EPA-650/2-74-128


NOVEMBER  1974       Environmental Protection Technology Series
                                        >F
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                                      55
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                            EPA-650/2-74-128
MEASUREMENT  OF THE OPACITY
  AND  MASS  CONCENTRATION
  OF  PARTICULATE EMISSIONS
     BY TRANSMISSOMETRY
                 by

             William D. Conner
        Chemistry and Physics Laboratory
             ROAP No. 26AAM
          Program Element No. 1AA010
     NATIONAL ENVIRONMENTAL RESEARCH CENTER
      OFFICE OF RESEARCH AND DEVELOPMENT
      U.S. ENVIRONMENTAL PROTECTION AGENCY
       RESEARCH TRIANGLE PARK, N. C. 27711

              November 1974

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                        EPA REVIEW NOTICE

This report lias been reviewed by (he National Knviromnenlul Research
Center -  Research Triangle Park, Office of Uesearch anil Development,
liPA , and approved  for publication.  Approval does not signify  that the
contents  necessarily reflect the views and policies of the Environmental
Protection Agency ,  nor does mention of trade  names or commercial
products constitute  endorsement or recommendation for use.
                    RESEARCH REPORTING SERIES

Research reports of the Office of Research and Development, U.S. Environ-
mental Protection Agency, have been grouped into series.  These broad
categories were established to facilitate further development and applica-
tion of environmental technology.  Elimination  of traditional grouping was
consciously planned to foster technology transfer and maximum interface
in related fields.  These series are:

           L.  ENVIRONMENTAL HEALTH EFFECTS RESEARCH

          2.  ENVIRONMENTAL PROTECTION TECHNOLOGY

          3.  ECOLOGICAL RESEARCH

          4.  ENVIRONMENTAL MONITORING

          5.  SOCIOECONOMIC ENVIRONMENTAL STUDIES

          6.  SCIENTIFIC AND TECHNICAL ASSESSMENT REPORTS

          9.  MISCELLANEOUS

This report has been assigned to the ENVIRONMENTAL PROTECTION
TECHNOLOGY series.  This series describes research performed to
develop and demonstrate instrumentation, equipment and methodology
to repair or prevent environmental degradation from point and non-
point sources of pollution.  This work provides the new or improved
technology required for the control and treatment of pollution sources
to meet environmental  quality standards.
 This document is available to the public for sale through the National
 Technical Information Service, Springfield,  Virginia 22161.

                 Publication No. EPA-650/2-74-128
                                  u

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                               CONTiNTS
                                                                       Page
LIST OF FIClMliS	  iv
INTRODUCTION 	   1
OPACITY AND VISUAL EFFECTS OF SMOKE PLUMES	   3
    Visibility Obscuration by Plumes 	   3
    Visibility of Smoke Plumes 	   7
    Observer Evaluation of Opacity		   8
MEASUREMENT OF SMOKE OPACITY BY TRANSMISSOMETRY	10
    Light Transmittance of Aerosols	10
    Wavelength Consideration 	  11
    Collimation Considerations 	  14
MEASUREMENT OF MASS CONCENTRATION BY TRANSMISSOMETRY 	  17
REMOTE MEASUREMENT OF PLUME OPACITY  	  24
    Sun Photometry	24
    Contrasting Target Telephotometry  	  25
    Lidar	25
SUMMARY AND CONCLUSIONS   	  27
REFERENCES	31
TECHNICAL REPORT DATA AND ABSTRACT 	  33
                                  111

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                             LIST OF FIGURES


Figure                                                                     Page


   1.   Observer Estimates of the Opacity of Black and White Experimental
       Plumes with Equivalent Vision Obscuration	7

   2.   Particle Extinction Coefficients for Various Aerosols Calculated
       from the Mie Theory	12

   3.   Opacity of an Experimental White (Oil) Plume to Light of Various
       Colors	13

   4.   Opacity of an Experimental Black (Carbon) Plume to Light of Various
       Colors	13

   5.   Schematic of Transmissometer with Collimating Optics	]4

   6.   Opacity of an Aerosol as Measured with Transmissomctcrs with
       Different Light Detection Angles as a Function of the True Opacity
       of the Aerosol	15

   7.   Opacity of Aerosols Containing Particles of Different Sizes as
       Measured with a 20 Degree Light Detection Angle as a Function of
       the True Opacity of the Aerosol	15

   8.   Opacity of Smoke Plumes Containing Particles of Different Sizes
       and Refractive Indexes as a Function of Their Mass Concentration  _  .19

   9.   Opacity-Mass Concentration Relationship of Laboratory Generated
       Coal - Fired Power Plant Emissions with Different Particle Sizes  .  .20

  10.   Opacity-Mass Concentration Relationship for Particulate Emissions
       from a Kraft Recovery Furnace   	22

  11.   Opacity-Mass Concentration Relationship for Particulate Emissions
       from a Cement Plant Kiln	23

  12.   Opacity-Mass Concentration Relationship for Particulate Emissions
       from a Bituminous-Coal-Fired Boiler	23
                                    IV

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                         MEASUREMENT



        OF  THE OPACITY  AND  MASS CONCENTRATION



    OF PARTICULATE EMISSIONS BY TRANSMISSOMETRY





                           INTRODUCTION



     Evaluation of smoke emissions on the  basis of appearance began near


the end of the nineteenth century when a number of different methods and


scales  for visual estimation of smoke were proposed.   It was during this


period  that Maximilian Ringelmann developed a series  of charts of gradu-


ated shades of gray for use as visual comparators for the evaluation of


gray or black smoke.    Ringelmann Charts are still considered the refer-


ence standard of smoke regulations for visible emissions in most industrial


nations.


     Although the Ringelmann Chart generally remains  the reference standard


for regulation of visible emissions, its method of application has changed,


and other measurement methods have been applied. "   One of the most common


methods is transmissometry, which has become an accepted instrumental


method  for measuring the opacity of visible emissions. An equivalency has


been accepted between the opacity readings and Ringelmann number values of


"black" plumes.  By the use of opacity measurements,  visible emissions

                                                                2
regulations have been extended to plumes that are not gray or black,  have


limited the effect of the environment on the method,  and have made the

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regulation better represent the concentration of the particulate emissions.




