Estimating The Transfer and Deposition of Dioxin and

Atrazine to the Great Lakes Basin with the NOAA
HYSPLIT Model — an Overview

John F. McDonald
International Joint Commission
Regional Office
100 Ouellette Ave., 8th Floor
Windsor, Ontario N9A 6T3

Dr. Mark Cohen
Air Resources Laboratory
National Oceanic and Atmospheric Administration
1315 East West Highway, R/ARL
Silver Spring, Maryland 20910

Debra Meyer
National Exposure Research Laboratory
U.S. Environmental Protection Agency
MD-75
Research Triangle Park. North Carolina 27711

Larissa Mathewson
Provincial Geomatics Service Center
Ontario Ministry of Natural Resources
300 Water Street, 5th Floor, South Tower
Peterborough, Ontario K9J 8M5

DISCLAIMER

The authors of this paper, while acknowledging the support of their parent agencies, note that the
comments, findings and conclusions are the authors' own and not necessarily representative of
the International Joint Commission, National Oceanic and Atmospheric Administration, U.S.
Environmental Protection Agency and/or the Ontario Ministry of Natural Resources who assisted
in and supported this work.

ABSTRACT

Over the last few years, the International Joint Commission has been supporting development of
a PC based transfer model, derived from the HYSPLIT model created at the National Oceanic
and Atmospheric Administration (NOAA), to determine, in a cost effective way, the extent of

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 deposition of selected persistent toxic substances to the Great Lakes from US and Canadian
 sources and source regions. Outputs for dioxin and atrazine will be described, quantifying the
 percentage of emissions of these substances from specific point and county level sources which
 would be deposited in Lake Superior. For the sake of brevity, these data are presented as an
 example of determinations available for all the other Great Lakes. The impact of specific sources
 and source categories will be considered. The authors believe this technology will prove useful
 as a tool in developing a strategy for further control of these sources. Illustrations can be viewed
 in color at the International Joint Commission website at: www.ijc.org/boards/iaqab,

 INTRODUCTION

 In the early 1980s, Steve Eisenreich and William Strachan made one of the first estimates of the
 relative polychlorinated biphenyls (PCBs) to the Great Lakes, suggesting that approximately 90
 percent of the loading of PCBs to Lake Superior could be attributed to deposition from the
 atmosphere, with the balance of the Great Lakes receiving relatively lesser, although significant,
 amounts from this pathway. [Mass Balancing of Toxic Chemical in the Great Lakes: the Role of
 Atmospheric Deposition, William M J. Strachan and Steven J. Eisenreich, Science Advisory
 Board/Water Quality Board/International Air Quality Advisory Board- International Joint
 Commission May 1988  l]

 In their 1985 report, the Water Quality Board of the International Joint Commission developed a
 list of 11 Critical Pollutants [Table 1 ].

 TabJe 1.  Eleven Critical Pollutants as Reported in 1985  Water Quality Board Report
-[Great Lakes Water Quality Board, International Joint Commission 1985 Report on Great Lakes
 Water Quality, Windsor, Ontario June 19852]
  Total polychlorinated biphenyi (PCB)
  Mirex
  Hexachlorobenzene
  Dieldrin
  DDT and metabolites
  2,3,?,8-tetrachlorodibenzo-p-dioxin(23,7,8-TCDD)
  2,3,7,8-tetrachloradibenzofuran
  Benzo-a-pyrene
  Alkylated lead
  Toxaphene
  Mercury
 For every one of these pollutants, there was reason to believe or evidence to support the fact that
 the atmosphere is likely to be a significant pathway. The Commission's International Air
 Quality Advisory Board (IAQAB) also developed a map of the atmospheric region of influence.

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delineating such regions on the basis of emission travel time (one day, three day, five day) to the
lakes and indicating that the scope of significant sources and source regions of these
contaminants can be continental, if not global. Following that report, a binational summary of
emissions of the Critical Pollutants, commissioned by the International Air Quality Advisory
Board was developed by E. Voldner and L. Smith(1991)}. These and other developments
contributed to the inclusion of Annex 15, on Airborne Toxic Substances, in the 1987 Protocol to
the Great Lakes Water Quality Agreement between the United States and Canada.  [Revised
Great Lakes Water Quality Agreement of 1978 As Amended by Protocol Signed November 18,
19874]

That Annex called for research, surveillance and monitoring, and implement of pollution control
measures for the purpose of reducing atmospheric deposition of toxic substances, particularly
persistent toxic substances (PTSs), to the Great Lakes Basin Ecosystem.  The research portion of
the Annex advocated activities to determine pathways, fate and effects of such toxic substances
on the Great Lakes System, Included was the development of models of the intermediate and
long-range movement of toxic substances to determine the relative importance of the
atmospheric pathway  and the  significant sources of such substances, particularly from outside the
Great Lakes System.

Following the inclusion of the Annex, the USEPA and Environment Canada engaged in various
efforts to model the transport  and deposition of PTSs to the Lakes, with limited results.  Some of
their backtrajectory models identified regions in the Carribean and Mexico as sources of
toxaphene and other organochlorides to Northern Canada. [Progress Report 12 of the
International Air Quality Advisory Board (IAQAB), International Joint Commission, October,
1991s]

The modelling effort emphasized regional to long range transport of pollutants rather than local
scale sources with a focus on  heavy metals, organochlorides and pesticides currently or
historically used in North America. Annual estimates of deposition to the individual lakes and
basins were computed for sulphur and nitrogen for the period 1980-1988; for toxaphene around
1980; and for mercury for a thirty day period in late 1980.

