Proceedings:  Annual Acid Deposition Emmission
    Inventory Symposium (2nd),  November 1985
    Radian Corp.,  Research Triangle Park,  NC
    Prepared  for

    Environmental  Protection Agency
    Research  Triangle Park,  NC
    Apr  86
                                                                PB86-217148
U.S. Mpartnwnt of

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                                         EPA/600/9-86/010
                                         April  1986
                 PROCEEDINGS:

         SECOND ANNUAL ACID DEPOSITION

         EMISSION INVENTORY SYMPOSIUM

               (November 1985)


             James B.  Homolya and
         Patricia A.  Cruse, Compilers
              Radian  Corporation
                   Box 13000
 Research Triangle Park,  North Carolina  27709



    EPA  Contract No.  68-02-3994, Task 032
             EPA Project Officer:

                J. David Mobley
Air and Energy Engineering Research Laboratory
     U. S. Environmental Protection Agency
 Research Triangle Park, North Carolina  27711
  AIR  AND ENERGY  ENGINEERING RESEARCH LABORATORY
       OFFICE  OF  RESEARCH AND DEVELOPMENT
      U.S.  ENVIRONMENTAL PROTECTION  AGENCY
        RESEARCH  TRIANGLE PARK,  NC 27711

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                                 TECHNICAL REPORT DATA
                           {Plcasf rraii /wn/urfiuni on the rrtenf bffort (.o
 \ R t PORT MO
  EPA/600/9-86/010
 J TiTLt A\O SUBTITLE
 Proceedings: Second Annual  Acid  Deposition
  Emission Inventory Symposium (November 1985)
                                    5 REPORT DATE
                                     April 1986
                                    6 PE RFORMING ORGANIZATION CODE
 'AuTnORtSI

 James B.  Hornolya and Patricia A.  Cruse, Compilers
                                                        8 PERFORMING ORGANIZATION REPORT NO
 9 PERFORMING ORGANIZATION NAME ANO AUORESS
 Radian Corporation
 P.O. Box 13000
 Research Triangle Park, North Carolina 27709
                                    3 RECIPIENT S ACCESSIOWNO
                                             ? 171  48 /AS
                                                        10 PROGRAM E LEMENT NO.
                                    11 CONTRACT/GHANT NO
                                     68-02-3994, Task 32
 12 SPONSORING AGENCY NAME ANO ADDRESS
  EPA, Office  of Research and Development
  Air and Energy Engineering Research Laboratory
  Research Triangle Park, NC 27711
                                                        13 TYPE OF REPORT AND PERIOD COVERED
                                     Proceedings; 11 /
                                    14. SPONSORING AGENCY CODE
                                      EPA/600/13
 15 SUPPLEMENTARY NOTES AEERL project officer is J.  David  Mobley, Mail Drop 61. 919/
 541-2612.
 16 ABSTRACT -phase proceedings document a 2-day symposium, held to discuss progress
 made by the National Acid Precipitation Program (NAPAP) and other organizations
 in developing emission inventories. The symposium was sponsored by EPA's Air
 and Energy Engineering Research Laboratory, in cooperation with EPA's Office  of
 Air Quality Planning and Standards, the U. S.  Department of Energy,  the National
 Oceanic and Atmospheric Administration, and NAPAP.  The meeting was intended
 primarily for government, academic,  and private sector individuals involved in
 developing or using emission inventories for acid deposition related  activities.
 Topics  addressed included historical emissions estimates,  the 1980 and 1985 emis-
 sion inventories,  Eulerian modeling analyses,  and uncertainties in emission inven-
 tories.  The proceedings  provide valuable documentation of results of efforts to date
 to develop emission factors and emission inventories for anthropogenic and natural
 sources.
                              KEY WORDS AND DOCUMENT ANALYSIS
                 DESCRIPTORS
 Pollution
 Emission
 Inventories
 Assessments
 Precipitation
  (Meteorology)
Acidification
Euler Equations  of
  Motion
Mathematical Models
Analyzing
                                           b IDENTIFIERS/OPEN ENDED TERMS
                                          Pollution Control
                                          Stationary Sources
                                          Emission Inventories
                                          Acid  Precipitation
                                          Emission Factors
                                          Eulerian Modeling
                                                                     c.  COSATI 1 leld/Group
13 B
14G
15E
14 B

