Sulfur Deposition Modeling In Support Of The Uscanadian Memorandum Of Intent On Acid Rain


                                            600783058
  SULFUR DEPOSITION  MODELING  IN SUPPORT OF THE
U.S./CANADIAN MEMORANDUM  OF INTENT ON ACID RAIN
                       by

                 Terry L.  Clark
                Dale H.  Coventry
      Meteorology and Assessment Division
   Environmental  Sciences  Research Laboratory
      U.S. Environmental  Protection Agency
 Research Triangle Park,  North Carolina  27711
    ENVIRONMENTAL SCIENCES RESEARCH LABORATORY
        OFFICE OF RESEARCH AND DEVELOPMENT
       U.S.  ENVIRONMENTAL PROTECTION AGENCY
  RESEARCH TRIANGLE PARK, NORTH CAROLINA  27711

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                               DISCLAIMER

     This report has been reviewed by the Environmental  Sciences
Research Laboratory, U.S. Environmental  Protection Agency,  and approved
for publication.  Mention of trade names or commercial  products does
not constitute endorsement or recommendation for use.
                              AFFILIATION

     Mr. Clark and Mr. Coventry, meteorologists in the Meteorology and
Assessment Division, Environmental Sciences Research Laboratory, Research
Triangle Park, NC 27711, are on assignment from the National Oceanic
and Atmospheric Administration, U.S. Department of Commerce.
                                  11

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                                PREFACE

     On August 5,  1980,  the Unitad States and Canada signed the Memorandum
of Intent on Transboundary Air Pollution, which established bilateral
scientific work groups to develop a consensus on the nature of the
trahsboundary air  pollution problem.  The resulting consensus would then
provide the basis  for the negotiation of a cooperative agreement on the
problem.

     During the ensuing year, the Environmental  Sciences Research
Laboratory (ESRL)  of the U.S. Environmental Protection Agency (EPA) at
Research Triangle  Park, North Carolina, participated in the Atmospheric
Sciences and Analysis Work Group (Work Group 2).  The goals of this
work group were 1) to describe the current state of the knowledge of
long-range transport, chemical transformation, and wet and dry sulfur
deposition modeling, 2) to define source/receptor relationships,
particularly for sensitive areas of eastern North America, and 3) to
assess and intercompare model results using atmospheric and precipitation
chemistry measurements.

     To accomplish these goals, Work Group 2 selected eight Canadian
and U.S. long-range transport models to be applied by the Regional
Modeling Subgroup.  The Eastern North American Model of Air Pollution
(ENAMAP-1), developed by SRI  International under EPA sponsorship, was
one of the models selected.  This report describes in detail the
technical aspects of the model and the results of the applications
performed at the request of Work Group 2.  This report documents the
actual scientific work performed by ESRL; a condensation of the material
in this report is presented in the Work Group 2 and Regional Modeling
Subgroup Final Reports.
                                   m

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     The model results presented and discussed in this report are deemed
to be preliminary and should not be. used as. a_ basis for the development
of regulatory policies. The results of these model applications are doc-
umented solely for the benefit of the scientific community. Further
model input/output and parameterization uncertainty analyses and a rig-
orous validation study must be accomplished to establish the credibility
of the model before it can be used as a regulatory tool. The uncertainty
analyses and the model validation study are to be conducted during 1983
and 1984.
                                iv

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                                ABSTRACT

     At the request of the U.S./Canadian Work  Group  2  of  the  Acid  Rain
Memorandum of Intent, the Eastern North American  Model  of Air Pollution
(EMAMAP-1) was applied to simulate the monthly wet and dry depositions
and "monthly averaged ambient concentrations  of S02 and $04 for January
and July 1973 across eastern North America.   Using these  model  results,
unit emissions (1.0 Tg S yr~M  transfer matrices, which describe source/
receptor relationships, were generated and a model performance study was
undertaken.  In addition, a model sensitivity study  was conducted  to
examine the consequence of model input parameter  uncertainties.

     The unit emission transfer matrices indicated that in July those
source regions closest to the sensitive receptors dominated the sulfur
wet deposition at those receptors.  During January,  the contributions
from the more distant source regions increased significantly  and one
source region did not dominate the sulfur deposition across the north-
eastern U.S. sensitive receptors.

     The January and July 1978 model results compared favorably with
the measured sulfur wet depositions (16 observations) and monthly
averaged  ambient SO^ concentrations (76 observations).  The mean
residuals  of the former and latter were of the order of 0.25  kg ha-*
and 0.4   v g m~3, respectively.  The mean calculations were within 20%
of the mean sulfur wet deposition and within 8% of the mean ambient
$04 concentrations.

     The  sensitivity analysis, which examined changes in the calculations
as a function of downwind distance, up  to 1500 km from a single source,
indicated that for high transport wind  speeds (>35 km h-1), a saw-
toothed downwind distribution of depositions and concentrations resulted
from simulations using 2- and 3-h time  steps.  The saw-toothed distribu-
tion also was noted  for moderate wind  speeds  (>20, but <35 km h~M in
the  simulations using  3-h time  steps.   In general, the greatest changes

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in the S02 wet depositions and  ambient concentrations occurred within 200
km of the source,  while those  in  the  SO^ wet depositions  and  ambient
concentrations occurred beyond  300  km.

     This report discusses the  work performed from October  1,  1981  to
April 30, 1982.
                                 VI

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                               CONTENTS


Preface                                                         iii
Abstract                                                        .Y.
Figures                                                        v1'11
Tables                                                           x

     1.  Introduction                                             1

     2.  Model Description                                        2

           Parameterizations                                      2

           Meteorological Fields                                 10

     3.  Model Applications and Evaluation                       12
           Applications                                          12

           Evaluation                                            14

     4.  Model Sensitivity Study                                 23

           Design                                                23

           Results                                               23

     5.  Summary and Conclusions                                 53

References                                                       57
Appendices                                                       58
     A.  44 by 44 Unit Transfer Matrices for January
            and July 1978                                        58
     B.  Unit Transfer Matrices for 11 Consolidated
            Emission Regions and 9 Sensitive Receptor
            Regions for January and July 1978
                                    vii

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                                 FIGURES

Number                                                               Page

  1    The 46 by 41  ENAMAP-1  grid network                               4

  2    Depiction and summary  of  ENAMAP-1 parameterizations              6

  3    The 9 sensitive areas  of  North America as
       designated by Work  Group  2.                                     14

  4    The 40 source/receptor regions of North America
       as designated by Work  Group  2.                                  14

  5    The location  of the sulfur wet deposition  sites and
       the ambient SO^ monitoring sites included  in Table 3.           '8

  6    The 1500-km track used for transport  of pollutant puffs
       from southern Ohio  in  the ENAMAP-1  sensitivity study.           25

  7    The 96-h average ambient  SO* concentrations  (ug m"3)
       at specific distances  upwind and downwind  of a single  source.   28

  8a   Wet depositions (mg nr2)  and concentrations  (ug nr3) of
       S02 and S0| as a function of wind speed (km  h"1) distance
       (km) downwind of the source.                                   30

  8b   Wet depositions (mg nr2)  and concentrations  (mg nr3) of
       SOo and SOJj as a function of precipitation rate  (mm h"1)
       and distance (km) downwind of the source.                       31

  8c   Wet depositions (mg nr2)  and concentrations  (mg nr3) of
       SOo and S0| as a function of puff expansion  rate  (km2  h'1)
       and distance (km) downwind of the source.32

  8d   Wet depositions (mg nr2)  and concentrations  (mg nr3) of
       SOo and SO^ as a function of transformation  rate  (% h"1)
       ana distance (km) downwind of the source.                       34

  8e   Wet depositions (mg nr2)  and concentrations  (mg nr3) of
       S02 and S0| as a function of mixing height (km)  and
       distance  (km) downwind of the source.                          35

  8f   Wet depositions (mg nr2)  and concentrations  (mg nr3) of
       SOo and SO^ as a function of initial  puff size (km)
       and distance (km) downwind of the  source.                       36

  8g   Wet depositions (mg nr2)  and concentrations  (mg  nr3) of
       S02 and SO 4 as a function of $02 wet deposition  rate
       (% mm"1)  and distance  (km)  downwind of the source.37

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Number                                                                Page

  8h   Wet depositions (mg m~2)  and concentrations  (mg  m~3)
       of S02 and S0| as a function of SO!*  wet deposition
       rate and distance (km)  downwind of the  source.                   39

  8i   Wet depositions (mg m~2)  and concentrations  (mg  m~3)
       of S02 and SO^ as a function of SOg  dry deposition
       factor and distance (kn)  downwind of the source.40

  8j   Wet depositions (mg m~2)  and concentrations  (mg  m-3)
       of S02 and SO^ as a function of SO^  dry deposition
       factor and distance (km)  downwind of the source.41

  8k   Wet depositions (mg m-2)  and concentrations  (mg  nr3)
       of S02 and SO* as a function of SO?  emission rate
       (kton h'1) ana distance (km) downwind of the source.             43

  81   Wet depositions (mg m~2)  and concentrations  (mg  m~3)
       of S02 and SO* as a function of $0^  emission rate
       (kton h~l) ana distance (km downwind of the  source.              44

  8m   Wet depositions (mg m~2)  and concentrations  mg m-3)  of
       S02 and SO^ as a function of SOo loss rate from
       mixed layer top (kton h~l) and distance (km) downwind
       of the source.                                                  45

  8n   Wet depositions (mg m-2)  and concentrations  (mg  m~3)  of
       S02 and S0| as a function of SO* loss rate from
       mixed layer top (kton h~l) and distance (km) downwind
       of the source.                                                  46

  9    Wet deposition of sulfur (mg m~2) per unit change in
       model input parameters as a function of distance (km)
       downwind of the source.                                         47

  10   Wet depositions and concentrations of SOp and S0|
       downwind of a single source as calculated from high  (*),
       basa  (x), and low (+) case sets of model input parameter
       values.                                                         50

  B-l  The 11 consolidated emission regions used in the condensed
       transfer matrices.                                             120

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                                  TABLES

Number                                                              Page

  1       Transformation  and Deposition  Rates  Suggested
          by Several  Investigators.                                    8

  2       Estimated 1978  S02 Emissions  for  the 35  Regions
          Within the ENAMAP-1 Domain.                                  17

  3       Modeled and Measured Monthly  Total  Sulfur Wet
          Depositions and Monthly  Average Ambient  SO^
          Concentrations                                               19

  4       Values of Statistical  Parameters  Calculated  for
          the ENAMAP-1 Results.                                        22

  5       Model  Input Parameter Values  Considered  in the
          Sensitivity Study.                                          24

  6       Maximum Changes in Wet Sulfur Deposition for
          Unit Increases  in Model  Input Parameters.                   48

  7       Extreme Values  Used in Two Applications  to
          Produce Minimum and Maximum Sulfur Wet
          Deposition Within 500 km of the  Source.                      49

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                                SECTION  1

                               INTRODUCTION

     In the mid 1970's,  SRI International  developed a Lagrangian-puff  air
pollution mdoel,  European Regional  Model of  Air  Pollution (EURMAP)  for
the Federal Environment Office of the Federal  Republic of Germany  (Johnson
et al., 1978).  This regional  model  was  capable  of calculating monthly
S02 and SO^ concentrations and dry and wet deposition patterns and
international  exchanges of sulfur across 13  countries of western and
central Europe.