Today, smoke inspectors are commonly trained to read visible emissions at a




plume evaluation school; they qualify when they learn to read black and




white training plumes with acceptable accuracies relative to transmissometer




measurements of the opacity of the emissions.




     Opacity and/or mass standards are, or will be, placed on the




particulate emissions from new and existing sources.  Emission controls




at these sources are required for implementation, maintenance, and




enforcement of emission standards and ambient air quality standards




promulgated by the Environmental Protection Agency as required by the




Clean Air Act of 1970.  Standards of performance for new stationary




sources also require the monitoring of smoke emissions from a number




of sources, and the requirement is expected to be extended to additional




new and existing sources.




     This paper discusses the relationship between the opacity, light




transmittance, visual effects, and mass concentration of particulate




emissions.  It also discusses some optical-design factors of transmis-




someters that can affect their measurement of the opacity of visible




emissions.

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              OPACITY AND VISUAL  EFFECTS OF SMOKE PLUMES

     Two different visual effects may be attributed  to plumes  containing
particles that scatter and/or absorb light:   (1)   the plumes become
visible, and (2) they obscure the visibility of  objects  behind them.
These visual effects have been analyzed in this  laboratory  in  terms  of
the luminance contrast between objects (or plumes) and their surroundings.
The work indicated that both effects are dependent not only on opacity  but
on the amount of light scattered by plumes into  the  viewer's eyes and,
consequently, are dependent upon the environmental lighting conditions  of
the plumes.  In the case of obscuration of visibility  by plumes,  however,
the ambient lighting conditions have been shown  to be  less  important.
     It is the obscuration of visibility by plumes that  represents the
basis for regulating plumes by a visual effect.   The term opacity has been
defined as "the degree to which emissions reduce the transmission of light
and obscure the view of an object in the background."    A theoretical
hypothesis of vision obscuration by a plume in terms of  the reduction  in
luminance contrast of an object viewed through the plume can be presented
to  illustrate the opacity concept.

VISIBILITY  OBSCURATION BY PLUMES
     The  luminance contrast  (C ) between  an object of luminance (B ) viewed
against an extended background such as the sky with luminance  (B ) is:
                                     :-Bs
                                     Bs

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     If the object is viewed through a plume, its apparent luminance (B  )
and the apparent luminance of the sky behind the plume (B  ) will depend
on the amount of light that the plume scatters from the surroundings and
sun into the viewer's eyes (B ), and on the amount of light transmitted
                             3.
through the plume from the background and object.  The apparent contrast
of the object (C  ) may be written as:
     R
.  .
                             c' .
     The denominator of equation (2) remains, as in equation (1), the
intrinsic luminance of the sky (B ) since it remains the dominant lumi-
nance of the scene.  Dividing by the intrinsic luminance of the sky
simplifies the analysis by removing the light scattering term (B ) from
                                                                3.
the final results.  This differs from a more complicated earlier analysis
from this laboratory in which the reduction in contrast between two con-
trasting targets located behind the plume was discussed.   Dividing by
the intrinsic luminance of the sky would not be realistic for atmospheric
pollution or for extended sources where the scatter and absorption of light
by the particulates would affect the luminance of the entire scene.  For
these cases, the denominator of equation (2) should be the apparent lumi-
nance of the sky  (B  ) .
     If the plume has a transmittance (T) and the amount of light scattered
by the plume toward the observer is B , then B_  = B T + B  and B   = B T + B
 /r                             a'ttasss
and equation (2) may be written:

                            ct> -     1^

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     The reduction in object to background contrast due to the plume may




be defined as:




                                  C  - C 1
                                   t    t

                             CR ' \-^                     <4>




which, after substitution of equations (1) and (3) and rearrangement,



becomes:




                                CR = 1 - T                     (5)



     Equation (5) indicates that the reduction in luminance contrast and




visibility of an object behind a plume viewed against an extended back-



ground is equivalent to one minus the transmittance (1-T) of the plume.



1-T is commonly called the opacity of the plume.  The relationship also




indicates that the visibility reduction is independent of the environmental




illumination, and that there is an equivalency between the opacity of



plumes and their reduction of visibility.



     The equivalent opacity concept was studied by the Bay Area Air Pollu-



tion Control District in the mid-1960's.   In that study, a group of



observers was used to determine the light transmittances  (opacities) of



black  (carbon) and white (oil) experimental plumes with equivalent vision



obscurations.  Because the observers had no previous experience in reading



smoke, they were screened to establish a statistically consistent group.



After  instruction in the use of the Ringelmann Charts for evaluating black




plumes, the observers were asked to assign Ringelmann number values to



black  plumes of various densities and to observe how much the black plumes



obscured the visibility of a target located behind them.  They were then



asked  to view a similar target behind whi£e plumes of various densities and



assign "equivalent Ringelmann numbers" to the plumes by equating their



                                                                           5

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visibility reduction to the black plumes.  During the tests, the opacity




of both plumes was monitored by identical photoelectric transmissometers.




The Bay Area APCD used the results of the tests to calibrate the trans-




missometers on the black and white smoke generators in terms of Ringelmann




numbers and "equivalent Ringelmann numbers," respectively.  These curves




represented the average of 14,400 observer estimates of the Ringelmann




number values of the black plumes (9 observers, 80 series of 20 readings),




and 8,120 observer estimates of the "equivalent Ringelmann number" values




of white plumes (7 observers, 58 series of 20 readings).




     Since the two Ringelmann number scales reported by the Bay Area APCD




are related through the equivalency in the vision obscuration produced by




the plumes, the two curves may be combined to show a general equivalency




in the transmissometer-measured opacity and the reduction in visibility




by the two plumes  (Figure 1).  The averaged data shown in Figure 1 indicate




that, in the  important opacity region below 35 percent, black plumes have




slightly greater vision obscuration than white plumes with equivalent




opacities.  In the opacity region above 35 percent, white plumes were




judged to have greater vision obscuration than black plumes with equivalent




opacities.  Since  standard deviations of up to 12 percent opacity are




reported for  the data, the averaged curve shown in Figure 1 is within one




standard deviation of the theoretical one-to-one relationship.