04B
07B.07C

   12 A
3 DISTRIBUTION STATEMENT

Release to Public
                                            19 SECURITY CLASS (THll Krporl/
                                            Unclassified
                                                   NO OF PAGES
                                                    279
                                           20 SECURITY CLASS (Thilpagr/
                                            Unclassified
                                                                     22 PRICE
EPA Form 2220-1 (»-73)

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                      NOTICE

This document has been reviewed in accordance with
U.S. Environmental Protection Agency policy and
approved for publication.   Mention of trade names
or commercial products does not constitute endorse-
ment or recommendation for use.
                       11

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                                  ABSTRACT

     A two-day symposium was held to discuss progress made by the National
Acid Precipitation Assessment Program and other organizations in the
development of emission inventories.  The symposium was sponsored by the
Environmental Protection Agency's Air and Energy Engineering Research
Laboratory, Research Triangle Park, North Carolina, in cooperation with the
EPA Office of Air Quality Planning and Standards, the U. S. Department of
Energy, the National Oceanic and Atmospneric Administration, and the National
Acid Precipitation Assessment Program.  The meeting was intended primarily
for government, academic,  and private sector individuals involved in the
development or use of emission inventories for acid deposition.   Topics
addressed at the meeting included historical emissions estimates and the 1980
emission inventory, the 1985 emission inventory, Eulerian modeling analyses,
and uncertainties in emission inventories.  The symposium proceedings provide
a valuable -"'"T'jm^r.i.ation Of results of efforts to date to develop emission
factors end emission inventories for anthropogenic and natural  sources.

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                                  ABSTRACT

     A two-day symposium was held to discuss progress made by the National
Acid Precipitation Assessment Program and other organizations in the
development of emission inventories.  The symposium was sponsored by the
Environmental Protection Agency's Air and Energy Engineering Research
Laboratory, Research Triangle Park, North Carolina, in cooperation with the
EPA Office of Air Quality Planning and Standards,  the U.  S.  Department of
Energy, the National Oceanic and Atmospheric Administration, and the National
Acid Precipitation Assessment Program.  The meeting was intended primarily
for government, academic, and private sector individuals  involved in the
development or use of emission inventories for acid deposition.   Topics
addressed at the meeting included historical emissions estimates and the 1980
emission inventory, the 1985 emission inventory, Eulerian modeling analyses,
and uncertainties in emission inventories.  The symposium proceedings provide
a valuable documentation of results of efforts to  date to develop emission
factors and emission inventories for anthropogenic and natural  sources.

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                              TABLE OF CONTENTS

                                                                      Page

ABSTRACT	   i i i

SESSION 1:  DEVELOPMENT OF NAPAP EMISSION INVENTORIES FOR
            ANTHROPOGENIC SOURCES	     1
     Ed Trexler, Chairman

Overview of NAPAP Emission Inventory Activities for
Anthropogenic Sources	     2
     J. David Mobley  (Speaker), Dale Pahl,  and Frederick Sellars

Assessment of the Final 1980 NAPAP Emissions Inventory	    13
     Douglas Toothman

Development of the NAPAP Utility Reference File	    22
     Edward Pechan (Speaker), James Wilson, and Kristin Graves

Development of an Emissions  Inventory to Support Testing of the
Eulerian Regional Acid Deposition Model	    31
     Frederick Sellars

Uncertainty Analysis  of the  NAPAP Emissions Inventory	    43
     Carmen Benkovitz

SESSION 2:  DEVELOPMENT OF NAPAP EMISSION INVENTORIES FOR
            ANTHROPOGENIC SOURCES (continued)	    54
     John Bosch, Chairman