     In the late  1970's, the U.S. Environmental  Protection Agency  (EPA)
sponsored SRI  International to adapt and apply EURMAP to easterh North
America.  The adapted version of this model, ENAMAP (Eastern North American
Model of Air Pollution), was capable of  calculating monthly S02 and S0|
concentrations and dry and wet deposition  patterns and interregional
exchanges of sulfur across a user-defined  number of regions (Bhumralkar
et al., 1980).  Thus it was possible to  assess the impact of sulfur
emissions from individual sites and provinces on the sulfur concentrations
and depositions across the same regions.

     In 1981, the ENAMAP-1 model was included as one of eight long-range
sulfur pollution models applied by the Atmospheric Sciences and  Analysis
Work Group (Work Group 2) of the U.S./Canadian Memorandum of Intent on
Transboundary Air Pollution.  This report  summarizes the work performed
by ESRL at the request of Work Group 2.   Such work included the  application
of the ENAMAP-1 model using January and July 1978 input data to  generate
transfer matrices, to assess model performance,  and to analyze model
sensitivity in input parameters.

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                                SECTION  2

                            MODEL  DESCRIPTION

Parameter"! zations

Basic structure

     In the design and development of any  air  quality simulation model,
there are usually two conflicting  goals: maximum  realism  and  accuracy  on
one hand, and minimum computational  requirements  on the other.  Greater
realism and accuracy usually require more  detailed information  and
sophisticated formulations of physical  processes, which in  turn require
more computer time and memory capacity.   It was clear from  the  outset
that the computer requirements could be severe for two reasons:

     1) The model must treat a very large  geographical area (2870  km
        north to south and 3220 km east to west)  and yet  preserve  acceptable
        spatial resolution (70 by  70 km).
     2) The model must compute monthly land annual mean concentration  and
        deposition fields while preserving the original  temporal  resolution
        (12 h) of standard meteorological  data; thus, the model must make
        repetitive calculations for long sequences of input data.

     Accordingly, as a first step, it was desirable to design a very
simple model having minimum computer requirements (i.e.,  a practical and
economical model that would offer acceptable realism in simulating the
most important processes involved in' the transboundary sulfur pollution
problem.  More sophisticated parameter!zations can replace the simplistic
approaches described here as knowledge  of the appropriate physical
processes accumulates.  Later, the simplistic parameter!'zations of vertical

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mixing, dry and wet depositions, and transformations of S02  will  be  replaced
by more sophisticated parameter! zations by the  end  of 1982.   Also by the
end of 1982, NOX chemistry will  be added to the model.

     EMAMAP-1 can calculate S02  and SO^ concentrations, wet  and  dry
depositions, and interregional  sulfur exchanges across  a 46  by 41 grid
network with a 70 -km resolution  (Figure 1).  Basically, ENAMAP-1 is  a mass-
conserving, Lagrangian puff model .  Linear chemical  processes within each
puff are parameterized as the puff is transported across the modeling
domain.  No additional emissions are added to the puff  while it  is transported.

     The concentrations within and the depositions  from each puff are
calculated at 3-h intervals.  The calculated concentrations  and  depositions
at each 3-h interval are apportioned to the grid cells  depicted  in Figure  1
on the basis of the portion of the puff area in each of these cells.

     The rate of loss of mass of S02 (dMj/dt) and $04 (dM2/dt) from  each
puff can be expressed by the following:
                 = -M(kt + kdl + kwl)     and

          dM2/dt = -M(-3kt/2 + kd2 + kw2)
where M = mass (kton)
      t = time (h)
      k^ = transformation rate of S02 to SO^ (h~*)
      k(j = dry deposition rate (h  )
      kw = wet deposition rate (h-~l).

The  3/2 factor in the second equation is the ratio of molecular weights
between SO^ and S02.

      It should be noted that there are significant disagreements among
atmospheric scientists about the magnitude of these rates.  This lack of a
consensus is responsible, to a significant degree, for the wide variations
in the model results generated by the eight models of Work Group 2.

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 o
 OJ
 s_
 en
 i
a.
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•=3-
 OJ
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Pol 1utant Transport

     Discrete puffs of S02 and S0| are released every 12 h from the 70  by
70 km emission grid cells, which coincide with the receptor cells.   The
mass of pollutants in each new puff is determined by dividing the annual
emissions in each cell  by 730, the number of 12-h periods in a year. As
Figure 2 illustrates, these puffs are transported using 3-h time steps
until 1) the puff is transported out of the model domain or 2) the mass of
S02~and SO^ in the puff decreases to less than 0.01 and 0.001 kton,
respectively.

     The individual puffs are transported across the model grid using
vertically integrated and horizontally interpolated wind fields applicable
at the respective time period.  The generation of these wind fields is
discussed in a subsequent subsection.

Diffusion

     Since, on the regional scale, diffusion is less significant than the
transport and removal processes, ENAMAP-1 parameterizes horizontal  and
vertical diffusion very  simply.  Upon release, each puff is assumed to
diffuse vertically in a  manner that produces, instantly, a thoroughly
mixed layer between  the  surface of the earth and the user-specified mixing
height.

     As parameterized in the  model, the mixing height, H  (km), is uniform
across  the  grid  network.  The actual  value used  in  the model applications
for  a month long period  does  not change and is determined  solely on the
season  according to  the  relation:

          H = 1.3 +  0.15 S

where S = -1  in  winter,  +1  in summer, and 0 in spring/autumn.  The  value
ranges  from 1.15 km  in winter to  1.45 km  in summer.  The model parame-
terizes diffusion  across the  top  of  the mixed layer according  to a
user-specified  rate.
                                    5

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 •70 km-!
               PUFFS ADVECTED WITH
              -OBSERVED  WIND FIELDp
               AND TRACKED AT     |
               3-HOUR TIME STEPS   i
     SO2 - S0|
     AT ASSUMED
     RATE OF 1%/HR
  EMISSIONS  "PUFFS"
 j RELEASED  EVERY
 r12 HOURS FROM
 j EACH EMISSIONS
 !GRID CELL
  DIFFUSION ASSUMPTIONS:
  FICKIAN (%t%) IN
  HORIZONTAL; UNIFORM
 "MIXING IN VERTICAL
  UP TO MIXING HEIGHT
CONCENTRATION  AND WET
AND DRY DEPOSITION
AMOUNTS ASSIGNED  TO
EACH RECEPTOR CELL  AT
EACH TIME  STEP  ACCORDING
TO CELL AREAS COVERED
BY PUFF
Figure 2.   Depiction and summary of ENAMAP-1 parameterizations.

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The initial horizontal  cross-sectional  area of each puff is  defined as the
area of a 70-grid square.  Fickian diffusion is then assumed during the
transport of the puffs so that at any time, t (h),  the radius,  r (km), of
any puff is

          r = (rj + Kht)1/2

where r0 is the initial  radius of the puff (km) and Kn is the horizontal
eddy diffusion coefficient (36 km2 h"1, or approximately 104 m^ s~M.

Transformation

     Although transformation of S02 to SO^ is recognized to  be  a significant
complex process in long-range transport, ENAMAP-1 parameterizes this process
very simply.  The transformation rate seems to be dependent  upon many
                                                            *
factors, some of which (e.g., relative humidity, clouds, precipitation
type, atmospheric stability, and solar radiation) can be parameterized with
a tolerable degree of accuracy and some of which (e.g., concentrations of
other chemical species,  such as ammonia and metal catalysts) cannot
(Weber, 1971).  However, the relationships between  the transformation  rate
and many of these factors are not precisely known.   Until  these relationships
are better known, the simplistic treatment of the transformation seems to
be a reasonable approach.

     In the ENAMAP-1 model, the transformation rate is constant throughout
the modeling period: it does not vary with latitude, season, time of day,
or precipitation.  A value of the transformation rate was chosen after a
review of field, laboratory, and theoretical  studies was conducted by  SRI
International.  Table 1 lists the values suggested by some atmospheric
scientists and those selected for use in ENAMAP-1.   The significant
disagreement evident in Table 1 reflects «the lack of reliable experimental
derived values.

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            TABLE 1 .   TRANSFORMATION  AND  DEPOSITION  RATES
                      SUGGESTED  BY  SEVERAL  INVESTIGATORS
Investigator
S02 to S0$
transformation
rate (h-1)
Deposition coefficients (h~M
     Dry  _          Wet#
S02     SO?       S02
Ottar (1978)                0.007
Renne and Elliott (1976)    0.050
Rao et al . (1976)          0.015
McMahon et al . (1976)    0.010-0.020
Johnson et al . (1978)       0.010
Bhumralkar et al. (1980)*    0.010
                  0.036
                  0.036
       0.0144
       0.0036
                  0 .054   0 .0070
                  0 .029   0 .0070
                  0 .037   0 .0070
0.144
0.500
0.050
                  0.216   0.108
                  0.216   0.070
                  0 .280   0 .70
* These values were used in ENAMAP-1 applications.
# The values presented are the washout coefficients,  we,  where kw = wcR and R
  is the precipitation rate (mm h-1) .

Dry Deposition

     Of all the parameters in the model,  dry depositions  of S02 and S0|
are probably the most difficult to ascertain.  First of all, the dry deposi-
tion rates depend on specific types of vegetation and material surfaces.
Secondly, these pollutants are removed from the atmosphere as both aerosols
and gases at different rates.  Thirdly, there is no widely accepted procedure
to measure dry deposition, making it nearly impossible to relate the theories
with measurments .