     Although the  opacity of plumes represents a measure of how much they




obscure visibility, the plumes are generally located where they are observ-




able only against  the sky, and their obscuration of visibility  (obscuration




of objects behind  them) is not observable.  Consequently, it is the visual

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  100


   90


   80




!"
of  60
       u  50
       >  40
       t-

       u


       £  30
          20




          10
                 I                                       I
                                I     I    I    I    I    I
                10   20   30   40   SO    60   70


                            OPACITY BLACK PLUME, percent
                                                 90   100
           Figure 1.  Observer estimates of the opacity of black and white
           experimental plumes with equivalent vision obscuration.



appearance of plumes that  is  usually observed by both  the  casual  observer



and by the trained observer  assessing their opacity.
VISIBILITY OF SMOKE PLUMES
                                          6 .
     Analysis of  the  visibility of plumes  in terms of their  luminance
contrast with their  background (C ) has shown that:
                             S = r- -
                                                                  (6)
where:  B  = the  amount of light scattered by the plume toward the

             observer


        B  = the  luminance of the background (usually the  sky)


        T  = the  light  transmittance of the plume


      (1-T) = the  opacity of the plume

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     Equation (6) indicates that the visibility of a plume depends on the



amount of light scattered by the plume from the sun and its surroundings



into the viewers eyes (B ) relative to the luminance of the plume's back-
                        a


ground (B ) and the opacity of the plume (1 - T).



     The dependency of the appearance of plumes on their environmental



lighting, background, and general viewing conditions makes plume visibility



or simple telephotometric contrast measurements undesirable for regulating



particulate emissions.  Consequently, visible emissions regulations are



based on the opacity  (visibility obscuration) of the plumes, which is an



intrinsic property of the plume and a better indicator of the particulate



emissions.  It may be measured instrumentally by transmissometry or esti-



mated by trained observers.






OBSERVER EVALUATION OF OPACITY



     The smoke inspector or trained observer receives training at a smoke



inspector  training school where he is taught to evaluate the opacity of



black and  white  training plumes with prescribed accuracies relative to



transmissometer  measurement of their opacities.  Upon passing the course,



he becomes  certified  by the school as capable of evaluating the opacity of



smoke plumes from their appearance.  This procedure requires the inspector



to evaluate an intrinsic optical property of the plumes  (their opacity) by



observing  their  visibility, which  is dependent not only  on their opacity,



but  also on their illumination and background viewing conditions.



     Clearly, the trained-observer method of evaluating  opacity has



limitations; e.g., at night when a plume cannot be seen, the method is

                                         o

not  generally applicable.  Halow and Zeek  have analyzed the visibility



of white plumes  in daylight and have shown that observer evaluations depend

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upon the background and environmental lighting conditions of the plumes.   A




white plume viewed against a white overcast sky is often invisible because




the amount of light it scatters toward the viewer equals the amount of




light that it attenuates from the background.  The visibility of a white




plume viewed on a clear day is particularly sensitive to the viewing direc-



tion relative to the sun.  The plume appears much brighter when the sun is



illuminating it from behind.  Tests with trained observers  have shown that



the evaluation of such plumes should be limited to times when they may be




seen with the sun illuminating them from the front.  There are many plume



background and illuminating conditions confronting the smoke inspector in



the field that may impose limitations on the visual evaluation of the



plumes; consequently, it is important that the inspectors be trained



under viewing conditions that generally prevail in the field, and that



the inspectors know of any limitations that may result because of




deviations from these conditions.

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         MEASUREMENT OF  SMOKE  OPACITY BY TRANSMISSOMETRY

     The measurement of the light  trausmittnixco or opacity of aerosols
by transmissometry requires the standardization of two important optical
characteristics of the transmissometer to  obtain similar performance
between instruments.  The need for standardizing the wavelength and
collimation characteristics of the transmissometer can best be illustrated
by examining the light-scattering  characteristics of fine particles.

LIGHT TRANSMITTANCE OF AEROSOLS
     A part of a parallel beam of  incident light upon an aerosol such as
a smoke plume will always be removed  from  the beam by scattering and also
by absorption if the smoke is composed of  absorbing particles.  A measure
of the amount of light that passes through the smoke relative to the
amount of incident light is the transmittance of the smoke.  The trans-
mitted light has not interacted with  the particulates and will emerge
from the smoke still parallel to the  incident beam.
     The transmittance of light through an aerosol of monodisperse
                                               9
spherical particles is defined by  Bouguer's  law:
                T =   - e -                                      (7)
                     o
 where:          T = transmittance of the aerosol
                F = light flux incident on the aerosol
                F = light flux transmitted through  aerosol
                L = light path length through the aerosol
                n = number concentration of the particles
                a = projected area of one of the  particles
                Q = particle extinction coefficient
                                    10

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     The particle extinction coefficient (Q) is defined as the total flux



scattered and absorbed by a particle divided by the flux geometrically



incident on the particle.  It is, in general, a function of the particle



size and shape, the refractive index, and the wavelength of the incident



light.  The product naQ=o is sometimes called the turbidity coefficient



or the attenuation coefficient of the aerosol and has the dimensions (length   )




WAVELENGTH CONSIDERATION



     The effect of wavelength on the transmittance of smoke depends



primarily on the size of the particulates in the smoke and their associated



extinction coefficients.  The particle size-extinction relationship can



usually be divided into three different light-scattering regions that



describe the scatter by particles much smaller than, larger than, and



comparable to  the illuminating wavelength.



      Particles that are much smaller than the illuminating wavelength



(d<0.05 micron in white  light) are in the dipole or Rayleigh scattering



region.  Particles in this region contribute little to the opacity of



smoke emissions since their extinction coefficients seldom exceed 10


                                                                -4
The extinction coefficients in this  region  are proportional to A   if the



particles  are  transparent, and proportional to K~  if the particles are



absorbing.



      Particles that are  large compared  to the  illuminating wavelength



 (d>2  micron  in white  light) are  in the  geometrical scattering  region.