At the time, the International Air Quality Advisory Board (IAQAB) of the International Joint
Commission noted that the quality of these model estimates of deposition would be very
dependent on the quality of emission inventories, on knowledge of the chemical and physical
processes affecting their lifetimes in the atmosphere, and on support for further model
development.

In March of 1995, the Commission was among the first to review a report "Quantitative
Estimation of the Entry of Dioxins, Furans and Hexachlorobenzene into the Great Lakes from
Airborne and Waterborne Sources," authored by Dr. Mark Cohen and Dr, Barry Commoner of
the Center for The Biology of Natural Systems (CBNS), Queens College. City University of
New York6 of an attempt to systematically model the atmospheric deposition of dioxin and

                                          -3-

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hexachlorobenzene from sources and source categories throughout the US and Canada.
In April of 1997, the US and Canada signed the Canada-United States Strategy for the Virtual
Elimination of Persistent Toxic Substances in the Great Lakes Basin (commonly referred to as
the Binational Toxics Strategy (BNS)).  This agreement adapted the 1985 WQB/IJC Critical
Pollutants as Level I Persistent Toxic Substances and added a number of pollutants as Level II
substances, [Table 2]

Table 2. Persistent Toxic Substances (Level I and Level II) Identified in the Great Lakes
Binational Toxics Strategy
 Critical pollutants identified by WQB in 1985 are indicated with an asterisk (*).  Persistent
 organic pollutants from CEC Council Resolution #95-5 are identified with a caret (A),
 LEVEL I
LEVEL I!
 Aldrin A
 Dieldrin *A
 Benzo(a)Pyrene {B(a)P} *
 Chlordane A
 DDT, ODD, DDE *A
 Alkylated lead *
 Mercury * and its compounds
 Mirex *A
 Octachlorostyrene
 PCBs *A
 Dioxins (PCDD: 2,3,7,8-TCDD) *A
 Furans (PCDF; 2,3,7,8-TCDF) *A
 Toxaphene *A

 NOTE: Hexabromobiphenyl and Penta-
 chlorophenal are listed as POPs on the CEC
 Council Resolution #95-5 but are not
 included on the Strategy list.
Cadmium and its compounds
1,4-Dichlorobenzene
3,3'-Dichlorobenzidine
Dinitropyrene
Endrin A
Heptachlor and heptachlor epoxide
Hexachlorobutadiene(l,2-and 1,3-)
Hexachlorocyclohexane
(including alpha, beta, delta, lindane)
4,4'-Methylenebis (2-chloroaniline)
Pentachlorobenzene
Pentachlorophenol
Tetrachlorobenzene (1,2,3,4- and 1,2,4.5-)
Tributyl tin
Polycyclic aromatic hydrocarbons (PAHs)
as a group, including but not limited to:
Anthracene
Perylene
Benzo(a)anthracene
Phenanthrene
Benzo(g,h,i)perylene
Over the same time period, the International Air Quality Advisory Board contracted with Dr.
Cohen to report on the status of available data and information on four prerequisites for the
modeling of atmospheric transport of the Level I and Level II contaminants under the 1997
Binational Toxics Strategy. Specifically, Dr. Cohen was asked to review the adequacy of
                                          .4.

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available information and programs in four areas: i) physical and chemical properties of the
BNS contaminants, ii) emission inventories for these contaminants iii) possible applicable
models of their atmospheric transport and deposition and iv) the adequacy of ambient monitoring
information for verification of model determinations.

The Cohen review, as summarized in the 1995-1997 Report of the Priorities and Progress under
the Great Lakes Water Quality Agreement (1997)', ranked contaminants with regard to their
potential for long range atmospheric transport, indicating that a significant majority of the BNS
Level I and Level II pollutants are or could be candidates for long range transport.  However,
modeling of this same majority was impeded by insufficient information on physical and
chemical properties, incomplete or largely non existent emission inventories (and the absence of
seamless binational inventories), limited ambient concentration data and lack of funding to apply
currently available pollutant models to modeling persistent toxic substances.

Notwithstanding these limitations, the Board supported further refinement of the original
Commoner/Cohen dioxin model and its extension to the transport and deposition of atrazine (a
non BNS pollutant), cadmium and mercury to the Great Lakes basin.

THE NOAA/HYSPLIT  MODEL - DIOXIN AND ATRAZINE OUTPUTS

In considering the commitments of the governments under Annex 15, and in search of a tool to
link external sources of persistent toxic substances to receptors in the Great Lakes, the 1AQAB
decided to join others in support of the further application of the HYSPLIT model. This decision
was based on a number of factors, chief among them being i) the availability of enhanced
information on US and Canadian emissions of dioxin from sources and source regions; ii)
reasonable agreement between predicted ambient annual concentrations of dioxin and ambient
measurements already achieved; iii) the efficiency and relatively low level of resources needed to
operate the model; and, iv) the opportunity to demonstrate that a truly binational picture of
sources and source regions of a persistent toxic substance to the Great Lakes, as called for in
Annex 15 of the Great Lakes Water Quality Agreement, could be developed.

Of these factors, perhaps the most intriguing was that the computations necessary to model
transport and deposition could be performed on a bank of personal computers, rather than a
mainframe or  a high end workstation. If the capabilities of the model could be further verified, it
could become attractive to entities whose access to sophisticated computation  facilities would be
limited or nonexistent.

The following discussion of the modeling outputs, of necessity, compresses the efforts and
activities of several individuals and organizations including my co-authors and their agencies, as
well as the Ontario Ministry of the Environment, Environment Canada, and members of the
International Air Quality Advisory Board and the binational Emissions Inventory Working
Group created expressly for this project. The securing and development of compatible emissions
                                         -5-

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 data and their inclusion in a seamless bi-national map required a much greater effort than was
 originally estimated.