     ENAMAP-1 parameterizes the dry deposition of S02 and of SO^ very simply.
They are not expressed as functions of land use, time of day, or the state
of the pollutants (aerosol or gaseous), but are treated as constants
throughout the modeling period.  The rates selected (identified in Table 1)
were determined from a consensus of values published in the literature.
These rates were used in earlier model applications performed by SRI,
International .  For the Work Group 2 work, however, the January dry deposition
rates of S02 and $04 were defined as 0.38 and 0.22 cm s'1, respectively;
the July rates were defined as 0.48 and 0.28 cm s~l .  These rates were
selected on the basis of suggestions by Shieh et al . (1979) and the other
Work Group 2 modelers.
                                      8

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Wet Deposition

     Although the wet deposition process is thought to be a function of the
cloud chemistry, cloud formation process, and the type of precipitation,
ENAMAP-1 parameterizes it as only a function of the precipitation rate.
For every 3-h simulation time step, the model  determines, via preprocessed,
objectively analyzed precipitation fields, the precipitation intensity in
the vicinity of each puff.  The 3-h precipitation rates are then multiplied
by the washout coefficients for S02 and SO^ (0.28 and 0.07 h"1, respectively)
to determine the total wet deposition from each puff during each time step.

     In the planned final ENAMAP version, the wet depositions are to be
functions of the precipitation rate raised to an empirically derived power.
This type of expression was used by Scott (1978) and McNaughton (1980).

Deposition and Concentration Patterns

     After each pollutant puff has been transported for a 3-h period, the
amount of S02 transformed to S0|, the resulting S02 and S0| concentrations,
and the amount of S02 and SO^ deposited from the puffs are determined in
that order.  Immediately afterwards, the 3-h depositions are apportioned to
the receptor grid squares according to the percentage of the cross-sectional
area of the puff over each square.  The mass of each pollutant is similarly
apportioned to each square.

     The monthly S02 and SO^ deposition patterns at the end of the month-
long simulation period are obtained by summing the 3-h contributions of
each puff to each receptor square.  Likewise, the 3-h contributions of the
mass of the two pollutants are summed for each grid square.  Monthly average
S02 and S0| concentration patterns are then obtained by dividing these
sums by the number of 3-h time steps in the month and the volume of the
receptor cell.  The mass  is assumed to be evenly distributed across each cell

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METEOROLOGICAL FIELDS

Transport Hind

Transport wind fields were generated  at  3-h  intervals  using the  7Q-km
receptor grid network and the 12-h  upper-air wind  data from several  Canadian
and about 50 U.S. sites.  At each of  these data  sites, average u and v
components of the transport wind within  the  simulated  mixed layer were
determined by the following formulae:
               I     (v,  +  v,  ,)
The subscripts denote pressure levels where wind data are available and I
represents the pressure level  closest to the simulated mixing height.

     The 46 by 41 transport wind fields were then generated from these
layer-averaged wind components by a distance-weighted interpolation scheme
using the weighting factor
          w =
              c
2 + R2
where c is 2500 km and R is the distance (km) between the grid point and the
observation point.

Precipitation

     Precipitation data with a resolution of 1 h were obtained from a dense
network of 2000 observational sites within the eastern and central U.S.  In
addition, precipitation data with a resolution of 6 h were obtained from
less than 200 observational sites (usually at airports) across the eastern
and central U.S. and southern Canada.

                                    10

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     Precipitation fields were generated for 3-h  intervals  using  the  same
70-km grid network.   For each grid cell  containing  a  6-h  precipitation
monitoring site, the 6-h average precipiation rate  was  computed.   Next,  3-h
average precipitation rates were computed for these cells by  assuming that
the measured 6-h precipitation occurred  at a constant rate.   For  cells
containing 1-h precipitation monitoring  sites, the  1-h  rates  were summed to
produce 3-h rates.  Finally, the average 3-h precipitation  rate was computed
for each grid cell for which data were available.

     For grid cells containing no precipitation monitoring  sites, but
adjacent to at least two cells containing such sites, simple  linear
interpolation was applied to estimate the 3-h rates.   Since precipitation
monitoring sites in southern Canada were sparse,  there  were many  clusters
of grid cells without monitoring sites,  especially  for the  winter months.
For these cells, the 3-h precipitation rates were assumed to  be equal to
those of the nearest cell having at least one monitoring  site.  The 3-h
rates over the Atlantic Ocean and the Gulf of Mexico  were estimated using
the same technique.
                                    11

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                                SECTION  3

                  MODEL APPLICATIONS AND EVALUATIONS

APPLICATIONS

     To accomplish its goals,  Work Group 2 requested that each  of the eight
long-range transport models generate the following model  output:

     1) annual  1978 unit transfer matrices of wet sulfur  deposition,  dry
        sulfur deposition, ambient S02 concentrations,  and ambient S0|
        concentrations normalized by a 1.0 Tg S yr"1 emission rate from
        each of the 40 source/receptor regions and 9 sensitive  receptors
        defined by Work Group 2, and
     2) January, July and annual 1978 wet sulfur depositions and average
        ambient S0| concentrations at monitoring sites  selected by Work
        Group 2.

The unit transfer matrices, although strongly influenced  by the meteorological
scenarios used in the simulation period, were to be used  by another work
group to assess the merits of several emission scenarios.  From these
transfer matrices, the effects of emissions from individual regions on the
sulfur  depositions and ambient concentrations across the nine sensitive
receptor areas (Figure 3) and the 40 source/receptor regions (Figure 4)
could be determined.  However, before any conclusions are drawn, one should
be aware of the caveats associated with the matrices (U.S ./Canadian Work
Group 2 Final Report, 1983; U .S ./Canadian Regional Modeling Subgroup Final
Report, 1983) .

     The January and July 1978 meteorological data used to generate the
transfer matrices were analyzed and gridded by preprocessors as described in
the previous section.  The emissions from each grid cell  within a given
source/ receptor region were multiplied by a constant factor so that the
total annual sulfur emissions from that region equaled 1.0 Tg.
                                    12

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                     ••  V
                     « /

                     2  \
                 "
                              V:
                    9»
                            X
Figure 3.  The 9 sensitive areas of North America as
           designated by Work Group 2.
Figure 4.   The 40 source/receptor regions of North America
           as designated by Work Group 2.
                           13

-------
     Since the meteorological  data  and analyses  for  the  entire year  of  1978
were unobtainable in the rather  brief  time  frame imposed upon the work
group, it was agreed that ENAMAP-1  would be applied  using only January  and
July 1978 input data.  Annual  estimates of  the transfer  matrices would  be
based only on matrices for those two months.  In addition,  since the ENAMAP-1
domain did not include western North America, only 35  instead of 40  source/
receptor regions were considered.

    -The ENAMAP-1 January and July  1978 unit transfer  matrices  are  presented
in the appendices in two forms.  In Appendix A,  the  complete unit transfer
matrices relate the impact of 1.0 Tg S yr"l emitted  by each of  the  35
regions on the sulfur depositions and  ambient sulfur concentrations  in  that
region.  The unit transfer matrices in Appendix  B relate the  impact  of  1.0
Tg S yr~l emitted from 11 consolidated regions on the  sulfur wet deposi-
tions and ambient S0| concentrations  in the 9 sensitive  receptor areas.
For all sets of transfer matrices,  the regional  distribution  of  emissions
was preserved.

     The transfer matrices indicated  that the sources  within  any  1  of the  35
regions contributed significantly to  the sulfur  depositions and concentra-
tions within that region.  In January, on the average, 68% of  S02 wet
deposition in a particular region was  a direct result  of 862 emissions
from that region.  Similarly, in July, an average of 64% of the $03 wet
deposition in a particular region resulted from  S02  emissions  from  that
region.  Since the ENAMAP-1 results indicated that much of the sulfur wet
deposition consisted of $63 wet deposition (in some  cases, wet deposition
of SC>2 was an order of magnitude greater than that of  S0|), the model
indicated that local sources have a very significant role in sulfur wet
deposition.

EVALUATION

      An ideal assessment of the performance of any regional sulfur model
would  require an extensive data base of dry sulfur depositions, wet sulfur
                                     14

-------
depositions,  and ambient S02 and S0| concentrations  measured  during  all
seasons of the year across all  portions  of the modeling  domain  that  are
removed from the effects of local  sources.  Unfortunately,  such a  data base
does not exist.  However, daily average  concentrations  of S02 and  S0|
from 1 Canadian and 53 U.S. sites were available from the Electric Power
Research Institute's Sulfur Regional Experiment (EPRI-SURE) .   Monthly sulfur
wet deposition data for these periods were available from several  Multistate
Atmosphere Power Production Pollution Study (MAP3S)  sites in  the northeastern
U.S.-and from about a dozen Canadian Network for Sampling Precipitation
(CANSAP) sites.  Together, these data formed the best available regional
sulfur modeling evaluation data base.

     Work Group 2 screened the data on ambient SO^ and sulfur wet depo-
sition for January and July 1978.  For the MAP3S network, precipitation
samples with a catch of less than 50% of a nearby rain gauge  measurement
were ignored.  Otherwise, the precipitation sample amount was adjusted to
the rain gauge measurement.  Valid monthly samples required a minimum 903
capture.  For CANSAP, 7 of the 16 operational  sites  were ignored because of
operational or siting problems.  Valid monthly samples required a  minimum
operational time of 20 and a minimum collection efficiency of 25% .  Collec-
tion efficiency was defined as the ratio (%) of the  precipitation  recorded
by the sampler to that measured by a colocated rain  gauge.  Since  even rain
gauges do not collect all of the precipitation (precipitation collection
efficiency is a function of gauge type,  site exposure, and wind velocity),
the rain gauge precipitation data from both networks were adjusted by Peck
(1982).

     The S02 emission data used in the evaluation study were  obtained from
several sources, since a complete 1978 emission inventory was not available.
Because much of the S02 was emitted from electric power plants, it was
imperative to accurately define the 1978 power plant emissions.  With this
in mind, Environment Canada prepared a 1978 S02 emission inventory for
large point sources.  Emissions from all other sources were assumed to be
the same as in 1976.  The 1978 S02 emissions from the U.S. power plants
                                    15

-------
were estimated from fuel  use records,  while  the  1978  emissions  from  all
other sources were assumed to be  the  same  as in  1980,  the year  for which
emissions data were available.

     Table 2 lists the total S02  emissions from  the  35 regions  used  in
this study.  These annual  rates were  used  by the other modelers of Work
Group 2 as well . To aggregate the total  state/province emissions to  a
useable grid network, the modelers used  an emission  inventory  for the
states/provinces that had been developed earlier by  Brookhaven  National
Laboratory.

     The emission data set was more precise  than the precipitation  data  set.
Due to the lack of extensive precipitation measurements in  Canada in the
winter, the 3-h precipitation amounts used in the. ENAMAP-1  applications  were
extrapolated for much of the Canadian portion of the grid  domain.  In
comparison to the data from the U.S. precipitation chemistry sites,  the
amounts measured at the Canadian  sites showed less agreement with the
monthly ENAMAP-1 precipitation amounts across the grid cells encompassing
each site.