In this  region, the extinction coefficient  will have the  value of 2  for



absorbing  and  irregularly  shaped particles, but  will oscillate around the



value of 2 for spherical transparent particles  (Figure  2).  For monodis-



perse spherical  transparent particles  in  air,  the  oscillations  in the


                                                                          11

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                                     OAVES FOR TRMSMKCNT MXTICUS
                                    >,B< UONOOtSFCKC smCRtS, « -1.55. 1.5
                                    C: IRREGULAR . RANDOM OmCNTMION , in • 1.9
                                    Q4VC9 FOR »tJOB8WO UONOOHPIRSI WHERU, m • |.S»
                                    0: TOTAL eiTINCIKM C.F: JUTTCRINO »
                                           ABSORPTION COMPONENTS
                                 PARTICLE-SIZE PARAMETER Q =7Td/\
                     0.5      1.0     1.5      2.0     2.5
                         AREA-MEAN PARTICLE DIAMETER (microns)
                            FOR WAVELENGTH OF 0.52 micron
             Figure 2. Particle extinction coefficients for various aerosols
             calculated from the Mie theory (except curve C).
extinction  coefficient can  result in extinction  coefficient values  in

this region being as high as  1.5 times the value of 2, to which  it  con-

verges  at  large particle sizes.   If the particles are absorbing  or

irregular  in shape  (randomly  oriented), the  limiting extinction  coef-

ficient value of 2 can be obtained at particle  sizes as small  as 0.3

micron  with little or no oscillation.  In practice, the particulates in

smoke emissions are polydisperse and the oscillatory behavior  of the

individual  particle extinction coefficients  is  smoothed.  Further

smoothing  results when the  particles vary in composition and the measure-

ments are  made with polychromatic (white) light; consequently,  smoke

emissions  with mean particle  sizes above 2 microns will generally have a

mean particle extinction coefficient of 2 and a transmittance  that  is not

a function of wavelength.

     The  intermediate size  region (0.05 
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region value of  10    to the plateau of 2 for  absorbing and irregularly

shaped particles, and sometimes to a maximum  value of 3 or 4 if the particles

are spherical, transparent, and monodisperse.

     As indicated above, the extinction coefficient of highly absorbing  and

irregularly shaped  particles will reach the value of 2 between 0.3 and  0.7

micron.  The maximum extinction coefficient value for transparent, spherical

particles  is obtained between 0.67 and 1 micron in visible light before

oscillating around  the value of 2.- Again,  the oscillations are smoothed

toward  the value of 2 for  smoke emissions  that are polydisperse and  of

varying composition.  Smoke emissions  in  this size region generally  have

an extinction  coefficient  proportional to X~n(0
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 COLLIMATION CONSIDERATIONS

      To measure the amount of  light  transmitted by an aerosol, the trans-

 missometer must be designed  to exclude  the  light scattered by the aerosol

 from the measurement.  The poorly  collimated transmissometer detects an

 excessive amount of scattered  light  along with the transmitted light and

 gives an erroneously high transmittance (low opacity) measurement of the

 aerosol.  Collimation  of the in-stack transmissometer is obtained by

 restricting the light  projection and detection angles of the instrument

 (Figure 5).
  VIEW LIMITING APERATURE


DETECTOR
  COMPACT
FILAMENT LAMP1
                          ANGLE OF VIEW -7  / PROJECTION ANGLE
                              i- -_-j'  ^
                              COLLIMATING LENS
                                 LENS CLEANING AIR
              Figure 5. Schematic of transmissometer with collimating optics.


      The error  in  the  transmittance measurement due to the use of trans-

 missometers  with different light detection angles has been analyzed

 theoretically by Ensor and Pilat   and shown to be a function of detection

 angle  and  aerosol  particle size.  They show that, in general, the error

 associated with a  given detector viewing angle increases with increased

 particle mean diameter and, at a given particle mean diameter, decreases


 14

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with increasing particle  size geometric  standard deviation (increasing


polydispersity of the particle size).  These results were used to calculate


the apparent opacity of a 10-micron aerosol  when measured with detection


angles of 0.2°, 2°, and 20°  (Figure 6),  and  the apparent  opacity of  2-,  5-,


10-, and 20-micron-sized  aerosols when measured with a  detection angle  of


20°  (Figure 7).  Figure 6 shows that, for a given aerosol size, increased


error  in the measurement  of opacity results  with increased detector  angles

of view; Figure 7 shows that, for a given angle of view,  increased error


in the measurement of opacity results with increased aerosol size.
   50
   40
   30
ui 20
cc

V)
   10
PARTICLE REFRACTIVE INDEX = 1.5
LIGHT WAVELENGTH=0.55 n
GEOMETRIC STANDARD DEVIATION
 PARTICLE SIZE DISTRIBUTION =
PARTICLE MASS MEAN DIAMETER = 10 fi'
LIGHT SOURCE PROJECTION ANGLE = 0
      ^
)NOF  A?

  fl || W
            10      20      30     40

               TRUE OPACITY, percent
                                            50
                                            40
                                    £  30
                                    u

                                    o
                                    a
                                    ui  20
                                          tu
                                          S
                                            10
                                  50
PARTICLE REFRACTIVE INDEX = 1.5
LIGHT WAVELENGTH = 0.55 \i
GEOMETRIC STANDARD DEVIATION OF
 PARTICLE SIZE DISTRIBUTION = 3
dgw= PARTICLE MASS MEAN DIAMETER
LIGHT SOURCE PROJECTION ANGLE = 0
LIGHT DETECTION ANGLE = 20
                       10      '20     30     40

                           TRUE OPACITY, percent
   Figure 6. Opacity of an aerosol as measured   Figure 7. Opacity of aerosols containing
   with transmissometers with different light     particles of different sizes as measured with a
   detection angles as a function of the true      transmissometer with a 20 degree light detection
   opacity of the aerosol.                     angle as a function of the true opacity of the
                                          aerosol.
      An experimental  study of the effect  of the collimating angles of the

detector and light source of a transmissometer on the  measurement of  the

opacity of emissions  from a coal-fired  steam generator was conducted  by

Peterson and Tomaides.     They show that  the size of the collimating  angles
                                                                                15

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 of the detector and light source produces similar errors, and both must be



 restricted to minimize the error in the measured transmittance or opacity.