 The NOAA HYSPLIT (Hybrid Single Particle Lagrangian Integrated Trajectory) computer
 model was originally developed at the US National Oceanic and Atmospheric Administration for
 medium and long range transport modeling of accidental releases of radioactive materials and is
 also currently used for emergency response situations at NOAA. The development, validation
 and operation of HYSPLIT are described elsewhere [Draxler and Hess, 1998]8.

 The model tracks pollutants emitted from user-specified locations as they are adverted,
 dispersed, and subjected to destruction and deposition phenomena thoughout the specified
 domain.  It has been used in the modeling of sulfur transport and deposition as well as
 contaminants associated with the oil fires in the Persian Gulf. It uses gridded meterological data
 computed by an external model,  in this case, output from the NOAA Nested Grid Model (NGM).
 The NGM takes weather-related  observations  and uses these data to estimate metoerological
 conditions between sources and receptors.  Wind speed and direction, amount and type of
 precipitation, temperature and humidity are among the parameters included in the NGM,

 The physical and chemical properties of the specific pollutants (dioxin and atrazine) were among
 the factors considered in the modification of the  model to ensure a better simulation of transport
 and fate.  Among the processes to be simulated are vapour/particle partitioning, wet and dry
 deposition, reaction with hydroxyl radical and photolysis.  The model and associated
 methodology have been specifically tailored to provide source/receptor information, in this case
 on an annual average basis, a feature not found in many fate and transport models. However,
- other models have been used to estimate fate and transport of persistent toxic substances,
 including~lhe application of RELMAP by the USEPA to dioxin, mercury and cadmium and the
 current use of an Eulerian framework (Models-3) for atrazine and mercury deposition into Lake
 Michigan.

 The modeling of dioxin was a multi-stage process.  First, a binational dioxin emission inventory
 of some quality was being assembled and critiqued. Simultaneously, theoretical transfer
 coefficients associated with a great majority of the counties and census divisions in both
 countries, using the physical and chemical properties of dioxin and meteorological factors, were
 prepared.

 A map of theoretical transport coefficients from various locales in the US and Canada to Lake
 Superior is shown in Figure 1. Regions are depicted in various shades, the darker indicating a
 higher potential for transport and deposition from within this zone to Lake Superior, and the
 lighter, a lower potential for such transport, should sources of dioxin be located within them.
 This theoretical transfer map  was an early step in the process; actual emissions data were then
 used in subsequent calculations to derive estimates of actual deposition contributions. The
 transfer map is different for each congener or mix of dioxin congeners considered, as well as for
 each receptor considered.  This map assumed a mix of congeners typical of the average mix of

                                           -6-

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                                      emissions in the binational emissions inventory.

                                      Figure 1. Dioxin Transfer Coefficients: Theoretical
                                      Fraction of 1996 Dioxin Emissions That Would Be
                                      Deposited in Lake Superior (grams TEQ deposited
                                      per year/grams TEQ emitted per year) from Various
                                      Regions in the United States and Canada

                                      As could be anticipated, given the prevalence of winds
                                      from the west, the Figure indicates that any sources
                                      oriented in this direction would have a greater
                                      potential for deposition in Lake Superior than a source
                                      of similar strength from the east. Distance from the
                                      receptor is obviously a factor; however, the transfer
                                      coefficients are not so reduced by greater distance as
                                      to become insignificant.
Figure 2. Total Dioxin Emissions
for 1995/1996 (County / Census
Division)

To derive an estimate of the actual
deposition of dioxin to Lake
Superior, the transfer coefficient
map is subsequently multiplied by
an emissions inventory map such as
shown in Figure 2. The
methodology assumes that the
atmospheric fate and transport of
dioxin emitted from distinct sources
is linearly independent, consistent
with the fact that concentrations of
dioxins are very low and their fate
processes in the atmosphere can be
characterized by first-order kinetic
rate expressions in which the rate is
a product of a constant and the
concentration.
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                                           -7-

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SOURCE RECEPTOR RESULTS - DIOXJN
in Lake Superior and Lake Huron in
comparison to the influence of more
proximate sources on the lakes Michigan,
Erie and Ontario, which are set in a more
industrial environment. For these latter
three lakes, sources within 100 km account
for a more significant portion of the
deposition. Overall, on the order of 25
percent of the dioxin deposited to each of
the lakes originates from within the Great
Lakes watershed.

Figure 4.  Percent of Total Emissions or
Deposition of Dioxin Arising From
Different Distances from Each Great Lake

A farther delineation of the binational
emission inventory allows a determination
of the contribution of specific source
categories to deposition.  Figure 5
                                           Figure 3 is a synthesis of the transfer coefficients
                                           and the emissions from US counties and
                                           Canadian grid squares, yielding an estimate of
                                           the quantity of dioxin deposited in Lake
                                           Superior from sources within the bounded areas
                                           of the US and Canada,  Similar maps for each of
                                           the lakes have been developed, but, for the sake
                                           of brevity, are not be presented here,

                                           Figure 3.  Mid Range Estimate of the
                                           Contribution of US and Canadian Source
                                           Regions to 1996 Atmospheric Deposition of
                                           Dioxin to Lake Superior

                                           These calculations allow an estimation of the
                                           significance of the contribution of sources in the
                                           various locales to deposition in particular Great
                                           Lakes.  Figure 4 indicates that more distant
                                           sources have a larger contribution to deposition
            toe
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                                             illustrates estimates of the contribution of
                                             specific source categories to the annual dioxin
                                             deposition flux (grams TEQ dioxin
                                             deposited per square kilometer of lake
                                             surface) in particular lakes and on average to
                                             the total surface area of the lakes. This
                                             annualized flux was further divided by the
                                             population of the county or grid to yield a
                                             measure of picograms TEQ deposited per
                                             square kilometer per person-year.