     Because of the high spatial  variability of  precipitation,  especially in
the summer, the precipitation at two nearby sites can be significantly
different over any time period. Since most Work  Group 2 long-range transport
models assumed a constant precipitation  rate across each grid cell,  it is
sometimes frivolous to compare model-calculated   sulfur wet depositions  over
a rather large area to those measured at a single point.

     The monthly total sulfur wet depositions and the monthly average
ambient S0$ concentrations calculated for grid cells encompassing moni-
toring sites are compared to observations in Table 3.  Missing data are
indicated by the blanks.  The site locations are identified in Figure 5.  No
attempt was made "to compare  the observations to  interpolated values from the
ENAMAP-1 output fields.
                                    16

-------
TABLE 2.  ESTIMATED 1978 SOa  EMISSIONS  FOR  THE 35
             REGIONS WITHIN THE  ENAMAP-1  DOMAIN
             (U.S./Canadian Work Group  2, 1982)
Region number
11
12
13
14
15
16
17
18
19
20
21
22
50
51
52
53
54
55 '
56
57
58
59
60
61
62
63
64
65
66
67
68
69
70
71

72
State/province Total S02 emissions
Southern Manitoba
Northwestern Ontario
Northeastern Ontario
Sudbury, Ontario
Southwestern Ontario
Southeastern Ontario
Southern Quebec
Northern Quebec
Gaspe Bay, Quebec
New Brunswick
Prince Edward Island/Nova Scotia
Newfound! and/Labrador
Ohio
11 1 i noi s
Pennsylvania
Indiana
Kentucky
Michigan
Tennessee
Missouri
West Virginia
New York
Alabama
Wisconsin/Iowa
Minnesota
Virginia/North Carolina
Fl ori da
Georgia/South Carolina
Maryland/Delaware/New Jersey/District of Columbia
Arkansas/Louisiana/Mississippi
Massachusetts/Connecticut/Rhode Is! and
Maine
Vermont/New Hampshire
Nebraska/North Dakota/South Dakota/
Montana/Wyoming
Oklahoma/Kansas/Colorado/New Mexico/Texas
(106 kg yr'1)
505.0
17.9
183.9
689.1
667.6
51.5
454.6
539.6
79.3
191.5
169.9
59.5
2778 .9
1557.4
1973.4
1225.2
1085.5
1059.7
1075.4
1107 .6
946.6
1007 .4
655.2
907.6
279.8
875.9
728.2
919.1
760.5
617.6
575.2
82.3
86.9

581.3
1698.1
                             17

-------
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                              '

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O JANUARY, JULY. AND

   ANNUAL

e JULY AND ANNUAL




• JANUARY AND JULY




A JULY




T JANUARY
                         (B)
Figure  5.  The location of  the sulfur wet  deposition sites (A) and

           the ambient SOj  monitoring sites (B) included  in Table 3,
                            18

-------
      Table 3 presents calculations from two different ENAMAP-1 applications;
 each application used a different value for the puff truncation (i.e.,  the
 deletion of a puff of pollution when the masses of S02 and SO^ both fall
 below user-specified values).  The first application used a value of 1Q-2
 kton; the results of this application were transmitted to the work group.
 Later, the sensitivity study showed that this puff truncation value ignored
 small sources of S02«  Therefore, in the subsequent application,  a truncation
 value of 10~4 kton was used.  A significant increase in the computation
 time resulted.  The two sets of ENAMAP-1 results in Table 3, therefore,
 provide an assessment of the role of the minor sources of S02 on  sulfur wet
 depositions and ambient SO^ concentrations in the U.S. and Canada.
TABLE 3.  MODELED AND MEASURED MONTHLY TOTAL SULFUR  WET  DEPOSITIONS  AND
          MONTHLY AVERAGE AMBIENT S07 CONCENTRATIONS USING  TWO  DIFFERENT
          PUFF TRUNCATION VALUES (lO'2 AND  lO'4 KTON)

Site                             Total  sulfur wet deposition  (kg ha~l)
                                  January 1978                July 1978

Shelburne, NS
Peterborough, ON
Simcoe, ON
Sept Isles, PQ
Maniwaki , PQ
Atikokan, ON
Charlo, NB
Chibougamau, PQ
Ithaca, NY
State College, PA
Charlottesville, VA
Model
10-2
0.03
0.54
2.97
0.18
0.42






ed
0.10
0.69
3.23
0.28
0.68






Observed
0.40
0.60
2.80
0.20
0.20






Model
10-2
0.08
0.79
1.20
0.06
0.58
0.01
0.18
0.19
1.78
1.55
0.69
ed
10-4
0.15
1.05
1.43
0.19
0.86
0.12
0.40
0.21
2.25
1.92
0.96
Observed
0.10
1.70
1.20
1.00
1.20
0.40
1.00
1.00
1.60
2.40
1.60
Average                     0.83   1.00     0.84          0.65  0.87     1.20
                                     19

-------
                            TABLE 3.   (CONTINUED)
Site
Average ambient SO^ concentration Uig nr3)
January 1978                 July 1978

Montague, MA
Scranton, PA
Indian River, DE
Duncan Falls, OH
Rockport, IN
Giles Co., TN
Fort Wayne, IN
Chapel Hill , NC
Lewisburg, WV
Beverly, MA
Fall River, MA
Albany, NY
Oswego, NY
Dunkirk, NY
Roseton, NY
Warren, PA
Louisville, PA
Brush Valley, PA
Wilmington, DE
Madison, KY
Louisa, KY
Sullivan, IN
Detroit, MI
Port Huron, MI
Springfield, IL
Braidwood, IL
Columbus, OH
Conneaut, PA
Toronto, ON
Huntington, NY
Loves Mill, TN
Hytop, AL
L-B-L, TN
Paradise, KY
Memphis, TN
St. Louis, MO
Nekoosa, WI
Ithaca, NY
Dayton, OH
Mt. Storm, VJV
Chesterfield, VA
Yorktown, VA
Model
10-2
4.2
5.4
5.9
4.2
4.8
6.4

7.4
6.3
3.4

4.0
5.1

4.7
4.4

4.8


6.9






4.4

6.0
6.3
7.0
7.0
5.4
6.6

0.4
5.5


6.4
6.3
ed
10-4
4.9
6.3
7.4
5.0
6.3
7.4

8.1
6.7
3.8

4.7
6.1

5.6
5.1

5.3


7.6






4.9

6.7
6.9
7.9
8.0
6.6
8.3

1.0
6.8


7.1
7.1
Observed
3.6
5.4
5.5
8.8
8.1
6.9

5.5
6.7
6.1

6.0 •
3.9

6.1
7.6

6.7


8.8






7.4

4.5
7.1
10.3
8.1
9.1
9.2

4.5
5.4


6.2
6.7
Model
10-2
9.3
15.2
8.7
10.3
4.4
5.6
4.6
5.7
10.1
5.8
5.1
11.7
12.4
11.0
8.9
10.9
11.6
14.6
9.6
6.5

4.5
9.1
8.4
3.0
5.2
11.1
9.6
11.1
7.4
6.5
4.9
6.4
4.5
1.7
4.2
0.8
13.8
8.8
13.2
6.6
6.4
ed
io-4
13.7
21.2
13.0
14.8
5.8
7.3
7.4
10.2
14.6
9.3
8.6
17.0
18.7
15.9
12.7
16.0
15.5
18.9
14.6
8.9

6.6
13.6
13.2
4.2
9.3
15.2
13.5
15.8
11.4
10.2
6.3
7.6
5.6
2.8
5.4
2.7
20.3
12.3
17.5
10.9
10.6
Observed
9.3
12.8
9.5
16.9
13.8
11.6
11.2
8.9
11.5
9.6
8.0
11.0
11.8
15.8
12.3
15.4
16.3
16.4
15.5
12.8

12.0
8.8
8.8
14.9
10.0
14.5
13.2
11.8
9.5
15.1
11.5
9.2
11.8
9.9
12.8
5.9
10.9
13.7
15.9
10.8
8.3
                                    20

-------
                            TABLE  3.   (CONTINUED)
Site                             Average  ambient  S0|  concentration  (;jg m~3)
                                 January  1978                 July  1978

Weatherspoon, NC
Atlanta, GA
Chester, NJ
Whiteface Mt., NY
York, PA
Kentshill , ME
Average
Mode'
10-2
7.5

5.9

5.9

5.5
led
io-4
8.4

6.6

6.6

6.3
Observed
6.9

7.0

9.4

6.8
Model
10-2
3.6
2.7
9.4
10.4
15.3
8.9
8.1
ed
io-4
7.5
3.8
14.0
16.0
20.7
14.1
11.8
Observed
6.4
9.6
12.7
7.0
11.0
7.5
11.6

     Realizing that the measured data  set was  inadequate  for  concrete
conclusions and unsure of the best method to statistically  assess model
performance, Work Group 2 decided to compute the  values of  selected  statis-
tical  parameters to assess the performance of  the models  for  January, July,
and annual  1978.  Models that were applied to  only  the  two  months were  not
evaluated for the annual period.  This model evaluation exercise was expected
to at least identify models that consistently  performed below an acceptable
level .

     Table 4 presents the values of the statistical  parameters calculated
for the ENAMAP-1 results. The residuals were determined by  substracting  the
calculated value from the observed value.  In  general,  a  model  is  said  to
overpredict the observations when the  mean residual  is  less than zero.   For
a "good" model, the correlation between the residual  and  the  calculation is
low in magnitude.  This parameter is a good measure of  a  model's ability to
correctly calculate the higher and lower observed values.

     It is difficult to state firmly that the  model  performed better for
ambient S0| concentrations than for total  sulfur  wet deposition.
Based on the correlation of the residual  and calculation, the model  performed
best for July sulfur wet deposition and January ambient S0| concentrations.
Furthermore, the values of the mean residuals  were  comparable.