 Detailed design and performance specifications for transmissometer opacity


                                        12
 measurement systems have been reported.
16

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       MEASUREMENT OF MASS CONCENTRATION BY TRANSMISSOMETRY

     The value of the transmissometer  for  monitoring the mass concentration
of particulate emissions  from pollution  sources has not been resolved.
Several investigators have reported  the  observation of good empirical cor-
relations between the mass concentration and  light transmittance of specific
sources, whereas others have pointed out that the usefulness of such relation-
ships is too dependent on invariable particulate characteristics of the
sources.  To understand the effect of  various aerosol characteristics on the
relationship, it is useful to express  Bouguer's transmittance law in terms
of the mass concentration of the aerosol.
     For a polydisperse aerosol, Bouguer's law, shown in equation  (7), may
be written as:

                           T = exp ^ Z  n.d2Q.                (8)
                                 * -4    i ixi                *• '
and the mass concentration (C )  of the aerosol may be written as:
where:  T  = transmittance of the aerosol
        L  = light path length through the aerosol
        d. = diameter of the particles within the size  increment  i
        n. = number of particles of size d.
        Q. = particle extinction coefficient of the particles  of  size d.
        p  = density of the particles in the aerosol
     Dividing equations (8) and (9) and solving for C   gives:
                               2En.d.3
                               SEn.d.  0.
                                  i i  xi
                                     17

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By defining a mean extinction coefficient, Q = En.d.^./En.d, 2, and a mean



particle diameter, d = En.d.3/En.d. 2, for the aerosol, equation (10) may



be written:



                              r    2dp    1                    ,  .
                              Cm = —— In =                    (11)

                                   3QL


d is often referred to as the volume-to-surface mean diameter of the



aerosol (sometimes called Sauter diameter).



     Pilot and linsor   express equation  (10) as:






                              Cm = E2- ln T                     (12)


and define K as the specific particulate volume (cm3 particles/m3 air)



divided by the aerosol attenuation coefficient  (m  ).  They show theoretical



values of K as a function of particle size for several aerosols with differ-



ent characteristics.  These values of K were used in equation  (12) to



calculate the effect of particle size and composition on the relationship



between the opacity and mass concentration of aerosols (Figure 8).



     Figure 8 shows that particle  size is the primary characteristic of the



aerosol affecting the opacity-mass concentration relationship when the



particle size of the aerosol is larger than 3 or 4 microns.  However, at



particle sizes below 3 or 4 microns, the refractive index of the particu-



lates also has a pronounced effect on the relationship.  This results in



the white particles in Figure 8 showing  a maximum opacity per unit mass



concentration at about 0.6 micron  particle size, whereas the black particles



show the maximum at about 0.15 micron.



     Pilot and Ensor 3 also show that the width of the size distribution



will usually affect the opacity-mass concentration relation.   In addition,



irregular transparent particles smaller  than 2 microns generally attenuate




 18

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    10

    20


    30

+*

§   40
09
a
UJ

    5°
2   60
    70
   80
                            \
                  \
                              \
 \
LOG NORMAL DISTRIBUTION
STANDARD DEVIATION OQ = 4
PARTICLE DENSITY = 2 gram/cm?
WAVELENGTH = 0.55 /u
REFRACTIVE INDEX
WHITE = 1.5
BLACK = 1.96-0.66i
            I  N
                  0.1
0.2            0.3
MASS CONCENTRATION, e/m3
                                          0.10
                                          0.20
                                                                         0.30
                                                                         0.40
                                                                              o
                                                                              o
  0.50
           0.4
0.5
  Figure 8. Opacity of smoke plumes containing particles of different sizes and refractive
  indexes as a function of their mass concentration.
                                                                  14
  less  light than spherical  particles of the same  projected area    con-

  sequently, the observed  mass concentration indicated in Figure 8 for  small

  transparent particles will be two to three times too low for irregular

  particles, but not appreciably different for  absorbing particles.

       The effect of particle size on the opacity-mass concentration  relation-

  ship  has been studied experimentally in the laboratory by Uthe and  Lapple.

  They  collected fly ash  from a bituminous coal-fired power plant  and

  classified it into a series of size fractions.   The various size fractions

  were  then pneumatically  injected into an aerosol chamber at controlled

  concentrations where the opacity was measured with a transmissometer.

                                                                               19

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Figure 9 is the  opacity-mass concentration relationship observed  by Uthe


and Lapple for  aerosols with four different mean sizes.  Each point shown

in the figure generally represents  an  average of two to six runs.   The

mass concentrations were calculated from aerosol generation rates.
 §   40 —
 E
 ro
 u
 4
              0.1
0.2
  0.3      0.4      0.5      0.6

MASS CONCENTRATION, g/m3
0.7
0.8
     Figure 9. Opacity - mass concentration relationship of laboratory generated coal-
     fired power plant emissions with different particle sizes.
      These results were as expected and show the particle  size dependence

 indicated from theoretical considerations.  Comparison  of  Figure 9 with

 the  theoretical calculations  of Figure 8 for spherical  particles with a

 refractive index of 1.5 and a specific gravity of 2  indicates that the

 coal-fired power plant fly ash attenuated around 50  percent as much light


 20

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for similar particle sizes and mass concentrations.  Considering the dif-



ferences in aerosol characteristics, better agreement was not to be



expected.  The ash used for the aerosol generation was reported to have



size distributions of o =1.5 and contained a good number of particulates
                       o


with absorption characteristics; additionally, the specific gravity of 2



used for the theoretical calculations may be somewhat low for fly ash.



