        no f/-^
                                        "'" fi^-'i OL/OTT on p,TP
                                                  ^   - • -- un CITE
     The toxicological  properties  of  inhaled  particles  are  related  to
a complex of factors  which  include the  specific  physical-chemical
properties of the particles themselves  and  host  conditions  which  affect
his response to exposure to these  particles.   With  regard to  the
toxicity of certain specific particulates which  may exist in  the
atmosphere,--moderate  amounts of  information are  known.   But such
information is not usually  available  in a form suitable for accurate
assessment of the minimum time-concentration  for exposure which will
lead to adverse health  effects.
     Even less'information  is known about how physical  environmental
variables (weather conditions) may interact with suspended  particulate
matter and alter its  chemical composition,  and thus affect  its  toxicity.
Weather conditions, per se, may  affect  man  in such  a way as to  alter
his exposure to inhaled particulates.   The  information  which  is
available, however, provides a basis  for estimating the relative
toxicity of certain substances and provides insights into  problem
areas where our information is inadequate.  '
b.  Pose-Response Relati onships
     The principal means through which  air  particulates exerts  an
effect on health is presumed to  be through  inhalation and  consequent
effects on the respiratory  system. This presumption is acceptable in the
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case of a determination of short-term effects of irritant  aerosols.
Such an assumption may be less tenable in the consideration of long-term
exposure effects where such responses as carcinogenesis, mutagenesis,
and subtle metabolic effects resulting from whole body burdens may
occur.  In these cases other routes of entry, as well  as inhalation,
may be important in establishing dose response relationships.   However,
inhalation may be a significant route of entry for non-respiratory
toxicants as an initial organ where substances are deposited  but
translocated to the gastro-intestinal system by muco-ciliary  transport
and swallowing, where they may exert a primary toxic effect or
be absorbed and translocated to other tissues where an adverse health
effect might be elicited.
c.  Physical  Factors
     Two physical factors common to all suspended particulate matter:
(1) particle size, and (2) particle density are of utmost  importance  in
ascertaining where inhaled particles may be expected to be deposited
in the respiratory tract.  Most of the calculated and experimental  data
on respiratory deposition of particles utilizes the term aerodynamic
diameter.
     Mass median diameter is a frequently used term utilized  in
studies of the respiratory deposition and retention of metallic ("hard")
particles.  This term takes into consideration particle density and,
indirectly, diameter, but it must be remembered that particle size
expressed by this term relates to mass,  In order to relate  the number
of particles to the mass size distribution, it is necessary to a
numbernumber size distribution.   Particle number can be
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                                                     ouniE <>'r:;
very important in  air  pollution toxicology, since the large surface
area provided by small  particles may provide both a reactive surface
for gas-particle interaction  and may result in greater particle deposi-
tion in the deeper regions  of the  respiratory system  and  a more
rapid dissolution.
     A moderate amount of information  is  available  concerning  respiratory
oarticle deposition in man and lower  animals.  These  data are  based
upon mathmatical calculations, and to a limited extent, experimental
data obtained from man.   The  calculated data agree, in general, with
experimental observations in  man.  A figure depicting the respiratory
deposition of particles  as  a  function of  particle diameter is shown
in Figure V-l .These  data indicates that most particles larger than
five  ym      are deposited  tn the  nasal cavity or nasopharynx.  As the
particle size becomes  smaller, an  increasing number of particles are
deposited in the lung.   This  point is thought to explain  the experimental
results of Amdur who has reported  that sulfate aerosols of 1 ym
diameter are greater respiratory irritants for guinea pigs than  2-3
i urn    sized aerosols.
     Only a few comparisons have been made concerning regional
respiratory particle deposition  in laboratory animals which  can  be
compared to man (Figure V-2).      Although some differences  in
particle deposition in rodents have been  observed,  especially  in
the efficiency of  nasal  deposition, the patterns are  sufficiently
similar to justify the use  of laboratory  animal experimentation  in
inhalation toxicology.