                                  21

-------
    TABLE 4.   VALUES  OF  STATISTICAL PARAMETERS CALCULATED FOR THE ENAMAP-1
              RESULTS USING  THE DIFFERENT PUFF TRUNCATION VALUES (KTON )
Parameter
  Total  sulfur wet deposition (kg  h
January  1978            July 1978
10-2   10-4            10-2   io-4

Sample size
Mean of observation
Mean of calculation
Mean residual
Standard deviation
of residual
Correlation of residual
and calculation
5
0.84
0.83
0.01

0.23

-0.32


1.00
-0.16

0.31

-0.62
11
1.20
0.65
0.55

0.42

0.44


0.87
0.33

0.46

0.18
Average ambient SOf concentration (yg m )


Sampl e si ze
Mean of observation
Mean of calculation
Mean residual
Standard deviation
of residual
Correlation of residual
and calculation
January
10-2
29
6.8
5.5
1.3

1.9

0.46
1978
10-4


6.3
0.5

1.8

0.14
July
10-2
47
11.6
8.1
3.5

3.6

0.44
1978
10-4


11.8
-0.2

4.9

-0.36

     It was observed that the 10~4 kton puff truncation  value improved the
concentration calculations, but degraded the deposition  calculations.   The
mean concentration and deposition calculations  became  closer to the mean
observations, with the exception of the January depositions.  There were
significant decreases in the mean residuals for the January  and July concen-
trations and the July depositions.  The major reason for the significant
increase in the absolute value of the mean residual  for  the  January deposi-
tion was the greater overprediction of the 2.80 kg ha~l  observation.
Significant decreases also were noted in the correlations between the
residuals and the calculations for the January  concentrations and the  July
depositions.
                                   22

-------
                              SECTION  4

                       MODEL SENSITIVITY  STUDY

DESIGN

     Every numerical  simulation  model  produces  results  that  do  not  concur
exactly with observations.  These discrepancies are  due partially to  uncer-
tainties in the values of model  input  parameters (e.g., dry  deposition
rates, scavenging coefficients,  mixing heights, transformation  rates, etc.).
Atmospheric scientists cannot reach  a  consensus on a single  appropriate
value for each of these model  input  parameters, but  a consensus can be
reached on a general  range of "acceptable"  values.

     Since there are  many "acceptable" values,  the modeler  is  faced with the
problem of selecting  one value to use  in  model  applications.  The magnitude
of this problem is proportional  to the model  sensitivity, or the degree of
observed change in the model calculation  from a unit change  in  the  model
input value.  If the  model proves sensitive to  a certain model  input  para-
meter, the modeler must carefully select  the value of that  parameter. A
model sensitivity study identifies those  model  input parameters whose values
must be chosen carefully.

     In a sensitivity study, the model is applied many  times;  the value of
one of the model input parameters is changed each time, and  the resultant
changes in model output are examined.  Typically, this  involves the consump-
tion of considerable  computer time.   To minimize this expense,  this sensiti-
vity study used an abbreviated version of ENAMAP-1 and  only  3  values  of each
of the 15 model input parameters (Table  5).  Two of  the three  values  represented
the low and high values of the "acceptable" range of each  parameter,  while
the third value (base case) was the  value used in past  ENAMAP-1 applications.
                                     23

-------
TABLE 5.  MODEL INPUT PARAMETER  VALUES  CONSIDERED  IN  THE  SENSITIVITY STUDY

Parameter
code
TIME INC
WINDSPD
PRCP RT
EXPN RT
TRAN RT
MIX HT
EMISCELL
WETDS02
WETDS04
DRYDS02
DRYDS04
S02EMIS
S04EMIS
TOPS02

TOPS04

Parameter
Computational time step (h)
Wind speed (km h~l)
Precipitation rate (mm h~l)
Puff expansion rate (km^ h'1)
Transformation rate (% h~M
Mixing height (km)
Initial puff size (km)*
S02 wet deposition rate (5 mm"l)
SOzf wet deposition rate (% mm-1)
S02 dry deposition factor#
S0| deposition factor#
S02 emission rate (kton h~l)
S0| emission rate (kton h"l)
S02 loss rate from mixed layer
top (kton h"1)
SO 4 loss rate from mixed layer
top (kton h-1)
Case
1
1.0
8.1
0.05
29.0
0.50
1.00
60.0
10.0
1.0
0.67
0.167
0.29
0.018

0.005

0.005
Base
case
3.0
24.2
0.10
36.0
1.00
1.45
70.0
28.0
7.0
1.00
1.000
0.36
0.000

0.000

0.000
Case
2
2.0
40.3
0.15
42.0
1.50
1.90
80.0
46.0
13.0
2.22
1.830
0.43
0.036

0.010

0.010

* The initial area of each puff is defined as  the  area  of a square  of
  sides EMISCELL.
# The land-use, stability-dependent dry deposition rates  are multiplied
  by these factors.

     The abbreviated version of ENAMAP-1 considered 1)  only one  emission
source, which emitted puffs of S02 and S0| at  12-h increments,  2)  a continuous
1.0 mm h~l precipitation rate, and 3)  a uniform transport wind  from
the southwest.  All  other parameterizations were preserved, with the
exception of the S02 and S0$ dry depositions,  which reflected the  parameteri-
zation used in a version of ENAMAP-1 currently under development.   This
parameterization is based on atmospheric stability and  land-use  charac-
teristics.

     Since the dry deposition rates depended on land-use  type,  a geographical
region of North America had to be chosen.  The region between southern Ohio
and eastern Quebec was selected (Figure 6).  The Adirondacks sensitive area
is located in the middle of this region, 700 km from the  source.
                                     24

-------
Figure 6.   The 1500-km track used for transport of pollutant
           puffs from southern Ohio in the ENAMAP-1 sensitivity
           study.
                          25

-------
     Wet and dry  deposition   and  ambient  concentrations  of 862  and  $64 were
determined for the  70-km grid square  containing the  source as well  as
those up to 1800  km downwind of the source.   Only  the wet depositions and
ambient concentrations are discussed  below,  however. The distance  from  the
center of the grid  square containing  the  source and  the  center  of the
receptor square immediately  downwind  was  99  km.   For simplicity, the following
discussions assume  a distance of  100  km.

RESULTS

Single Parameter  Variations

     The first parameter examined was TIME INC, the  frequency  of the deposi-
tion and concentration calculations.   The model calculates  the  mass of
pollutants removed  from each puff, the volume of  each  puff,  and the concen-
trations within each puff every TIME  INC  hours.   On  one  hand,  this  value
should be small enough so that depositions and concentrations  within the
grid squares downwind of the source(s) are not underestimated  due  to trans-
port of the puffs over the squares before depositions and  concentrations
within these squares are determined.   On  the other hand, smaller values
entail more frequent calculations of  depositions  and concentrations, and
hence more computer time and expense.

     The actual value for this parameter  should be chosen  on the  basis  of
the maximum expected wind speed.   A higher transport wind  speed necessitates
a lower TIME INC value, to insure a smooth distribution  of depositions  and
concentrations along the puff transport path.  As an example,  if  the transport
wind speed is 40 km h~l and TIME   INC  is 3 h, the  center  of the puff is
transported 120 km across the 70-km receptor grid network  before  the deposi-
tion and concentration calculations are performed.  As a result,  the model
calculates depositions and concentrations in the receptor cell  along the
puff transport path and between the source and the current location of the
puff center that are much lower than  those in the receptor cell containing
the puff center.
                                     26

-------
     Figure 7 illustrates the $04 concentrations  (ug  nr3)  at  equally
spaced distances from the source for three  different  wind  speeds  (8.1,  24.2,
and 40.3 km h'1) for a TIME INC of 3, 2,  and  1  h.   All  remaining  parameters
were assigned their base case values.  With TIME  INC  equal  to 3 h (as  in
previous ENAMAP-1 applications), the concentration  curve was  rather smooth
for the low wind speed, erratic for the moderate wind speed,  and  very
erratic for the high wind speed.  In the  case of  the  high  wind speed,  the
concentrations downwind of the source periodically  approached zero, since
the puffs were transported across some of the receptor cells  before the
calculations were performed.

     When the value of TIME INC was lowered to  2  h, the concentration  curve
for the moderate wind speed case became smooth, but the curve for the  high
wind speed case was periodically erratic.  An improvement  in  the  concentra-
tion curve for the high wind speed was noted, however.  Instead of periodic
occurrences of declines to near zero (as  with TIME  INC 3h) there  were  peaks
in the concentration curve.  This could be a  result of the puff center
remaining in the same receptor cell for two consecutive calculation time
steps.

     When TIME  INC was decreased to 1 h,  the  concentration curves for  the
lowest two wind speeds were unchanged.  The amplitude of the  perturbations
in the concentration curve for the high wind  speed  decreased, however; the
curve became more saw-toothed.  The fact that the concentration curve  was '
not smooth even for the 1-h calculation time  step does not present a  serious
problem, since wind speeds of 40 km h~l occur infrequently.

     As a result of this investigation, it was decided that a TIME INC value
of 2 h would be used in the remainder of the  sensitivity study.   Except for
the low wind speed case, the 2-h calculation  time step yielded a  significant
improvement in  the concentration curves over  those resulting  from the  3-h
step.  The curves resulting from the 1-h step were not significantly  better
than those resulting from the 2-h step, therefore,  the added  expense  of
doubling the number of computations was not justified.
                                    27

-------
35.0
17.5
0.0  J
Figure 7.
 The 96-h average ambient SO? concentrations (yg m  )
 at specific distances upwind and downwind of a single      ,
 source.  Wind speed = 8.1 (+), 24.2 M, and 40.3 (*) km h"1,
 TIME INC = 3 (plot A), 2 (plot B), and 1 (plot C) h.
                28

-------
     Figures 8a through 8n illustrate the S02 and  S0|  wet depositions  and
concentrations as a function of distance from the  source  and  one  of  the
model input parameters.  The order of appearance of  the model  input  para-
meters in this series of figures matches that of Table 5.

     Figure 8a illustrates the four sets of curves resulting  from the  three
different wind speed values .  The periodic perturbations  noted earlier in
the S0$ concentration curve at the high wind speed also appeared  in  the
curves for S02 concentration and S02 and S0| wet depositions.  The location
of the peaks in the concentrations was clearly a function of  wind speed.  At
the low wind speed, the magnitude of the peak deposition  and  concentrations
near the source greatly increased, especially for
     Changes in model  output due to changing the precipitation  rate are
illustrated in Figure 8b .  These changes appeared to be linear  for the
concentrations, but not for the depositions.  The increase in wet deposition
per 0.50 mm h-1 increase in the precipitation rate appeared to  lessen.
The amount of S0| wet deposited 500 km from the source increased 65%
when the precipitation rate was doubled, but the amount wet deposited over
the same receptor cell doubled when the precipitation rate was  tripled.  As
the precipitation rate increased, more S02 and S0| was deposited closer
to the source, which left less S02 in the puff to transform to  S0| and less
S0| to be transported downwind.  The wet deposition of S02 and  S0| in a
constant light rain scenario dropped significantly beyond 500 km.