                                             Figure 5. Contribution of Different Source
                                             Sectors to Atmospheric Deposition of
                                             Dioxin to the Great Lakes (pg TEQ
                                             deposition / km2) / (person-year)	

                                             Sources were aggregated into three
                                             categories - incineration, metallurgical
                                             processes, and fuel combustion, with the
                                             incineration sector dominant.  Even on a per-
capita basis, the US contribution appears to be relatively large in comparison to Canada, although
the absence of an estimate of emissions from informal combustion of waste (backyard burning)
in the Canadian inventory may account for some portion of this difference.

MODEL EVALUATION FOR DIOXIN

The modeling predictions at specific locales were compared to local ambient measurements
where such were available. In 1996. 30 day rural ambient air measurements were taken at two
sites in Vermont and a second two in Wisconsin, and one site in Connecticut. Figure 6 shows a
comparison of the modeling predictions with the five available rural samples.


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 The ambient concentrations predicted by the model are consistent with actual ambient
 measurements within the uncertainty of each. However, the uncertainty estimate for the model
 was derived solely from an estimate of uncertainties in the emission inventory; the overall
 uncertainty would be greater when other sources of error in the modeling process are considered.
 While further attempts will be made to estimate the model uncertainty, it is hoped that the two
 governments would extend ambient measurements of dioxin to other locations in the Great Lakes
 basin and thus, create a larger and more regionally based data source for this comparison.

 SOURCE RECEPTOR RESULTS - ATRAZINE

 The HYSPLIT modeling technique was then extended to atrazine, a herbicide in current use
 largely on com and sorghum in the US and Canada. While not yet designated as BNS
 contaminant, it has demonstrated a persistence in the environment significantly above that
 postulated on its introduction. Concentrations above the established USEPA maximum
 contaminant level of 3 ppb have been found in surface and groundwaters and in rainfall. It has
 been targeted as  a pollutant of concern in the Lake Michigan Lakewide Management process and
 was one of four contaminants included in the multi-million dollar USEPA Lake Michigan Mass
 Balance Study. An emission inventory of  some quality, extrapolated from temporally resolved
 estimates oTemissions following application, was available for the year 1991, which indicated
 that 32 million kilograms of active ingredient atrazine were used in the US and Canada.

 Model ing "of atrazine was very similar to that used for dioxin; however, temporal, including
 diurnal, variations were included and the outputs were modeled on a weekly basis over a period
 from March 5  to July 23, 1991.  Approximately 95 percent of estimated emissions in the US and
-Canada would occur during that period.  Theoretical predictions using a Junge-type adsorption
 methodotogy suggest that a significant fraction of the atrazine should exist in the vapor phase.
 However, some measurements have found significant fractions of atrazine in the particulate
 phase (Hillery et al. 19979; Sweet 1999'°).  Thus, the characterization of atrazine's atmospheric
 vapor/particle  partitioning behavior is uncertain. A sensitivity analysis was performed to
 investigate the influence of this uncertainty on the modeling results. It was found that the results
 were relatively insensitive to the vapor/particle characterization.  This finding is likely the result
 of the fact that wet deposition is a dominant fate pathway for atmospheric atrazine. and both
 vapor and particle phase atrazine are very effectively wet-deposited.

 The HYSPLIT Transfer coefficient map was derived and weekly emissions estimates were
 applied to it to yield the map shown in Figure 7. While the significance of sources as far away as
 1000 kms is appreciable, much of the deposited atrazine originates from more proximate locales.
                                          -10-

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Figure 7. Mid Range Estimate of the Contribution of
Regions in the United States and Canada to Deposition
of Atrazine to Lake Superior — March 5 - July 23, 1991
Figure 8 indicates that, for all the lakes except Superior,
about 30 percent of the contribution arises from
emissions within 100 km of the lake; sources within the
Great Lakes basin account for 40 percent of that
deposited in Lake Ontario and 50 percent for lakes
Huron and Erie,
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                                       Figure 8. Percent of Total Emissions or Deposition
                                       of Atrazine with Distance from each Great Lake

                                       MODEL EVALUATION FOR
                                       ATRAZINE

                                       Weekly measurements of atrazine concentrations in
                                       rainfall for 1991 were available from approximately
                                       20 sites remote from heavy atrazine use in the upper
                                       Midwest and the Northeastern United States.
                                       Ambient air or dry deposition concentrations could
                                       not be obtained and  processing of this information
                                       and comparison to the modeling results is ongoing.

                                       In previous work (Cohen et al., 1997"), weekly
                                       calculated model values of atrazine wet deposition
                                       flux were compared against 400 data points available
                                       from 20 wet deposition monitoring sites over a 20
                                       week modeling period.  Except for six outliers, there
                                       was reasonable agreement with the remaining 394
values. The standard deviation between the predicted and measured values  for deposition over
the 20 week study period was 25 percent of the mean measured value; if outliers were excluded,
the standard deviation would be 11 percent.
                                         -II-

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PRELIMINARY CONCLUSIONS

The work to date does allow for a few preliminary conclusions.

1.     The Board and other parties in the HYSPLIT model application recognize that its
       functionality must be subject to further review. Opportunities for same are being actively
       explored.

2.     Notwithstanding this, comparison of outputs to date for dioxin and atrazine to ambient
       measurements suggests that this may be a cost effective technique of linking regional and
       more distant sources and source regions of persistent toxic substances to deposition of
       these substances in particular regions.