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                                                VtT p.'! i '"--f','
     A major question exists, however, in  whether respiratory
deposition data from normal individualsare applicable in predicting
how exposure to suspended particulate matter may affect particle
deposition rates and regional deposition.  To the extent that suspended
particulate may act as a respiratory irritant, consequent effects on
mechanics of breathing may affect both the rate and site of particle
deposition.        Under these circumstances, the total inhaled dose
may be increased.  However, this hypothesis lacks experimental verification
Also, many of the diseases and symptoms associated with elevated
levels of particulate matter are airway related.  In these diseases,
the contribution of inhaled particulate matter to their pathogenesis
may not require penetration into the alveolar region to induce a toxic
effect.  This point cannot be fully evaluated, however, since the
pathogenesis of chronic obstructive lung  disease  is not adequately
understood.
d.  Host-related  Factors

     The state of health,  especially of  the cardiorespiratory system,
and the amount of activity of an  individual,  affect the total amount
and site of deposition of  particulates that an  individual may inhale
at any given time.  The  pattern of  breathing  affects the depth of
particle deposition,  ie. deep breathing  increases alveolar  deposition
of particles.  During exercise men  commonly shift from nose ton'mouth
breathing and probably thereby  increasing particle  penetration  into
lungs.
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Figure  V-l   Effect of Particle Size  on  Regional

                Respiratory Particle Deposition  in  Man.
    EACH OF THE SHADED AREAS (ENVELOPES) INDICATES THE VARIABILITY
    OF DEPOSITION FOR A GIVEN MASS MEDIAN (AERODYNAMIC) DIAMETER IN
    EACH COMPARTMENT WHEN THE DISTRIBUTION PARAMETERrfgVARIES
    FROM 1.2 TO 4.5 AND THE TIDAL VOLUME IS 1450 ml.
                0.05  0.1       0.5  1.0        5   10
                       MASS MEDIAN DIAMETER, microns
50  100
                              -76-

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        FIGURE  V-2
                                                       •DRAFT
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              U I
       - - Mon
      D- Monkey
      o- Guinea Pig
Irarl'aml in ill!'
Palm ct o/.'1
SIZE  OF UNIT DENSITY SPHERES, MICRONS
  vursu.- particle plr
 f llic f{ninc;i pij; and monkey compared villi num. (.Adiiplud
                             -77-

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     At the same time exercise increases  respiratory volume  which
consequently increases the inhaled  dose of any toxicant.   This  effect
of exercise has been demonstrated  in  men  exposed  experimentally to
ozone,   and would presumably occur with  inhalation of particulates
as well.
     Pre-existing>'disease of the airways  or alveoli are thought to
predispose affected individuals to  more severe response when subsequently
exposed to atmospheres which contain  high suspended particulate matter.
Exacerbation of symptoms of disease which occur in such individuals
usually occur in conjunction with  weather conditions, ie.  cold  and high
relative humidity, which in themselves may have adverse health
effects.         Just how this interaction between physical,.weather
factors,  particulate matter, and gaseous  pollutants interact to affect
health is inadequately understood.
e.  "Retention "Factors
     The deposition rate and retention time of inhaled particles are
separate phenomena but have overlapping biologic  effects.   Particle
retention time is dependent upon (1)  the  site of initial  deposition
in the respiratory tract, and (2)  the chemical composition and  properties
of the particles.
     If the particles are deposited in the ciliated epithelium  of the
airways,  particle clearance is reasonably rapid.     In this  event the
toxicity is dependent upon the solubility of the particle in mucus while
in transit up the muco-ciliary escalator.  If the particle is
highly soluble, toxic inflammation in the airway epithelium may occur.
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     Particles deposited in the alveoli of the lung may be only
very slowly cleared from this location. -        The extent to which
it is cleared reflects it solubility and subsequent translocation
via lymphatic drainage or macrophage phagocytosis and clearance
via the muco-ciliary transport mechanisms.
     The preponderance of evidence clearly indicates, however, that
non-soluble particles remain in the deep lung for"long periods of
time (weeks, months and even years).  As a result of this slow clearance,
the carcinogenic hazard of long-lived radioactive metals, ie., plutonium
and uranium, and airborne chemicals, especially hydrocarbons, is of
special concern.
     Because certain metals may be soluble in respiratory secretions,
the toxic properties of these substances may be manifested in the  lung
parenchyma or airway epithelium, or may be translocated and induce
lesions in other sensitive tissues.  Vanadium is one example of such a
metal whose effects may be exhibited through this mechanism.    However,
the minimum time-concentration of vanadium exposure, and other metals,
which produces toxicity is not adequately understood.  Also the toxi-
cological assessment  .of metals which accumulate in the lung or other
tissues present a different problemUhan many other respiratory irritants,
since the relationship of tissue burdens to carcinogenesis, metabolic
defects and mutagenesis or tetrogeaesis is more difficult and time
consuming to assess.
f.  Biological Resplrabfte Particles
     There are species of pollens, fungi, bacteria and viruses within
the respirable range in particle size.  These biological particles
are included among the particles which are collected for measurement
                             -79-

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                                                 DfMF
                                            f\?OT P?r :
as respirable particles.   However,  it  is difficult to characterize the
concentration of these  particles  because of  the complexities  involved
in precise species identification and,   in  the case of viruses  and
bacteria, the concentrations  may  be very low thus causing  problems in
measurement.   Respirable biological particles have received  low  priority
within EPA due to lack  of an  appropriate technology for their control
which may be applied to the general population.