Application of the NAPAP Emission Inventories  to Eulerian
Model ing	    55
     Joan Novak  (Speaker) and Paulette Middleton

Historic Emissions of SO- and NO  Since 1900 by Stack Height
Range and by Season	    61
     Gerhardt Gschwandtner

Development of Monthly Emissions Trends for Recent Years	    71
     Duane Knudson

Application of Historic Emissions Inventories  to the Development
of the 1984 Acid Deposition  Assessment	    86
     Paul  Schwengels

Overview of the Development  of the 1985 NAPAP Inventory	   88
     Charles Mann
      Preceding page blank

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                                                                       Page

 Assistance to the States in the Development of the 1985 NAPAP
 Emissions Inventory .................................................    94
     David Johnson (Speaker) and Mark Hodges

 SESSION 3:  FORMULATION OF MAN-MADE POLLUTANT EMISSION FACTORS ......   120
     Dale Pahl , Chairman

 Development of NAPAP Emission Factors for Anthropogenic Sources .....   121
     Jim Homolya

 Size-Selective Participate Emission Factors for Emission
 Inventories [[[
     Frank Noonan
Field Measurement Studies for the Development of Point Source
Emission Factors [[[   153
     James Ekmann

VOC Composition of Automotive Exhaust and Solvent Usage in
Europe [[[   161
     C.  Veldt

SESSION 4:  DEVELOPMENT OF EMISSION INVENTORIES FOR NATURAL
            SOURCES .................................................   176
     Fred Fehsenfeld, Chairman

Measurement of Biogenic Sulfur Fluxes at Three Sites in the
Eastern  United States ...............................................   177
     Paul Goldan (Speaker),  W. C. Kuster, F. C. Fehsenfeld, and
     D.  L. Albritton

Determination of Nitrogen Emissions from Natural Sources ............   184
     Fred Fehsenfeld (Speaker),  E. J. Williams, and D. D. Parrish

Alkaline Aerosols Emissions ..........................                  193
     Dale Gillette

Methodology for Estimating Natural Hydrocarbon Emissions ............   201
     James Reagan

SESSION  5:  RELATED EMISSION INVENTORY DEVELOPMENT ACTIVITIES .......   207

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                                                                      Page

Generation of Temporally-Resolved Emission Inventories for
Canada	   220
     Trevor Scholtz (Speaker) and Frank Vena

Historical Analysis of Sulfur Dioxide and Nitrogen Oxide
Emissions in Canada	   234
     Tom Furmanczyk (presented by Frank Vena)

United Kingdom Emission Inventories	   245
     Simon Cjgleston

APPENDIX:  ATTENDEES	   261
                                    VI 1

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         SESSION 1:   DEVELOPMENT  OF  NAPAP  EMISSION  INVENTORIES FOR
                                 ANTHROPOGENIC  SOURCES

Chairman:   Ed Trexler
           U. S.  Department  of  Energy  FE-13
           Washington,  D.C.   20545

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           OVERVIEW OF NAPAP EMISSIONS INVENTORY

           ACTIVITIES FOR ANTHROPOGENIC SOURCES
                            by

             J. David Mobley and Dale A. Pahl
      Air and Energy Engineering Research Laboratory
           U.S. Environmental Protection Agency
       Research Triangle Park,  North  Carolina  27711

                   Frederick M. Sellars
                  GCA/Technology Division
               Bedford,  Massachusetts  01730
                       Presented  at:

Second Annual  Acid Deposition Emission Inventory Symposium
                Charleston, South Carolina


                   November 12-14,  1985

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                 OVERVIEW OF NAPAF EMISSIONS INVENTORY
                  ACTIVITIES  FOX ANTHROPOGENIC  SOURCES
                                ABSTRACT