     It is clear that for a useful relationship to exist between the



opacity and mass concentration of the particulate emissions from a pol-



lution source, the characteristics of the particulates (size, shape, and



composition) must be sufficiently constant, and for a conventional trans-



missometer to be useful as a monitor of the mass concentration,  the



particulate characteristics must remain constant over a useful period of



time.  Some experimental data are available that show good empirical



opacity-mass concentration calibrations can be obtained for transmissometers



on some sources (Figures 10, 11, and 12).  Although these data indicate the



particle characteristics were sufficiently constant during the time of



calibration, no data on the long-terra usefulness of the calibrations seem



to be available.  Considering the simplicity of the transmissometer, the



collection of such data seems to be highly desirable in order to evaluate



its potential as a mass monitor for specific sources.  It is likely that



particulate emission control equipment will also control the characteristic



of the aerosol that most affects the relationship  (particle size) and



improve the potential of the transmissometer as a mass monitor.
                                                                          21

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   30
   25
*  20
I   «
CO
to
n



i
                  0.10




                  0.09



                  0.08



                  0.07



                  0.06
                                                                                        0.05 £
                                                               STANDARD CONDITIONS

                                                               DRY GAS
                0.02
0.12
0.14
                0.04        0.06       0.08        0.10


                          MASS CONCENTRATION, g/m3

Figure 10. Opacity-mass concentration relationship for particulate emissions

from a kraft recovery furnace.16
                      UJ
                      O
                      o

                  0.04 z
                      o



                  0.03 ^

                      2
                      ui


                  0.02 £




                  0.01




                  0
  22

-------
    45
    40
~  30
o   20
    10
                                                            0.30
                                         STANDARD CONDITIONS
                                         DRY GAS
                 0.1          0.2         0.3
                       MASS CONCENTRATION, g/m3
                                                0.4
                                                                0.20
                                                             0.15 it
                                                                o
                                                                o
                                                                z
                                                                o
                                                                <
                                                             0.1 Oz
                                                            0.05
0.5
   Figure 11. Opacity-mass concentration relationship for paniculate
   emissions from a cement plant kiln.17
§
2
o
60

50

40

30
20
10
                                          STANDARD CONDITIONS
                                          DRY GAS
  0.20
  0.18.
  0.16
  0.14
  0.12
  0.10
  0.08
  0.06
  0.04
  0.02
            0.1      0.2     0.3     0.4      0.5    0.6
                        MASS CONCENTRATION. g/m3
                                                    0.7
0.8
    Figure 12. Opacity-mass concentration relationship for particulate
    emissions from a bituminous coal-fired boilerJo
                                                                               23

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                REMOTE MEASUREMENT  OF PLUME OPACITY




     There are three instrumental methods that  have  been described  for



remote measurement of plume opacity.  Two of the methods use photometry of



the sun or of contrasting targets through the plumes for the measurements.



These methods are considered methods  of opportunity  since  they  are  applicable



only under certain conditions.   The third method is  more general  and uses a



laser radar (lidar) technique.   With  this method,  the plume opacity is



determined by shooting a pulse  of light through the  plume  and measuring the



ratio of the light backscattered from the pulse by the atmosphere before and



after the plume.




SUN PHOTOMETRY



     Measurement of plume opacity by  sun photometry  is restricted to times



when the sun is unobstructed by clouds  and may  be viewed through  a  discrete



cross section of the plume at the stack exit.  Conditions  for the measure-



ment are usually best on clear days when the sun is  relatively  low  in the



sky, the sun can be viewed through the  plume at the  stack  exit, and the



direction of flow of the dispersing plume in the atmosphere  is  away from



the sun.  A sun photometer specifically designed for plume opacity  measure-



ments is available from the Shell Development Company. The measurement can


                                                                           19
also be made with a standard sun photometer, e.g., the Volz  sun photometer.



However, it may be necessary to modify  the spectral  response of the standard



sun photometer to obtain good sensitivity to visible light.  A  Volz sun



photometer modified for plume opacity measurements has been  described.
                                    24

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CONTRASTING TARGET TELEPHOTOMETRY
     Measurement of plume opacity by contrasting target telephotometry is
restricted to times when contrasting targets can be viewed through the plume
at the stack exit and to times when the ambient illumination of the plume is
stable during the measurement.  The contrasting targets may be distant hills,
tall buildings, or towers and the sky adjacent to them.  For the plume
illumination to be sufficiently stable during the measurement normally
requires that the sky be clear or uniformly overcast.  The plume opacity is
determined by using a narrow-angle-view (less than 1/2 degree) telephotometer
to measure the ratio of the luminance difference between targets when viewed
through and beside the plume.  Narrow-angle telephotometers suitable for the
measurement are commercially available.
     It is also feasible to determine the opacity of a plume by photo-
graphing the contrasting targets through them, e.g., from a helicopter.  The
ratio of the luminance differences between the targets is then measured from
the film images with a laboratory densitometer.  Plume opacity measurements
by telephotometry and photography of contrasting targets have been described
•  j *  -i 6,20
in detail.

LIDAR
     The technique of determining plume opacity by lidar was first proposed
to the  Edison Electric Institute and the U. S. Public Health Service by the
late M.G.H. Ligda of Stanford Research Institute  (SRI) during the middle
1960's.  EEI and PHS pursued  the development of the technique as part of a
cooperative research study in the measurement of the opacity of plumes from
stacks  of steam electric power plants.  They contracted SRI to conduct a
laboratory and field study of the method using existing SRI lidar equipment
                                                                           25

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designed for atmospheric studies.  The results indicated the method was



feasible and defined many of the design parameters needed for a lidar


                                      21
system for plume opacity measurements.    The General Electric Company



was then contracted to develop a mobile lidar system specifically designed


                                        20 22
for remote measurement of plume opacity.  '     The performance of the lidar



is presently being evaluated by the Environmental Protection Agency in con-



junction with studies to develop and evaluate opacity measurement methods



for various sources.



     Application of the pulsed lidar system described above is primarily


                                 ^

for opacity research studies and for further development of the method.  In



its present form the instrument would have little application for surveil-



lance work by a control agency because of cost, operating power, and com-



plexity.  For the development of a smaller, low-powered, and less expensive



instrument for remote measurement of plume opacity, a lidar technique using



a frequency modulated, continuous wave  (CW) laser is being investigated.