2.  Epidemiology
     Though numerous epidemiologic  studies have assessed the  effects
of total  suspended particles  on  human  health, very few have  differentiated
one particle size from  another.   In fact,  in the epidemiologic portion
of the Air Quality Criteria for  Particulate  Matter, no attempt is made
to relate specific particle sizes to specific health effects.  The
few studies which have  considered particle sizes have yielded plausible
working hypotheses.  However, their findings cannot yet be interpreted
as established fact.  The same caveat  holds  true for studies  which
have specifically considered  particle  chemistry.
a.  Asthma  Study—
     Kenline correlated daily variations  in  participate levels to
daily variations in clinic visits for  asthma in  New Orleans  in October
1963.     In general, the correlation  coefficient  between  the number
of daily asthma visits  and the concentration of  particulate  increased
as the maximum particle size  measured  decreased.   For  particles  whose
largest diameter was 22y,ffl,f was  0.61;  for  particles whose  largest
                         -80-

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diameter was 8ym,r was 0.81.  The author noted that on days of
particularly frequent asthma visits, particles in the following size
ranges increased in number:  0.5-1 .OynM-8ym;and 3-16ym. Particles
in the range of 1-4  did not increase in number.
     Though the internal consistency of the New Orleans asthma study
is impressive, its-results must be replicated before they can be
accepted with complete confidence.
b.  Chess Studies--
     In 1970 and 1971, the CHESS program of EPA gathered a considerable
amount of epidemiologic data to implicate suspended particulate
sulfate   as a pollutant of major importance in producing average
effects on healtn.     In general, the effects of sulfates were
most clearly demonstrated in health parameters which reflected acute
exposures rather than chronic ones.  In Utah, for instance, the
incidence of asthma attacks was found to increase on days of elevated
sulfate exposure.  When 'Other pollutants' concentrations increased,
the frequency of asthma attacks did not increase consistently.
Similar findings were made  in the New York City area.   In both areas,
threshold levels of sulfates necessary to influence attack rates
were elevated at low temperatures.
     In New York, panels of patients with pulmonary, cardiac, or combined
carciopulmonary disease suffered exascerbation  of symptoms when daily
sulfate levels were elevated.  The effect was most marked  in cardio-
pulmonary patients, for whom it was estimated that a sulfate level  of
8-10 yg/m  might produce increased symptom rates.
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     These     studies also uncovered  some  evidence  that  chronic  sulfate
exposures might impair health or physiologic  function.   In  Cincinnati
neighborhoods, where annual average S02  levels  wece  under the  moderate
level of 57 yg/m3,  and sulfate levels  averaged  9.5 yg/m3, white  second
graders were shown  to have slightly but  significantly decreased  three-
quarter second forced expiratory volumes.
     Retrospective  studies of acute lower respiratory disease  in
Utah and Idaho-Montana children suggested that  sulfates were more
important than SCL  in producing elevated illness  rates.   It was
the investigators'  best judgment that  exposure  to an annual  average
          o
of 15 yg/m  of S02  could produce excess  lower respiratory disease.
     At present, the evidence from CHESS indicts  acute exposures  to
sulfates more strongly than chronic exposures.   Before any  evidence
can confidently be  accepted as fact, the data from  replicate studies
must be analyzed and compared to the 1970-1971  data.  In   these
studies ,  the  sulfate  effect  could  not be completely
separated from the  effects of S02 and  other suspended particulates
in the air, particularly suspended nitrates.   Furthermore,  no  attempt
was made to measure particle sizes in  detail.  Thus, the  importance
of specific particle chemistry and particle physics  could not  be
assessed.
     At present,data  are being analyzed from
Southeastern cities of Charlotte and Birmingham.   These areas  were
selected to contain a minimum of pollutants other than particulates.
Thus the observed effects of particulates,  sulfates among them,
should not be greatly confounded by the effects of other
pollutants.