3.     The model indicates that, in the management of persistent toxic substances, the
       geographic range of sources which must be considered is quite broad and certainly
       beyond those sources contained in the  Great Lakes region itself.

4.     The model appears to have the potential to be a valuable tool in the evolution of a
       binational (US/Canada) cooperative strategy to manage such emissions.  It could also be
       extended to Mexico as better emissions data from their sources come available.

5.     Although some success in linking sources and receptors of dioxin and atrazine to
       receptors is apparent, and further success is anticipated in ongoing modeling of mercury,
       the binational and national environmental management infrastructure must be
       strengthened if this approach is to be further verified and extended to other contaminants.
       However, significant investment in research associated with the physical and chemical
       properties of the BNS pollutants, improvement (or in some cases, creation) of
       comprehensive emissions inventories of known quality, extension of ambient and source
       monitoring programs to embrace more of these contaminants and support for the
       modeling activity itself, are all necessary if this and similar tools are to be refined.

REFERENCES

1.      William MJ. Strachan and Steven J, Eisenreich,  Science Advisory Board/Water Quality
       Board/International  Air Quality Advisory Board- International Joint Commission May
       1988.  Mass Balancing of Toxic Chemical in (he  Great Lakes: the Role of Atmospheric
       Deposition,

2.      Great Lakes Water Quality Board, International Joint Commission 1985 Report on Great
       Lakes  Water Quality, Windsor, Ontario June 1985
                                         -12-

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3.     Joint Water Quality Board / Science Advisory Board / International Air Quality Advisory
       Board of the International Joint Commission Production, Usage and Atmospheric
       Emissions of 14 Priority Toxic Chemicals, Invited Paper by Eva C, Voldner and Lowell
       Smith. 1991.

4.     Revised Great Lakes Water Quality Agreement of 1978 As Amended by Protocol Signed
       November 18, 1987

5.     International Air Quality Advisory Board of the International Joint Commission,  October,
       1991 Progress Report 12 of the International Air Quality Advisory Board (I AQAB),

6.     Dr. Mark Cohen, Dr. Barry Commoner, Center for the Biology of Natural Systems,
       Queens College, Flushing, NY, May 1995.  Quantitative Estimation of the Entry of
       Dioxins, Fur cms and Hexachlorobenzene into the Great Lakes from Airborne and
       Water borne Sources,

1.     International Joint Commission, Great Lakes Regional Office, Windsor, Ontario,  Canada,
       Fall 1997 1995-1997 Report of the Priorities and Progress under the Great Lakes Water
       Quality Agreement

8.     Draxler, R., and G.D. Hess (1998). "An Overview of the HYSPLITjt  Modeling  System
       for Trajectories, Dispersion, and Deposition." Australian Meteorological Magazine.
       47(4): 295-308.

9.     Sweet, C. (1999), Illinois State Water Survey. Personal Communication.

10,    Hillery, B.R.. I, Basu. and R.A. Hites (1997). Organohalogen Compounds 32: 210-215.

11.    Cohen, M., B. Commoner,  P.W. Bartlett, P. Cooney, H. Eisl (1997). Exposure to
       Endocrine Disruptors from Long Range Air Transport of Pesticides, Report to the W.
       Alton Jones Foundation. Flushing NY:CBNS
KEY WORDS

dioxin, atrazine, modeling, deposition, toxic pollutants, Great Lakes
                                        -13-

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Figure I.  Dioxin Transfer Coefficients: Theoretical Fraction of 1996 Dioxin Emissions That
Would Be Deposited in Lake Superior (grams TEQ deposited per year/grams TEQ emitted per
year) from Various Regions in the United States and Canada
Overall transfer Coefficient
(fraction deposited)

|	 j   0,00001.0.0001

       0.0001-0.001

       0.001 - 0.002 J

       0.0015-0.005

       0.005 -0.01

       0:01 -Oj025

       0,025 - O.OJ

       005-01

       outside of nvxtding dajnam
                                                                               Projection: Lambert Conform!
                                                                                             Conic
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Figure 2. Total Dioxin Emissions for 1995/1996 (County / Census Division)
Airal Density of Dioxin
Emissions (jig TEQton -year)
0-01
OJ -25
25 • 50
50 -75
75 - i 00
k •« 100 • 300
j^HI 300 - 5000
m 5000 - 300000
| | H
-------
Figure 3, Mid Range Estimate of the Contribution of US and Canadian Source Regions to 1996
Atmospheric Deposition  of Dioxin to Lake Superior
                                    300    0     300   600 Ml«
                                                                      Pro jten on; Lambert Conforral
                                                                                     Cone
                                                                       EHmatef were 4cvdope4 bjr
                                                                     combinin); Eamitcd Emiinonf
                                                                        wtttt tht Ex&turtcii Tnmfer

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Figure 4.  Percent of Total Emissions or Deposition of Dioxin Arising From Different Distances
from Each Great Lake
                                              A LtfceSupwni
               0-100
       70040D        700-1000       1500-2000      2500-35)10      5000-10000
tOO 200        400700        1000 1900      20002500      KOB-SOOO
                   Distance Hang* (KM L*k« flu*}
           60

           40
                                               8 UU HMOM
               8-100         200400        700-1000       1300-2000      2800-3500      5000-1000*
                     100-200        400-TOO       1000-1SOO       2000-2500      J500-SOOO
                                               Range INM Lake Qml
           so
         I"
         • 20
              0-100
       200400        700-1000       1W»2000      2MO-3500      5000-10000
100-200        400-700        1000-1SOO      2000-2SDO      3500-SQOO
                   Bitlanc* RanQB ho* LA* |k»l
          GO