     Regarding $02 and S0| concentrations, the location of the  peak of
the former was not a function of the precipitation rate, while  that of the
latter was.  The peak S0z[ concentration occurred closer to the  source
as the precipitation rate increased (800 km from the source for 0.05 mm
h~l, 600 km for 0.10 mm h"1, and 400 km for 0.15 mm h-1) .

     Figure 8c illustrates the changes in model output when the puff expansion
rate was decreased and increased by 20% of the base' case value  of 36.0 km^ h"1
Very little change was noted in the deposition and concentration curves.
                                    29

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     Figure 8d  illustrates  the  changes  in model output when the transforma-
tion rate of S02 to  S0|. was decreased and increased by 50% of  its
base case value of 1.0% h~l.  For S0| wet deposition  and concentration,
the difference  between  the  base case and high  transformation rate case was
slightly less than that between the base case  and  the low transformation
case.  However, the  $62 wet deposition  and  concentration exhibited  less of
a difference, percentage wise.   The downwind location of neither the maximum
S0| concentration nor the maximum S0| wet deposition  was a function of
the transformation rate.

     Changes in model  output as a result of changing  the mixing height are
illustrated in  Figure 8e.  Increasing the mixing height  increased the
volume, but not the  mass, of the puff.  Since  depositions were not  a function
of puff volume, no changes  in the depositions  were observed.   The concentra-
tions, naturally, decreased proportionally  with  increased in mixing height.
A twofold increase in mixing height yielded a  twofold decrease in concentra-
tions.

     Changes in model  output as a result of a  10-km decrease and increase in
the value of EMISCELL are illustrated in Figure  8f.   The value of this model
input parameter determined  the  initial  cross-sectional area of the  puff,
which was equal to the area of a square of  sides EMISCELL.  Increases in
EMISCELL caused slight linear decreases in  the depositions and concentrations

     Figure 8g illustrates  the changes  in model  output as the  S02 wet
deposition rate was  decreased and increased by approximately 65% of the base
case value of 28.0%  mm"1.  As one would expect,  the S02  and S0| depositions
and concentrations decreased as the  rate increased.   Once again, the changes
in model output as the input parameter  value  increased from the base case
value were smaller than those resulting form an  equal decrease in the input
value.
                                    33

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                                 37
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     The effects of changing the 504  wet deposition  rate  by  approximately
90% of its 7.0% mnrl base case value  are illustrated in Figure  8h.   Naturally,
the changes in this model  input parameter did not affect  the $03  concentrations
and depositions.  For the lowest wet  deposition  rate,  the amount  of S0|
deposited in each receptor cell  downwind of the  source was small  and nearly
uniform.  In this case, the decreasing 504 concentrations downwind  of the
location of the concentration peak were due primarily  to  the dispersion  and
dry deposition.  The more this input  parameter value increased, the more
the~ampl itude of the peak increased in the wet deposition curve.   The peak
did not shift further downwind as the wet deposition rate increased, however.

     Figures 8i and 8j illustrate the changes in model output resulting
from changing the S02 and SO^ dry deposition factors,  respectively.  The
dry deposition rates assigned to each receptor cell, according  to the
defined predominant land-use type within the cell, were  multiplied by the
respective factor.  Typical dry deposition rates of S02  and 504 across
the chosen geographical region were about 0.5 and 0.9 cm s-1, respectively.

     Since the factors equaled 1.0 in the base case, the  dry deposition
rates currently used in ENAMAP-1 were designated as the  base case.   The
lowest value of the S02 dry deposition factor is much closer to the base
case value of 1.0 than is the higher value, since the S02 dry deposition
rates used in ENAMAP-1 are closer to the lower end of the range of rates
reported  in the literature.

     For  the highest value of the S02 dry deposition  factor  (2.22 times the
base case), the S02 and SQ^ wet depositions and concentrations decreased
only slightly  (up  to 10%) within 400 km of the source, but decreased to a
greater extent  (up  to  20%) beyond this distance.  Such was not the case for
the $04 dry deposition factor.  Of course, this model input  parameter had
no bearing on  S02  depositions and concentrations, but the changes  in the
504 wet  depositions  and concentrations within 400 km  of  the  source, after
the SO^  dry deposition factor was raised  to  1.80, were greater,  percen-
                                   38
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            41
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tage wise,  than those observed  after  the  factor was  raised to 2.22.  The
504 wet depositions  and concentrations  1500  km downwind of the source
decreased by about 40% when  the factor  was increased from 0.167 to 1.83.
The effect was less  dramatic closer to  the source  (30% at 500 km), but
still substantial.

     Figures 8k and  81  illustrate  the effects of changing the SOg and SO^
emission rates.  Since ENAMAP-1 assumes only linear  chemistry, it was no
surprise that the S02 and 504 wet  depositions and  concentrations increased
linearly, at respective receptor cells, with increasing S02  and $04
emission rates.

     The greatest changes occurred in the 504 wet  depositions and concen-
trations near the source when the  $04 emission  rate  was increased.
Increasing the emission rate from  0.00  to 0.036 kton h-1 increased the
$04 concentration across the source cell  from nearly 0 to approximately
10 ug m-3.  Meanwhile, across the  adjacent downwind  receptor cell, the
$04 concentrations increased almost  threefold from approximately 11  to
approximately 28 ug  nr3.  This  illustrates the  importance of considering
primary emissions of 504 in sulfur pollution modeling.

     The last pair of figures in this series, Figures  8m and 8n,  illlustrate
the changes in model output that resulted from  changing  the  rate of  $0g  and
S0| mass transfer to the layer above  the  mixed  layer,  respectively.
Since little is known about the vertical  flux of  pollutants  from the mixed
layer, the values of these model input  parameters  were arbitrarily  chosen
to be 0.005 and 0.010 kton h~l.  Changes  in these  parameters caused linear
changes  in the wet depositions and concentrations.  At 1500  km  from the
source,  increasing the S02 or S0| loss  rate from  0.005 to  0.010  kton h"1
resulted in a 25% decrease in 504 wet depositions  and concentrations.  At
500  km,  only a 10% difference was observed.

     To  summarize the preceding discussion, Figure 9 presents plots of the
changes  in wet sulfur depositions resulting from unit increases  in the model
                                   42
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                             47
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input parameters as a function  of  distance  downwind  from the  source.  When
interpreting these plots,  one  should  bear in  mind  that  they were  generated
assuming

     1)  the ranges of parameter values  listed in Table  5,  and
     2)  that, at each receptor  cell  downwind  of the  source, the wet  sulfur
        depositions changed linearly  with changes  in the  input parameter
        values.

Table 6 lists the maximum  observed changes  in wet  sulfur  depositions  for
unit increases in 14 of the 15  model  input  parameters considered  in  this
sensitivity analysis.
TABLE 6.  MAXIMUM CHANGES IN WET SULFUR DEPOSITION FOR UNIT
          INCREASES IN MODEL INPUT PARAMETERS
Model input   Parameter   Maximum change (mg m~2)  per unit   Distance downwind
Parameter*      Units     increase in the parameter              of source (km)
WINDSPD
PRCP RT
EXPN RT
TRAN RT
MIX HT
EMISCELL
WETDS02
WETDS04
DRYDS02
DRYDS04
S02EMIS
S04EMIS
TOPS02
TOPS04
km h-1
mm h"1
km2 h'1
% h-1
km
km2
% nun"-'-
% mm"1
-
_
kton h'1
kton h'1
kton h'1
kton h'1
-15.7
2400 .0
0.9
-17.4
0.0
0.6
8.4
1.1
-20.0
2.6
785.0
149.0
-2420 .0
-1770.0
100
100
200
400
1 —
400
100
400, 500
400
1500
100
100
400
1300, 1400

* Parameter codes are defined in Table 5.

Multiple Parameter Variations

     This subsection addresses the sensitivity of the model to changes in
the values of a set of model input parameters.

                                     48
-------
     The abbreviated version of ENAMAP-1  was  applied  two more  times  to
compare the calculated wet depositions  and  concentrations  of S02  and
$05 at 100-km increments downwind of the  source  using the  extreme values
of many of the input parameters.  These values are  defined in  Table  7.
The first application used values that  would  individually  contribute to
minimal wet deposition downwind of the  source, while  the second application
used values that would individually contribute to maximum  wet  deposition.
Base case values of the wind speed (24.2  km h"1), precipitation rate (0.1
mm h~l), mixing height (1.45 km), and S02 and S0| emission rates  (0.36
and 0.00 kton h"l, respectively) were used  in each  of these applications,
however.
     TABLE 7.  EXTREME VALUES USED IN TWO APPLICATIONS
               TO PRODUCE MINIMUM AND MAXIMUM SULFUR WET
               DEPOSITION WITHIN 500 KM OF THE SOURCE*

Parameter
code#
EXPN RT
TRAN RT
EMISCELL
WETDS02
WETDS04
DRYS02
DRTS04
TOPS02
TOPS04
Value contributing
to minimum
42.0
0.015
80.0
0.10
0.01
2.22
1.830
0.01
0.01
Value contributing
to maximum
29.0
0.005
60.0
0.46
0.13
0.67
0.167
0.00
0.00

* Base case values were used for emissions and meteorological
  parameters.
# Parameter codes and units are defined in Table 5.
     The resulting sets of model  output serve as an estimate of the  range  of
the model uncertainty.  Figure 10 presents the wet depositions  and concentra-
tions of S02 and S0| as functions of these two sets of model  input parameter
values and downwind distance from the source.  Model  results for the entire
base case set of values are plotted as a reference.  The base case plots
represent the values of input parameters used in previous ENAMAP-1 applica-
tions .
                                  49
-------
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     The greatest variation was observed in $03  wet deposition  100  km
downwind of the source.   At this distance,  the values ranged from about
150 to about 950 mg m-2} w-jth the base case value exactly  in between.
As the distance from the source increased,  the high case S02 wet depo-
sitions approached that  of the base case,  since, for the former, less
S02 remained suspended in the air further downwind.

     There was a significant difference between  SO^ deposition  for  the
low case and for the high case.  The difference  peaked at a distance of
400 km from the source,  where the low case produced about 4 mg-2 while
the high and base cases  produced about 25 mg m-2.  Even at a distance
of 1500 km from the source, where S0| wet deposition was identical  in
the high and base cases  (15 mg m"2), SO^ wet deposition in the  low
case was about 2 mg m~2.  The higher dry deposition rates, the  lower
wet deposition rates, and the higher loss rates  used in the low case
were responsible for these differences.  Regarding total sulfur wet
deposition, both the magnitude and the variations of SOg wet deposi-
tions were much more significant.