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3.  Relative Toxicity
     The class of fine participates which has  been  most studied  is
sulfates.  Nearly all work has been done  with  animals,  and cannot be
directly extrapolated toniman.   Amdur has  examined the effects of
zinc sulfate, ammounium sulfate,  zinc ammonium sulfate,  and  sulfuric
acid aerosols on airway flowrresistance in  guinda pigs.   She found
that sulfuric acid aerosol  produced a greater  increase  in airway
resistance than zinc ammonium  sulfate  particulate  of  similar particle
size and at similar concentration.    However,  zinc  ammonium  sulfate
was more potent per molar concentration of  sulfur contained.
     At a particle mass median diameter of  0.29ym zinc  ammonium  sulfate
was found to be about twice as potent as  zinc  sulfate,  and about four
times as potent as ammonium sulfate.  For all  these^compounds, toxicity
increased as mass median diameter decreased.
     A great deal of work in ranking the  toxicity of particulate remains
to be done.  For example, there is  essentially no knowledge  of the
toxicity of suspended nitrates and  nitric acid aerosol ,  relative to
other particulates or relative to each other.
     Amdur has shown quite conclusively that  particulate sulfates are
more irritating than sulfur dioxide gas at  similar  concentrations.  She
has also shown that the interaction of^sulfur  dioxide with the  particulates
                                    +2    +2        +5
of certain metal cations, such as Fe  , Mn   ,  and V  ,  potentiates  its
effects on guinea pig airway resistance.   The  latter finding is crucial,
for sulfur dioxide is certainly never found alone in urban atmospheres.
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     Amdur's work has also  demonstrated  the wide  variation  in  toxicTty
of different species of participates.  This variability  makes  it  quite
fruitless to compare the toxicity of fine  particulates as a class
to other species or classes of pollutants.
4.  Problems Areas

a.  Aerometry--
     (1)  At present, it is prohibitively  expensive  and  difficult to
measure all substances trapped by a particulate filter from the ambient
air.  Thus, in certain individual areas, particulate substances which
may be unique to those areas,  and important  in causing  health effects,
may not be identified.
     (2)   In many instances, the compounds on a particulate filter may
not be the same compounds as are present in the ambient  air.  For exapple,
sulfites in the air may be transformed to sulfates after the filter
has trapped them.
     (3)   The sizes of certain particles on the filter may  be different
from their sizes in the ambient air.  It is quite conceivable that certain
large particles are broken into smaller ones on impact with the filter.
It  is also conceivable that certain small  particles coalesce on the
filter to  form larger ones.  Thus, the sizes of particles  in the air
may be inaccurately measured.
b.  Health—                	
1.  The only rational approach to the fine particulate problem will be
to  treat particle physics and particle chemistry with equal importance.
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To the present time,  too many investigators have considered only one
disciplines or the other.
2.  There has been very little investigation of effects of particulate
substances in locations other than their sites of deposition.  Such
effects could be  indirect, mediated through neurologic or immune
mechanisms.   The  effects could also be direct, caused by the substance
after it has  been  relocated in the body.
3.  As yet, there  are few epidemiologic indicators that specifically
reflect exposure to a single substance.
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B.  EFFECTS ON VISIBILITY,  WEATHER,  AND  CLIMATED
1.  Visibility
     Because of their much  greater surface area  per unit mass, and because
their diameter is the same  order  of  magnitude as the wavelengths of
visible light, fine particles  account  for most of the light scattering.
They also have higher light absorption coefficients than larger particles
(higher imaginary index of  refraction).  The two mechanisms, light
scattering and light absorption by fine  particles, are responsible for
visibility reduction.  The  absorption  of water vapor by hygroscopic
and deliquescent fine particles can  lead to large decreases in visibility
as relative humidity increases,
2.  Weather and Climate
     There are two  ways  in which suspended fine particulate matter
could affect weather  and  climate on either a local or large scale.
First, the energy budget  at  the earth's surface can be modified
by changes in the distribution and amount of incident solar energy.
Second, particulates  are  often effective condensation and ice nuclei
and, as such, can affect the physical processes of condensation and
           1
precipitation.     <      " •>  - _
     Atmospheric particulates attenuate^&lar  radiation by  re-directing,
or scattering, and  by adsobring the energy incident  upon them.  A
fraction of this scattered energy  is  directed  backward  (in  essence
reflected) away from the earth.  By this process  alone, the albedo
(reflectivity) of the earth  is increased with  a resulting decrease
in the amount of energy incident at the earth's surface.  When
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  particles absorb solar  radiation, the energy is not lost to the
  earth-atmosphere system,  but  is simply transferred from the surface to
  the  atmosphere.