          40

          2O
              
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Figure 5. Contribution of Different Source Sectors to Atmospheric Deposition of Dioxin to the
Great Lakes (pg TEQ deposition / km2) / (person-year)
          Great Lakes Average
           incin  metals  fuel
Lake Superior
3
2
1
0





^M
Ut^-— 	 — —




incin metals fuel
               Lake Huron
       -2
        1
       LO
           incin metals  fuel
  Lake Michigan
incin metals  fuel
                Lake Erie
           incin metals  fuel
   Lake Ontario
incin metals  fuel
                                    UMtedStdtes
                               [    I
           "Incin" = wat le inciner aHon;"meUJ*" = n» el ditugical pi oces* ing; "luel"* fael com bu* lion

-------
Figure 6. Comparison of Model Predictions with Ambient Measurements at Month-Long
Sample Sites [Total PCDD/F (TEQ)]



-------
Figure 7. Mid Range Estimate of the Contribution of Regions in the United States and Canada
to Deposition of Atrazine to Lake Superior — March 5 - July 23,  1991
        Cortnbution to
        Deposition
        (grams !o Lake Sup/
        km2 of emissions ares)
           a-onoi
           0.001- 001
           001 -0.1
        -^af 0,1 • i
        •• 1 • 10
        ••10-20
        ••20-30
        •• 30- 39
        *-— Utxise (net Mtelu6*d in 3n»i
        Kill Llk« s«ip«rior
                   OUTICK. Ajrentai^ Cnx*.
                   CtKcrl'or V»o4 «nS A0fcufcr«l Psllrr.
                                 •4MOAA
                                 10O3
1000
2000  Kilometers

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Figure 8, Percent of Total Emissions or Deposition of Atrazine with Distance from each Great
Lake
                                 LahtSupfrior
                                 Lilt Huron
                                Lifci Michigan
                                  Uit Erie
                                 Lilt Ontario
             0-    100.   200   400-  TOO-  1000-  1500-  2000.  2500- 3500-  5000-
            100    200   400   700   1000  1500  2000  2500  3500  5000  10000

                  DISTANCE RANGE FROM LAKE (kilometers)

                         0  Emissions   | Deposition

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                               International Joint Commission
                              Commission mixte Internationale
                                               April 28, 2000
Ms. Amy Butler,
Air and Waste Management Association,
One Gateway Center, Third Floor.
Pittsburgh, PA.
15222

Dear Amy;

Enclosed, as per instructions, is a printed copy of the paper Estimating the Transfer ofDioxin
andAtrazine to the Great Lakes Basin with the NOAA HYSPLIT Model - an Overview. An
electronic file and author release forms accompany the paper.

I understand that this paper (Abstract 984) has been shifted to the Atmospheric Deposition
session AM3-b at the Salt Lake Conference and look forward to an opportunity to present it
there.

In hindsight, I have recognized that the reproduction of complex color illustrations in black and
white and the extensive review process required by my U.S. government co-authors added
considerable time and effort to this particular paper. The patience of you and your colleague, Mr.
Brian Gaetano, are most appreciated.

See vou in Salt Lake.
John F. McDonald,
Great Lakes Regional Office.
International Joint Commission,
P.O. Box 32869,
Detroit, Michigan 48232-2869
mcdonal dj @ vvi ndsor. i j c .org
519-257-6712
                               Windsor * Ottawa  • Washington
                 100, avenue Oueilette Avenue, Windsor, Ontario N9A6T3 (519) 257-6700
                                                            226-2170

-------
Am & WASH MANAGEMENT
ASSOCIATION
        SwtlWJ
                                  REQUEST FOR PERMISSION
                     Estimating The Transfer and Deposition of Dioxin and
Manuscript Title. _ Atraz|ne to tke Qreat Lakes Basin with the NOAA
_  HYSPLIT Model — an Overview
  uthor(s): ."^  f^Oa-in^    Q. &&.JA*-,  A.  **
             ............. .......   p— ™«— •    -....- — ...... - ........... -        .....     .-~ • .- ....................    - .......
The Air & Waste Management Association (A&WMA) requests permission to publish and redistribute your manuscript
(please specify above) in all media of expression now known or later developed, including in paper and/or electronic
form (on the A&WMA web site and/or CD-ROM), as well as sales of paper and/or electronic reprints.

By signing this release, the Author confirms that the manuscript is original on the Author's part except for such excerpts
from copyrighted works as may be included with the written permission of the copyright owners. The Author further
warrants that the manuscript contains no libelous. obscene, or unlawful statements, and does not infringe upon or violate
any copyright, trademark, or other right or the privacy of others. The Author also warrants that in the case of sole
authorship, the Author is the sole owner of the manuscript and all copyrights therein, and has full power and authority to
register all copyrights therein and to make this Agreement, and that in the case of multiple authorship, these powers of
ownership are shared with all other contributing authors. The Author acknowledges that the Air & Waste Management
Association is relying on this release in publishing this manuscript, and agrees to indemnify the Air & Waste
Management Association against liability and expense, including reasonable counsel fees, arising from or out of any
breach of these warranties.

Considering that the Author(s) retain the copyright to this manuscript, please indicate your agreement to grant the
permissions requested for the uses specified above by signing below,

U.S. Government Employees, Grant or Contract Authors: By signing this release, you are certifying that this
manuscript was prepared as part of your official duties, and as such, is a "work of the United States Government" and is
in the public domain and is freely reproducible.
Name:   >4 r. K.v^_  (- <.'•".  < "..*'..-.        Title:   ,^~- -^;.-   ^'^. /  -••-	

Company:   4 i-r '   .'  ,"-,•,   >v       Phone:  f-:- <',  - ^ ^'v / - -/T i.y.