     The variations in S02 concentration seemed  less significant that
those in wet deposition.  The greatest variation occurred 100 km down-
wind of the source, where the concentrations ranged from about 110  to
150  yg m-3.  The base case concentration, about 140 yg nr3, was
much closer to that of the high case.  Beyond 400 km, the base case
concentration slightly exceeded those of the other two cases.

     The variations in SO^ concentration were more significant than
those in S02 concentration.  The variations peaked in magnitude at
400 km from the source.   The concentrations at this distance ranged
from about 13 to about 24 ug m-3: the maximum was nearly twice the
minimum.  Beyond 500 km, the base case concentration surpassed those
of the other two cases.   At 1500 km, the base case concentration was
15 ug m-3; the other two concentrations were about 9 yg nr3.
                                    51
-------
     That the base case 864 concentration exceeded those of the other
two cases beyond 500 km was somewhat surprising,  since 1)  the other two
cases employed extreme values of the model  input  parameters, and 2) the
S02 and SO^ depositions and the S02 concentrations for the base case and
the high case were very similar beyond 500 km.  The differences in SO^
concentration resulted directly from the following conditions: 1) the
transformation rate for the base case was double  that in the high case,
2) the S02 wet deposition rate for the base case  was lower, enabling
more S02 to transform to 504.  The differences  occurred in spite of the
facts that 1) the puffs in the base case expanded at a faster rate, and
2) both the S02 and SO^ wet depositions for the two cases were nearly
identical, the 504 wet deposition rate was not  a  significant factor in
the differences in 504 concentration.

This set of model results appeared to reinforce a previously stated
conclusion: that ENAMAP-1 appears most sensitive  to the S02 wet deposi-
tion rate.  Therefore, further model improvements should focus on the
S02 wet deposition parameterization.
                                  52
-------
                               SECTION 5

                        SUMMARY AND CONCLUSIONS

     In support of Work Group 2 of the U.S./Canadian Memorandum of
Intent on Transboundary Air Pollution, ENAMAP-1 was applied 1)  to
generate January and July 1978 unit transfer matrices for eastern
North America, and 2) to evaluate model-calculated sulfur wet deposi-
tions and $04 concentrations using measured data for January and
July 1978.  Furthermore, a shortened version of the model  was applied
to study the sensitivity of the model  output to the values of the
model input parameters, as requested by Work Group 2.

     The ENAMAP-1 unit transfer matrices defined the source/receptor
relationships for 35 source regions, each emitting 1.0 Tg sulfur per
year, and 44 receptor regions comprised of the same 35 source regions
plus 9 sensitive areas.  From these January and July 1978 unit transfer
matrices, estimates of the 1978 annual transfer matrices were generated.
Unfortunately, the calculated matrix element values could not be evalu-
ated, since the actual contributions of one region to another were
unknown.

     The unit transfer matrices indicated that the sources within a
region contributed significantly to the sulfur depositions and concen-
trations in that region.  Of the total mass of S02 wet deposition in
any  region, 68 and 64% of the S02 was emitted from sources within the
region itself-for January and July 1978, respectively.  Since the
model results showed that much more S02 than $04 was deposited by
precipitation, the transfer matrices indicated that local sources
impact very significantly on sulfur wet deposition in a given region.

                                  53
-------
     Although the extensive evaluation  data  set was  not available, a
model  evaluation study was conducted  using screened  data available for
January and July 1978.  "Hie screening process  left only 5 and 11 sulfur
wet deposition measurements for January and  July, respectively, and
29 and 47 ambient SOJj concentration measurements for January and July,
respectively.  Many of the sulfur  wet deposition measurement sites
were located in Canada, while many of the  ambient S0| monitoring sites
were located in the U.S.

     Any conclusions drawn from such  a  small evaluation data set appli-
cable to only two 1-month periods  would not  likely apply to much longer
periods.  However, for this evaluation  data  set, the model (using the
10~4 kton puff truncation value) performed rather well.  The ENAMAP-1
January mean sulfur wet deposition was  slightly greater than the monthly
mean of the measurements at the five  sites;  the ENAMAP-1 July mean was
slightly less than the mean measurement.   The  mean ambient S0|
concentrations calculated by the model  (6.3  and 11.8 ug m~3 for
January and July, respectively) compared very  favorably with the mean
measurements (6.8 and 11.6 ug m~3  for January  and July, respectively).
The mean residuals for both January and July were less than 1.0 ug
m~3.  Except for the case of sulfur wet deposition in January, the
absolute values of the correlation between the residuals and the model
calculations were less than 0.40,  indicating that the model performed
well for the two 1-month periods.

     The model sensitivity study assessed  the  changes in the model output
at 100-km increments downwind of a single  source due to changes in the
values of one of the model input parameters.  Some significant conclu-
sions of this study were:

     1) The 3-h time step used in  previous ENAMAP-1  applications led
        to a saw-toothed distribution in the model output for moderate
        and high wind speeds (>20  km  h"1).
-------
2) A 2-h time step led to a saw-toothed distribution  in  the  model
   output for only the high wind speed (>35  km h~M.

3) A 1-h time step did not remove the saw-toohed distribution  in
   the model  output for the high wind speed,  but it did  reduce
   the amplitude of the fluctuations.

4) Within 700 km of the source,  S02 wet deposition  was sensi-
   tive to the S02 wet deposition rate; at a  distance of 100 km
   from the source, S02 wet deposition increased from about
   200 to about 800 mg nr2 as a  result in an  increase in the
   S02 wet deposition rate of from 0.10 to 0.46% mm"*.

5) Beyond 200 km of the source,  SO^ wet deposition  was sensi-
   tive to the S02 wet deposition rate; at a  distance of 1500
   km from the source, SO^ wet deposition decreased from about
   25 to about 10 mg m~2 for the same increase in the S02 wet
   deposition rate.

6) Beyond 100 and 300 km the ambient concentrations of S02 and
   $04, respectively, were sensitive to the S02 deposition rate.

7) The changes in the S02 dry deposition rate (from 67 to 220%
   of the base case value) did not affect wet deposition and con-
   centrations nearly as much as did the S0£ and $04  wet de-
   position rates.

8) Changing the SO^ dry deposition rate (from 16.7  to 183.0%
   of the base case value) affected the 504 concentrations and
   wet depositions much as did changing the S02 wet deposition
   rate.

9) The consideration of a small  $04 emission rate,  18 t  h~*
   or 5% of the base case S02 emission rate, resulted in signi-
   ficant increases in 504 concentrations and wet deposition;
   at 200 km from the source, deposition and concentration
   increased 35 and 48%, respectively.

                             55
-------
     The model  sensitivity study  also assessed changes  in  model  out-
put at 100-km increments downwind of a single  source  due to  changes  in
all the model  input parameters  except those relating  to meteorological
and emission scenarios.   Three  cases were considered:  a case case con-
sisting of values used in previous ENAMAP-1 applications,  a  set of values
that tended to maximize  sulfur  wet deposition, and a  set that tended
to minimize deposition.

     This assessment showed that  the SO^ wet depositions and $62
concentrations calculated using the base case  values  were  very similar
to those calculated using the high case values.  Furthermore, the S0|
concentrations beyond 500 km of the source calculated for  the base
case were greater than those calculated for the other two  cases.
                                   56
-------
                               REFERENCES
Bhumralkar,  C.  M.; R.  L.  Mancuso;  D.  E.  Wolff;  R.  A.  Thill ier;  K.  C.
Mitz; and W. B. Johnson (1980).  ENAMAP-1 Long-Term Air Pollution Model:
Adaptation and  Application to Eastern North America.  U.S.  Environmental
Protection Agency, EPA-600/4-80-039,  93  p.

Johnson, W.  B.; D. E.  Wolff; and R.  L. Mancuso  (1978). Long-Term Regional
Patterns and Transfrontier Exchanges of Airborne Sulfur Pollution in
Europe. Atmos.  Environ.,  12, pp. 51-527.

McMahon. T.  A.; P  J.  Denison; and R. Fleming (1976). A Long-Distance
Air Pollution Transportation Model Incorporating Washout and Dry
Deposition Components.  Atmos. Environ., 10, pp. 751-761.

McNaugton, D. J. (1980).   Initial  Comparison of SURE/MAP3S Sulfur
Oxide Observations with Long-Term Regional  Model Predictions. Atmos.
Environ., 14, pp. 55-63.

Ottar, B. (1978). The OECD Study on Long-Range  Transport of Air Pollutants
(LRTAP). Proceedings of the International Symposium on Sulfur in the
Atmosphere, 7-14 Sept., 1977, Dubrovnik, Yugoslavia.  Atmos. Environ.,
12, pp. 445-454.

Peck, E. L.  (1982).  Precipitation Data Analyses for Evaluation of Air
Quality Simulation Models.  Hydex Corporation.  Final  Report. University
of Illinois Subcontract No. 81-139.

Rao, K. S.; T.  Thomson; and B. A. Egan (1976).  Regional Transport Model
of Atmospheric Sulfate. Paper No. 76-34.3.  69th Annual Meeting of the
Air Pollution Control  Association, June 1976, Portland, Oregon.

Renne, D. S. and D. L. Elliot (1976). Regional  Air Quality Assessment
for Northwest Energy Scenarios. Paper No. 76-23.5. 69th Annual  Meeting
of the Air Pollution Control Association, June  1976,  Portland,  Oregon.

Scott, B. C. (1978). Parameterization of Sulfur Removal by Precipitation.
J. Appl. Meteor., 17_, p.p. 1375-1389.

Shieh, C. M.; M. L. Wesely, and B. B. Hicks (1979). Estimated Dry Depo-
sition Velocities of Sulfur over  the Eastern United States and Surrounding
Regions. Atmos.  Environ., 13, pp. 1361-1368.

U.S./Canadian Regional Modeling Subgroup Final  Report. In print.

U.S./Canadian Work Group 2 Final  Report.  In print.

Weber, E. (1971).  Removal of Sulfur Dioxide from the Atmosphere. Report
No. 5, Chapter XII, Proceedings of the Second Meeting, NATO/CCMS Panel
on Modeling, July 1971, Paris,  France.

                                     57
-------
                                   APPENDIX A


        44 BY  44 UNIT TRANSFER MATRICES FOR JANUARY AND JULY 1978


      The following  transfer matrices show  the effects of 1.0 Tg yr-1

sulfur emissions from 44 emission  regions  (35 of  the 40  Work Group 2
regions plus  the 9  Work Group 2 sensitive  receptors) on  the monthly wet
and  dry depositions and ambient concentrations of S02 and S0|  across
the  same regions (see Figure 4).   The units of the deposition  matrix
elements are  mg nr2(Tg S yr"1)-1;  those of the concentration matrix
elements are  mg m~3(Tg S yr*1)-1.   To convert the deposition units to

kg ha -1(Tg  S yr-1)'1, the  values  must be  divided by 100.