       Many studies  of  urban climates have shown that the added particles
  in the  atmosphere  can significantly reduce the solar radiation incident
  at ground level.   The reduction increases with particle concentration
  and  with  the  solar path length through the atmosphere.  Moreover,
  the  effect of the  particles is most evident at the short, or ultraviolet,
  wavelengths.
    If particle concentrations over large areas of  the
earth  significantly increase,  large  scale  weather  and climate  patterns
may occur.   If the particles  act  solely as  scatterers of  radiation
their  net effect will be  to cool  the earth.   However, if  they  also
absorb energy, which many do,  their  net effect,  i.e., whether  a  net
cooling or warming will occur,  depends critically  on the  particles
absorption  to backscatter ratio as well as  the albedo of  the underlying
earth's surface.   Current research is directed toward incorporating
atmospheric particles into  both local-scale  and  global-scale numerical
models of the atmosphere.   In  this manner  the specific  effects that
will  likely result from given  particle concentrations can be determined.
    Another meteorological  parameter that  can be altered  by fine
particulates is precipitation.  When many  particles which are active
cloud  condensation nuclei  are  present in a  supersaturated atmosphere
they compete for the available  liquid water.  Many small water droplets
form and  a  stable cloud results.  Thus, this effect of  fine particles
is to   inhibit rainfall.   Conversely, particles which are active freezing
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nuclei encourage the freezing  of  supercooled water drops.  The associated
release of latent heat aids  the cloud  instability and thus the particle
effect is to enhance rainfall.  Therefore, because of these competing
processes and variable effectiveness of particles with different com-
positions one cannot generally relate  increased pollution levels to
a specific change in precipitation.
    Recent studies of the precipitation climatology of several mid-
western and eastern U. S. cities  have  shown that immediately downwind
of these cities precipitation  is  augmented by  about 5 to 10%.  In addition
to the added nuclei in the urban  atmosphere the recorded increases could
 result from heat emissions  or increased turbulence generated over
 the city.   Research in the  St. Louis area is now focusing on eluci-
 dation of the specific mechanism or mechanisms responsible for
 peculiarities in urban precipitation patterns.
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C.   ECOLOGY
     Relatively little is known about the ecological effects of fine
participates in the atmosphere.  The problems here involve complex
relationships, either direct or indirect, between atmospheric loading
and removal mechanisms.  Deposition of fine participates on soil
or water surfaces may alter the characteristics of the medium, and
hence have some effect upon the flora and fauna of the area.
For example,  acid rainfall  may alter the pH of soil  or water.
In addition the deposition  of fine particulates on plant surfaces
could influence not only the plants themselves but the microflora of the
plant surfaces.  Lead, chlorine and bromine containing particles have
been detected on the bark of trees.  These effects are not necessarily
detrimental.   Toxic elements or compounds found in fine particulates
may be taken  up by plants through the root systems and concentrated
within the food chain.  On  the other hand, the biological  processes
within the soil or water may alter the chemical nature of the
particulate material  in such a manner as to inhibit the buildup of
potentiallynharmful pollutants.  This appears to be the case with
carbon monoxide and a wide  variety of hydrocarbons.
     Much additional  work needs to be done in this area.  Specific
problems which should be addressed include:
     (1)  The identification and characterization of fine particulates
from man-made sources which may have an adverse ecological effect,
     (2)  The ecological effects of fine particulates from natural sources,
     (3)  The nature and behavior of ecological removal mechanisms for
fine particulates.

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                    VI.   CONTROL STRATEGIES
     Control  strategy options  must  be  considered  in  the  formualation
and conduct of research and  development  efforts related  to  fine
particulates  in the atmosphere.   As needed Information is obtained
regarding the health and welfare  effects resulting from  the atmosphere
loading of fine particulates,  control  options  under  the  provisions
of the Clean  Air Act must be reviewed.   These  considerations then
become important imputs to ensure a viable  program in. stationary
and mobile emissions and control.   Our data  base  is  not  adequate at
this time to  make final decisions regarding  control  strategies.
The use of a  pollutant category of  fine  particulates, as opposed
to individual pollutant species,  may not prove to be a practical  .
approach.
     The issue can be resolved  by obtaining  answers  to
the fundamental  scientific and  technical  questions regarding  fine
particulates in the atmosphere  and their  effect  upon human  health
and welfare.
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