The initial investigation of the CW lidar indicates that the method is


                                             23
feasible, and further development is planned.
 26

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                       SUMMARY  AND CONCLUSIONS





     Visible emission standards have been used  for  regulating  the parti-




culate emissions of stationary sources  for more than  75  years.  During




most of this period, the regulations applied only to  emissions that



appeared gray or black, and the primary method  of measuring  the blackness




of the emissions was the Ringelmann Chart comparators.   However, during



the past 20 years, visible emissions regulations have been extended  to



any emission affecting visibility regardless of color.   This general




application of the visible emissions regulations has  been accomplished by



defining the emission standards in terms of the opacity  of the plumes



emitted by the sources.  Plume opacity is an intrinsic optical property



of the emissions that is measured instrumentally by light transmission



methods.  To permit the older Ringelmann number standards to also be




measured by light transmission methods, a Ringelmann  number  1, 2, 3, 4,-



opacity 20, 40, 60, 80 equivalency is normally accepted.



     Opacity of plumes is also measured by trained  smoke observers who



attend a smoke-reading course where they are taught to assign  opacity



values to plumes based on their appearance.  The inspectors  become certified



smoke readers when they learn to assign opacity values to a  range of black



and white training plumes with a specified accuracy relative to a calibrated



in-stack transmission meter.  It should be noted that the trained observer



is not actually evaluating the visibility of plumes but  is evaluating the



opacity of plumes by observing their visibility.  The actual visibility  of



plumes is generally too dependent upon ambient illumination  and background



viewing conditions to be well regulated by opacity standards.   The plume




                                    27

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visual effect best regulated by the opacity standards is the obscuration




of visibility.




     The transmissometer used to measure the opacity of particulates must



have two essential design features.  The spectral response of the instru-




ment should be limited to visible light and, moreover, should be mostly



sensitive to green light.  The instrument should also be designed with




light collimating optics to exclude light scattered by the particulates




from the measurement.  A properly designed and installed in-stack transmis-




someter should be capable of monitoring the opacity of the plume emitted




from the stack provided water in condensed form is not present and the




characteristics of the aerosols in the effluent are maintained between the




in-stack measurement point and the plume.




      In considering the relationship between opacity and mass concentration



of a particulate emission, it should be recognized that the opacity of the




emission is a stack-size dependent measurement, whereas its mass concentra-



tion  is not.  In addition, the relationship between the opacity or light



transmittance and mass concentration of particulate  emissions is complicated



due to its dependence upon the characteristics of the particulates, e.g.,



size, shape, composition, etc.  Nevertheless, as the opacity of the particu-



late  emissions approaches zero, their mass concentrations also approach zero;



consequently, limiting the opacity of the emissions has the effect of




limiting their mass concentration.



      Although only a  limited opacity-mass concentration relationship can be




expected between sources of different sizes and particulate characteristics,



or for sources with fluctuating particulate characteristics, a good opacity-





28

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mass concentration relationship can be expected for sources with particulate



characteristics that are stable.  Development of such relationshipj  is




usually done by empirical calibration of a transmissometer on the source with




an accepted manual gravimetric sampling method.  Good empirical opacity-mass




concentration calibrations have been obtained for transmissometers on a




number of stationary sources; however, the precision of the calibrations for



long-term mass monitoring of the sources by transmissometry has not been



determined nor has the precision of the calibration within a source category



been determined.  Clearly, the usefulness of the calibration depends on the



stability of the particulate characteristics of the source and the similarity



of the particulate characteristics between sources within a source category.



     Remote instrumental measurement of plume opacity is complicated by the



ambient light scattered by the plume in the direction of the viewer.  This



scattered light generally prevents opacity measurement by simple plume-to-



background contrast measurements by direct telephotometry or by photometry



of plume photographs  although  such methods may at times give reasonable



estimates of plume opacity if the plume consists of light-absorbing particles



such that the amount of light scattered by the plume toward the viewer is



small when compared to the brightness of the plume background.



     Two relatively simple methods exist for remote instrumental measurement




of opacity, but both are methods of opportunity.  They are through-the-plume



photometry of the sun and telephotometry of contrasting targets.  The sun



photometer method is most applicable in those areas with a large number of



clear days. It is also limited to those sources whose plumes can be viewed with
                                                                             29

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the sun behind them.  The telephotometry-of-contrasting-target method is




limited to those sources whose plumes can be viewed with contrasting scenes




behind them, e.g., a hill or building and the adjacent sky.  The method is




difficult to apply if the environmental or background lighting conditions



of the plumes or the opacity of the plumes is fluctuating.




     A more general laser radar (lidar) method for remote measurement of




plume opacity is being developed, but at present the instrumentation is




complicated and expensive.  Development of simpler instrumentation for the



method is being pursued.
  30

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                                 REFERENCES

 1.   Ringelmann,  M.   Method of Estimating Smoke  Produced  by  Industrial
     Installations.   Rev.  Techniques.   268-271,  June  1898.

 2.   Coons,  J.  D.,  H. A.  James,  H.  C.  Johnson,  and M.  S.  Walker.   Develop-
     ment, Calibration,  and Use of  a Plume Evaluation  Training Unit.
     Journal of Air Pollution Control  Association lj^: 199-203,  May 1965.

 3.   Rose, A.  H., J.  S.  Nader, and  P.  A.  Drinker.   Development of an
     Improved Smoke Inspection Guide.   Journal  of Air  Pollution Control
     Association 8^:112-116, August  1958.

 4.   Rose, A.  H., and J.  S. Nader.   Field Evaluation  of an  Improved Smoke
     Inspection Guide.  Journal of  Air Pollution Control  Association  8_:117-
     119,  August 1958.

 5.   Conner, W. D.,  C. F.  Smith, and J.  S. Nader.   Development of a Smoke
     Guide for the Evaluation of White Plumes.   Journal of  Air Pollution
     Control Association l&i748-758, November 1968.

 6.   Conner, W. D.,  and  J.  R.  Hodkinson.   Optical Properties  and Visual
     Effects of Smoke-Stack Plumes.   U.  S. Public Health  Service Publica-
     tion  No.  999-AP-30.   NTIS Publication Number PB  174-705.   Springfield,
     Virginia,  1967.   89pp.

 7.   Standards of Performance for New Stationary Sources.  Federal Register
     36 (247):24876-24895,  December 23,  1971.

 8.   Halow,  J.  S.,  and S.  J.  Zeek.   Predicting  Ringelmann Number and  Optical
     Characteristics  of Plumes.   Journal of Air Pollution Control Association
     23^:676-684,  August  1973.