      The 44  source/receptor regions in these matrices are defined as
follows:
        Number
State/Province
1
2
3
4
5
6
7
8
9
10
11
12
13
14
IS
16
17
Ohio
Illinois
Pennsylvania
Indiana
Kentucky
Michigan
Tennessee
Missouri
West Virginia
New York
Alabama
Wisconsin, Iowa
Minnesota
Virginia, North
Northern Florid
Georgia, South i
Maryland, D.C.
                 Delaware,  New Jersey
         18       Louisiana, Arkansas
                 Mississippi
         19       Connecticut, Rhode Island
                 Massachusetts
         20       Maine
         21       New Hampshire, Vermont
         22       Nebraska,  South Dakota,
                 North Dakota
Number   State/Province

  23     Texas, Oklahoma
        Kansas, Eastern Colorado
  24     Southern Manitoba,
        Southern Saskatchewan
  25     Western Ontario
  26     Central Ontario
  27     Sudbury, Ontario
  28     Southern Quebec
  29     Eastern Ontario
  30     Southern Quebec
  31     Central Quebec
  32     Eastern Quebec
  33     New Brunswick
  34     Southern Nova Scotia,
        Prince Edward Island
  35     Labrador
  36     Boundary Water, Ontario*
  37     Algoma, Ontario*
  38     Muskoka, Ontario*
  39     Laurentian Mountains,
          Quebec*
  40     Southern Nova Scotia*
  41     Northern New Hampshire*
  42     Adirondack Mountains*
  43     Central Pennsylvania*
  44     Great Smoky Mountains*
        * The 9 sensitive receptors  were also considered as sources.
                                      58
-------
Wet Deposition Unit Transfer Matrix
         January 1978
            59
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SO, Wet Deposition Unit Transfer Matrix
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                 74
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JANUARY 1978
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                79
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~ 	 JANUARY 1978
TOTAL CONTRIBUTIONS TO iO<« DRY DEPOSITION MtRMS/M2 WITHIN RECEPTOR REGIONS
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SCL Ambient Concentration Unit Transfer Matrix
               January 1978
                  84
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JANUARY 1978
TOTAL CONTRIBUTIONS TO 5,04 CONCENTRATION U6RMS/M3 U1TH1N RECEPTOR REGIONS
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TOTAL CJNTRIBUT10NS TO S04 CONCtNTR ATiON UGRMS/H.1
TIER 25 "26 27 2B 2>
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00
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                                                           118
-------
                               APPENDIX B

      UNIT TRANSFER MATRICES FOR 11  CONSOLIDATED  EMISSION REGIONS
       AND 9 SENSITIVE RECEPTOR REGIONS FOR JANUARY  AND JULY  1978

     The large unit transfer matrices (Appendix A) were condensed  by
consolidating 35 emission regions (ignoring the emissions from the sen-
sitive receptors) into 11 regions (Figure  B-l).  The emission rate for
each of these 11 regions was normalized to 1.0 Tg S  yr~l.  The resulting
transfer matrices, presented in this appendix, show  the effects of sulfur
emissions from each of the 11 regions on the wet  and dry depositions  of
sulfur and ambient concentrations of S02 and SOjj  across the 9 sensi-
tive receptor areas.  The units of the sulfur wet and dry depositions
are kg S ha-*(Tg S yr ~1)~1; those of the  concentrations are  mg m~3
(Tg S yr-l)-l.

     The location of the 9 sensitive receptor areas  are indicated  in
Figure 3.  The abbreviations used in this  appendix are:

         Abbreviation              Sensitive Receptor Area
             BW                    Boundary Waters
             ALG                   Algoma, Ontario
             MUS                   Muskoka, Ontario
             QUE                   Laurentian Mountains, Quebec
             SNS                   Southern Nova  Scotia
             NH                    Northern New Hampshire
             ADIR                  Adirondack Mountains
             PENN                  Central Pennsylvania
             SMOK                  Great Smoky Mountains National  Park
                                 119
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          120
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JANUARY 1978
EMISS
REG


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JULY  1978
EMISS
REG

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1
2
3
4
5
6
7
8
9
10
11
1
2
3
4
5
6
7
8
9
10
11
1
2
3
4
5
6
7
8
9
10
11
1
2
3
4
5
6
7
8
9
10
11
BW
.000
,000
.164
.000
.000
.000
.000
.000
.000
.044
.000
.000
.000
.312
.000
.000
.000
.000
.000
.000
.170
.002
.000
.000
1.504
.000
.000
.000
.000
.000
.000
.797
.008
.000
.000
.620
.000
,000
.000
.000
.000
.006
.410
.023
ALG
.000
.009
.068
.000
.000
.000
.000
.000
.005
.018
.000
.000
.009
.056
.000
.000
.000
.000
.000
.013
.028
.000
.000
.035
.223
.000
.000
.000
.000
.000
.022
.096
.000
.000
.103
.480
.000
.000
.002
.000
.000
.326
.350
.003
MUS
.000
.007
.286
.000
.001
.016
.000
.001
.022
.065
.000
.000
.036
.826
.000
.001
.025
.000
.000
.028
.129
.000
.000
.125
3.723
.000
.005
.084
.000
.000
.054
.523
.000
.000
.446
3.282
.000
.011
.339
.000
.005
.677
.999
.002
QUE
.003
.245
.089
.000
.006
.003
.000
.000
.009
.030
.000
.001
.596
.090
.000
.013
.005
.000
.000
,007
.016
.000
.003
2.760
.229
.000
.054
.007
.000
.000
.004
.026
.000
.023
1.809
1.781
.000
.100
.157
.000
.000
.242
.418
.000
SNS
.086
.002
.002
.000
.078
.015
.008
.000
.001
.001
.000
.532
.015
.005
.000
.405
.030
.085
.001
.003
.002
.000
2.493
.026
.003
.000
1.640
.040
.266
.000
.001
.000
.000
1.067
.355
.170
.000
1,968
.753
.614
.021
.106
.069
.000
NH
.000
.067
.009
.000
.074
.114
.022
.001
.009
.003
.000
.004
.200
.026
.000
.291
.095
.015
.000
.009
.005
.000
.016
.898
.084
.000
1.364
.337
.058
.000
.008
.009
.000
.045
.801
.373
.000
.755
1.168
.121
.003
.301
.109
.000
ADIR
.000
.002
.032
.000
.069
.144
.018
.000
.014
.009
.000
.000
.327
.143
.000
.288
.161
.028
.000
.013
.028
.000
.000
1.461
.585
.000
1.352
.662
.123
.000
.020
.094
.000
.000
1.358
1.010
.000
.736
1.287
.167
.003
.371
.375
.000
PENN
.000
.000
.017
.000
.008
.314
.004
.001
.021
.013
.000
.000
.023
.048
.000
.066
1.420
.019
.004
.033
.019
.000
.000
.078
.183
.000
.277
6.767
.089
.011
.111
.062
.000
.006
.285
.474
.000
.434
2.696
.046
.092
.455
.253
.002
SMOK
.000
.000
.000
.000
.000
.006
.039
.109
.102
.000
.002
.000
.000
.000
.000
.000
.017
.123
.332
.237
.000
.002
.000
.000
.000
.000
.000
.069
.594
1.55
1.069
.001
.003
.000
.000
.000
.000
.000
.121
.188
.965
.964
.003
.041
 122
-------
                                  TECHNICAL REPORT DATA
                           (Please read Inunctions on the reverse before completing)
1. REPORT NO.
                             2.
                                                           3. RECIPIENT'S ACCES5ION>NO.
4. TITLE AND SUBTITLE
                                                          5. REPORT DATE
     SULFUR DEPOSITION MODELING IN SUPPORT OF  THE
     U.S./CANADIAN MEMORANDUM OF INTENT ON ACID RAIN
             6. PERFORMING ORGANIZATION CODE
7. AUTHORIS)

     T.L. Clark  and  D.H. Coventry
                                                           8. PERFORMING ORGANIZATION REPORT NO.
9. PERFORMING ORGANIZATION NAME AND ADDRESS
      (same as  Block 12)
             10. PROGRAM ELEMENT NO.

                CCVN1A/01-2057 (FY-83)
                                                           11. CONTRACT/GRANT NO.
12. SPONSORING AGENCY NAME AND ADDRESS
     Environmental  Sciences Research Laboratory-RTP,NC
     Office  of Research and Development
     U.S.  Environmental Protection Agency
     Research  Triangle Park, NC 27711	
                                                           13. TYPE OF REPORT AND PERIOD COVERED
             14. SPONSORING AGENCY CODE
                   EPA/600/09
15. SUPPLEMENTARY NOTES
16. ABSTRACT
     At  the  request of the U.S./Canadian  Work  Group 2 of the Acid Rain  Memorandum of
     Intent,  the Eastern North American Model  of Air Pollution (ENAMAP-1)  was  applied
     to  two  months of 1978 to simulate the  monthly wet and dry depositions and monthly
     average ambient concentrations of S02  and sulfate across eastern North America.
     Using these model  results, unit emission  (1.0 Tg S yr~') transfer  matrices were
     generated  and a model performance study was performed. In addition, a model  sen-
     sitivity study was conducted to examine the consequences of model  input parameter
     uncertainties.
     The mean calculations were within 20%  of  the mean sulfur wet depositions  and
     within  8%  of the mean ambient sulfate  concentration. The mean residuals of the
     sulfur  wet depositions were of the order  of 0.25 kg ha'T, while those for the
     monthly average ambient sulfate concentrations were of the order of 0.4 ug m~3.
     The sensitivity analysis indicated that for high wind speeds (greater than 35 km
     h"'), a  saw-toothed downwind distribution of depositions and concentrations re-
     sulted  from simulations using 2- and 3-h  time steps. In general, the  greatest
     changes  in the S02 wet depositions and ambient concentrations ocurred within 200
     km of the  source,  while those in the sulfate wet depositions and concentrations
     ocuurred beyond 300 km.
17.
                               KEY WORDS AND DOCUMENT ANALYSIS
                  DESCRIPTORS
b.lDENTIFIERS/OPEN ENDED TERMS  C. COSATI Field/Group
13. DISTRIBUTION STATEMENT


      RELEASE TO THE PUBLIC
19. SECURITY CLASS (This Report}
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-------