SIGNATURE:    '    •	^  /' .-' / '. : s  „   -	     DATE:  ^ y :  >/' - >r  ' " '-^

Note; No paper will be published by A&WMA unless A&WMA has received a signed permission form from
of the manuscript. In the case of a "work made for  hire" fa work prepared by an employee within the scope of his or her
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should sign.

A&WMA Contact:
              Amy Butler                                       P: (412) 232-3444 x. 3119
              Technical Program Coordinator                       F: (412) 232-3450
              Air & Waste Management Association                 e-mail: abutlera>awma.org
              One Gateway Center. Third Floor
              Pittsburgh, PA 15222 USA

-------
Am & WASIE MANAGEMENT
                                  REQUEST FOR PERMISSION
                     Estimating The Transfer and Deposition of Dioxin and
Manuscript Title: „ Atfm^ ^ ^ Grcat Lakes Bag|jl ^^ the NOAA

	  HYSPLTT Model — an Overview
 -uthorts);
The Air & Waste Management Association (A&WMA) requests permission TO publish and redistribute _ our manuscript
(please specify above) in all media of expression now known or later developed, including in paper and/or electronic
form (on the A&WMA web site and/or CD-ROM), as well as sales of paper and/or electronic reprints.

By signing this release, the Author confirms that the manuscript is original on the Author's part except for such excerpts
from copyrighted works «s may be included with the written permission of the copyright owners. The Author further
warrants that the manuscript contains no libelous, obscene, or unlawful statements, and does not infringe upon or violate
any copyright, trademark, or other right or the privacy af others. The Author also warrants that in the case of sole
authorship, the Author is the sole owner of the manuscript and all copyrights therein, and has full power and authority to
register all copyrights therein and to make this Agreement, and thai in the case of multiple authorship, these powers of
ownership are shared with a!! other contributing authors. The Author acknowledges that the Air &  Waste Management
Association i$ relying on this release in publishing this manuscript, and agrees to indemnify the Air & Waste
Management Association against liability and expense, including reasonable counsel fees, arising from or out of any
breach of these warranties.

ConsJiirirtg that the Aatborfs) retain the copyright to this manuscript, please indicate your agreement to grant die
permissions requested for the uses specified above by signing below.

U.S. Government Employees, Grant  or Contract Authors:  By signing this release, you are certifying that this
manuscript was prepared as part of your official duties, and as such,  is a "work of the United Sates Government** and is
in the public domain and is freely reproducible.

Name;  L MjftSA     STr^U           Trtle:
Company: rViaBgift  fr//AJ/sngW .Qf  fiMHJiGAL f^TiMf^one:
                                                            DATE; AfT i / (f f
Note: No paper will be published by A&WMA unless A&WMA has received a signed permission form from all authors
of the manuscript. In tjie case of a '*work made for hire" (a work prepared by an employee within the scope of his or her
employment or commissioned as a work for hire under written agreement), an authorised representative of the employer
should sign.

        Contact:
             Amy Butler                                      P; C412) 23 2-34*4 x, 3 J19
             TechnieaJ Prognra Coordinator                       F: (A 12} 232-34 SO
             Air & Waste Managemeru Association                  «-maii: ab
             One G«cway Center, Third Floor
             Pittsburgh, PA 15222 USA

-------
Ala fe WAVTT MAM
* » • a c i Trio
                                 REQUEST FOR PERMISSION
                     Estimating The Transfer and Deposition of Dtoiio and
                     4^^ f<| t||e Grea| LmMfS Bft§il|

                     HYSPLIT Model — an Overview
The Air & Waste Management Association (A&WMA) request! permission to publish and redistribute your manuscript
(please specify above) in all media of expression now known or later developed, including in paper and/or electronic
form (on the AAWMA web site nut/or CO-ROM), at well as sales of paper and/or electronic reprints.

By signing this release, the Author confirms that the manuscript is original on the Author's part except for such excerpts
from copyrighted works aa may be included with the written permission of the copyright owners. The Author further
warrants that the manuscript contains no libelout, obscene, or unlawful statements, and does not infringe upon or violate
•ny copyright, trademark, or other right or the privacy of others. The Author also warrants t hm in the case of sole
authorship, die Author is the sole owner of the manuscript and all copyrights therein, and has full power and authority to
register all copyrights therein and to make this Agreement end that in  the case of multiple authorship, these powers of
ownership arc shared with all other contributing authors. The Author acknowledges that the Air & Waste Management
Association is relying on this  release in publishing this manuscript, and agrees to indemnify the Air & Waste
Management Association against liability and expense, including reasonable counsel fees, arising from or cut of any
breach of these warranties.

Considering that the Authors) retain the copyright to this manuscript,  please indicate your agreement to grant the
permissions requested for the uses specified above by signing below.

U.S. Government Employ***, Grant or Contract Authors: By signing this release, you are certifying that this
manuscript was prepared as part of you? official duties, and as such, is a "work of the United States Government" and i»
m the public domain and is freely reproducible.

     «     MAEK   Catted            ™.:_
SIGNATURE:
Note: Mo paper will be published by A&WMA unless A&WM A has received ft signed permissioii form from all authors
of the manuscript. In the case of a "work made for hire" (a work prepared by an employee within tin.- scope of his or her
employment or commissioned as a work for hire under written agreement), an authorised representative of the employer
should sign.