 9.   Hodkinson, J.  R.  The Optical  Measurement  of Aerosols.   In:   Aerosol
     Science,  Davies, C.  N. (ed.).   New York,  Academic Press,  1966. p.288.

10.   Ensor,  D.  S., and M.  J.  Pilat.   The Effect of Particle Size Distribution
     on Light Transmittance Measurement.  American Industrial  Hygiene Associa-
     tion  Journal 32_: 287-292, May 1971.

11.   Peterson,  C. M., and M.  Tomaides. In-Stack Transmittance  Techniques for
     Measuring Opacities of Particulate Emissions from Stationary Sources.
     Prepared for EPA by Environmental Research Corporation under Contract
     Number  68-02-0309.   NTIS Publication Number PB 212-741.   Springfield,
     Virginia,  April 1972.   87pp.

12.   Nader,  J.  S., F. Jaye, and W.  Conner.  Performance Specifications for
     Stationary Source Monitoring Systems for Gases and Visible Emissions.
     Environmental Protection Agency.   Publication Number EPA-650/2-74-013.
     Research Triangle Park,  N. C.   January 1974.  74p.

                                      31

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13.   Pilat,  M.  J., and D.  S. Ensor.  Plume Opacity and Particulate Mass
     Concentration.  Atmospheric Environment.   4_: 163-173,  April 1970.

14.   Hodkinson, J. R.  The Physical Basis of Dust  Measurement by Light
     Scattering.  In:  Aerosols:  Physical Chemistry and Application.
     Spurney, K. (ed.).  Publishing House of the Czechoslovak Academy  of
     Science, 1965.  p.184.

15.   Uthe, E. E., and C. E. Lapple.  Study of Laser Backscatter by Particu-
     lates in Stack Emissions.  Prepared for EPA by Stanford Research
     Institute under Contract Number CPA 70-173.  NTIS Publication Number
     PB 212-530.  Springfield, Virginia.  January 1972.  58p.

16.   National Council for Air and Stream Improvement Test Report.  Pre-
     sented at West Coast Regional NCASI Meeting,  Portland, Oregon, 1972.

17.   Buhne,  K.W., and L. Duwel.  Recording Dust Emission Measurements  in
     the Cement Industry with the RM4 Smoke Density Meter made by Messrs
     Sick.  Staub ^2(8):19-26, August 1972.

18.   Schneider, W. A.  Opacity Monitoring of Stack Emissions:  A Design
     Tool with Promising Results.  The 1974 Electric Utility - Generation
     Planbook.  New York, Mc-Graw-Hill, 1974.  p.73.

19.   Volz. F.  A Photometer for Measuring Solar Radiation.  Arch. Met.,
     Geophys. and Blokl. BIO;100-131.  1959.

20.   Cook, C. S., G. W. Bethke, and W. D. Conner.   Remote Measurement  of
     Smoke Plume Transmittance Using Lidar.  Applied Optics 11:1742-1748,
     August 1972.

21.   Evens, W. E.  Development of Lidar Stack Effluent Opacity Measuring
     System.  Prepared for Edison Electric Institute by Stanford Research
     Institute under SRI Project Number 6529.  NTIS Publication Number
     PB 233-135/AS.  Springfield, Virginia, July 1967.

22.   Bethke, G. W.  Development of Range Squared and Off-Gating Modifications
     for a Lidar System.   Prepared for EPA by General Electric Company under
     Contract 68-02-0570.  Publication Number EPA-650/2-73-040.  Research
     Triangle Park, N. C., December 1973.  47pp.

23.   Ferguson, R. A.   Feasibility of a CW Lidar Technique for Measurement of
     Plume Opacity.  Prepared  for EPA by Stanford Research Institute under
     Contract Number 68-02-0543.  Publication Number EPA-650/2-73-037.
     Research Triangle Park, N. C., November 1973.  90p.
 32

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                                   TECHNICAL REPORT DATA
                            (Please read Instructions on the reverse before completing)
1. REPORT NO.

       IiPA-650/2-74-128
                              2.
                                                            3. RECIPIENT'S ACCESSION*NO.
4. TITLE AND SUBTITLE
       Measurement of the  Opacity and Mass  Concentration
       of Particulate Emissions by Transmissometry
             6. REPORT DATE
               November  1974
             6. PERFORMING ORGANIZATION CODE
7. AUTHORIS)

        William D. Conner
                                                            8. PERFORMING ORGANIZATION REPORT NO.
9. PERFORMING ORGANIZATION NAME AND ADDRESS

       Chemistry and  Physics Laboratory
       Environmental  Protection Agency
       National Environmental Research Center
  	Research Triangle  Park.  N.C.  27711
             10. PROGRAM ELEMENT NO.

                     10    ROAP No.  26AAM
             11.C
ACT/GRANT NO.
12. SPONSORING AGENCY NAME AND ADDRESS
                                                            13. TYPE OF REPORT AND PERIOD COVERED
                                                            14. SPONSORING AGENCY CODE
IB. SUPPLEMENTARY NOTES
16. ABSTRACT
        This report is  a  review of particulate opacity measurement techniques.
        The relationship  between the opacity of plumes and  their visual  effects,
        and the relationship between the  opacity of plumes  and their particulate
        mass concentration are discussed.   The report also  discusses optical
        design characteristics of transmissometers that are necessary for
        measurement of  the opacity of particulate emissions.  Various methods
        for remote measurement of plume opacity are reviewed including the
        visible emission  observer.
17.
                                KEY WORDS AND DOCUMENT ANALYSIS
                  DESCRIPTORS
                                               b.lOENTIFIERS/OPEN ENDED TERMS
                           c.  COSATI Field/Group
        opacity
        visible emissions
        transmissometry
        particulate  emissions
        lidar
        photometry
18. DISTRIBUTION STATEMENT

   Release unlimited
19. SECURITY CLASS (This Report)
  None
       21. NO. OF PAGES
           39
                                               20. SECURITY CLASS (Thispage)
                                                 None
                                                                          22. PRICE
EPA Form 2220-1 (9-73)
                                              33

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