A&WMA Conner:
             Amy lulter                                      P: (412) 233-3444 ».3\\V
             Technical Program Coontinwar                       fr:(4f2
             Air & Wane Mtnigtfntnt Aisoci«uon                  ««in»il:
             On* Gateway Center. Third Floor
             Plmburgh. PA 13222 USA

-------
   it WASH:
        S,..-cl«m
                                  REQUEST FOR PERMISSION
                     Estimating The Transfer and Deposition of Dioxin and
Manuscript Title: _  Atrazine tft the Qrcat Lake§ Basin ^^ the NOAA

— _ , _  HYSPLIT Model — an Overview

*. ythor(s): Jo>U  McDonald'  Mark (thenj  ])<*. <6/2t Af^y^r ' larissa.  Ma+YJtfi*it* *

The Air & Waste Management Association (A&WMA) requests permission to publish and red'-strcbiite ^our manuscript
(please specify above) in ail media of expression now known or later developed, including in paper and/or electronic
form (on the A&WMA web site and/or CD-ROM)* as well as sales of paper and/or electronic reprints,

By signing this release, the Author confirms chat the manuscript is original on the Author's part except for such excerpts
from copyrighted works as may be included with the written permission of the copyright owners. The Author further
warrants that the manuscript contains no libelous, obscene, or unlawful statements, and does not infringe upon or violate
any copyright, trademark, or other right or the privacy of others. The Autitor also warrants thai in the case of sole
authorship, the Author is the Sole owner of the manuscript and all copyrights therein. a»d ha* full power and authority 10
register all copyrights therein and to make this Agreement, and that in the ease of multiple authorship, these powers of
ownership are shared with all other contributing authors- The Author acknowledges that the Air &. Waste Management
Association is relying on this release in  publishing this manuscript, and agrees to indemnify the Air &. Wasts
Management Association against liability and expense, including reasonable counsel fees, arising from or ojt of any
breach of these warranties,

Considering that the Authorfs) retain the copyright to this manuscript, please indicate your agreement to grant the
permissions requested for the uses specified above by signing below,

U.S. Government Employees, Crawl or Contract Authors; By signing this release, you .ire certifying that this
manuscript was prepared as part of your official duties, and as such, is a "work of the United States Government" and is
in the  public domain and is freely reproducible.

Name; .. .  \ \)^Qf~Q*__ . JsAje,,'4:g.:C _ Title: ..

Company:   U.S.  £ P A _ _____   Phone: (3 \3\jP-Syj-Ob t#

SiGNATURS;   ^^^£>L^yi^€^^ _      DATE:  _^L28 /OO
                                                                        "^
Note: No paper will be published by A&WMA unless A&WMA has received a signed permission form from allllirtRors
of the manuscript. In the case of a "work made for hire" (a work prepared by an employee within the scope of his or her
employment or commissioned as a work for hire under written agreement), an authorized reprtseiitaiive of the employer
should sign.

         Contact;
              Amy iwtler                                      Ft 14 12) 232-3444 x. ; J 1 9
              Technical Program Coordinator                        F: (412) 232-3450
              ftir & Waste Management Association                   e-mail: abut|cr(2>a*»tna.cpri»
              One Caiewoy Center, Third Floor
              Pittsburgh, PA  15222 USA

-------
    N1IL-RTP-IO-00-088
TECHNICAL  REPORT DATA
 1. REPORT NO.

EPA/600/A-00/033
                                                          3,RECIPIENT'S ACCESSION NO.
 4. TITLE AND SUBTITLE

 Estimating the Transfer and Deposition of Dioxin and
 Atrazine to the Great  Lakes Basin with the NOAA
 HYSPLIT Model - an Overview
                                                          5.REPORT DATE
                           6.PERFORMING ORGANIZATION CODE
7. AUTHOR(S)

John McDonald  (IJC),  Dr.  Mark Cohen  (NOAA),  Debra
Meyer (USBPA), Larissa Mathewson  (OMNR)
                                                          8.PERFORMING ORGANIZATION REPORT NO.
9. PERFORMING ORGANIZATION NAME AND ADDRESS

International Joint  Commission
Regional Office
100  Ouellette Ave.,  8th Floor
Windsor,  Ontario N9A 6T3
                                                          10.PROGRAM ELEMENT NO.
                           11. CONTRACT/GRANT NO,
12. SPONSORING AGENCY NAME AND ADDRESS

Air  &  Waste Management  Association
One  Gateway Center, Third Floor
Pittsburgh,  PA 15222
                           13.TYPE OF REPORT AND PERIOD COVERED

                           Conference Proceedings,  FYOO
                           14.  SPONSORING AGENCY CODE
15. SUPPLEMENTARY NOTES"
16. ABSTRACT
Over  the last few years,  the International Joint Commission  has been supporting
development of a PC-based transfer model,  derived from the HYSPLIT model created at
the National Oceanic  and Atmospheric Administration  (NOAA),  to determine, in a cost-
effective way, the extent of deposition  of selected persistent toxic substances  to
the Great Lakes from  US  and Canadian sources and source regions.   Outputs for dioxin
and atrazine will be  described, quantifying the percentage of  emissions of these
substances from specific point and county  level sources which  will be deposited  in
Lake  Superior.  The impact of specific sources and source categories will be
considered.  The authors believe this technology will prove  useful as a took in
developing a strategy for further control  of these sources.
17.
                                KEY WORDS AND DOCUMENT ANALYSIS
a.
                  DESCRIPTORS
               b.IDENTIFIERS/ OPEN ENDED
               TERMS
                                                                          C.COSATI
18. DISTRIBUTIOS STATEMENT
                                               19. SECURITY CLASS (This
                                               Report)
                                          21.NO. OF PAGES

                                              26
                                               20. SECURITY CLASS (This
                                               Psge)
                                                                          22. PRICE

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