     The National  Acid Precipitation  Assessment  Program  (NAPAP)  has
charged its Task Group B  on  Man-Made  Sources with  the  development  of
comprehensive and accurate inventories  of  emissions  from anthropogenic
sources believed to be important in acid deposition  processes.   This
effort involves developing estimates  of past,  present, and  future  acid
deposition precursor emissions  with adequate geographic,  temporal, and
sectoral resolution to support  the research requirements  of NAPAP.   It
also entails quantifying  the degree of  uncertainty associated with those
estimates.  The major anticipated needs for emissions  data  include:
historical analyses of short- and long-term trends in  emissions;
atmospheric modeling using Lagrangian and  Eulerian techniques;  and
overall assessments of the acid deposition phenomenon.   This paper
presents an overview of the  current and future activities related  to the
development of anthropogenic emissions  inventory data.   Included are
descriptions of the products that have  been generated  by  Task Group  B
and plans for the integration of activities surrounding  the development
of the 1985 NAPAP Emissions  Inventory.

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                  OVERVIEW OF NAPAP EMISSIONS INVENTORY
                  ACTIVITIES FOR ANTHROPOGENIC SOURCES
                               INTRODUCTION

     The National Acid PrecipitatVn Assessment Program (NA°AP) was
 established by Congress in 1980 to coordinate and expand research on
 problems posed by acid deposition in and around the United States.  The
 program is composed of 10 task groups having specific technical
 responsibilites.  One of these groups, Task Group B:  Man-Made Sources,
 is charged with providing a complete and accurate inventory of emissions
 from anthropogenic sources thought to be important in acid-deposition
 processes.
     To fulfill its stated objectives and to support other related NAPAP
 research, Task Group B either has generated or is planning the following
 major data bases:

     •    Historical Emissions Estimates.
     •    1980 NAPAP Emissions Inventory (Versions 1.0 through 5.2).
     •    1985 NAPAP Emissions Inventory.
     •    Regional Acid Deposition Model Field Validation Emissions
          Inventory.

     The primary focus of FY 85 emissions inventory activities was
directed toward fulfillment of the emissions data base requirements for
development and testing of the Eulerian Regional  Acid Deposition Model
 (RADM).   Within the EPA's Office of Research and Development, the
Atmospheric Sciences Research Laboratory has been assigned the lead

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responsibility for developing the RADM.   National  Center for Atmospheric
Research (NCAR) has been assigned the Usk  of developing the model
framework which includes a number of chemical  transformation modules.
The variety of these modules under development dictates the specific
chemical species required in the emissions  inventory.
     The FY 85 emissions inventory development program was also directly
supportive of certain "assessment" activities.   The emissions inventory's
needs for assessment purposes are generally less detailed and resource
intensive than modeling requirements, but are nonetheless extremely
important to the overall  NAPAP program.   Assessment projects use more
aggregated emissions information In combination with models or other
analytic techniques to evaluate the relative importance of various
pollutants, regions, and types of sources,  to the  acid deposition
problem.  Results of these studies have  implications for planning
additional  research needed and development  of potential
control/mitigation strategies.

                               DISCUSSION

     The major tasks accomplished during FY 85  and planned for FY 86 are
discussed below.
Historical  Emissions Estimates
     In  order to provide a basis for evaluating acid precipitation
related  damage and for studying trends in water chemistry and deposition
m<  Jtoring data,  it is important to understand  both historic (long-term)
and recent (short-term) trends in emissions.  Historic SO  and NO
emission levels for the U.S.  were estimated by  individual  source
category on the state level  from 1900 to 1980 for  every fifth year and
for 1978.   These emissions were calculated  from fuel consumption and
industrial  output statistics,  estimates  of  average statewide fuel
properties, and estimates  of emission factors specific to each source
category.   The emissions  estimates were  then aggregated to show the
emissions trends  by state,  region,  and all  states  combined.

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     To support a number of short-term trends analyses, Task Group B
developed monthly SO- and NO  emissions estimates for the years 1975
through 1983.  Annual state total S0? and NO  estimates were used
with fuel consumption and industrial production data to provide monthly
values on a  state-by-state basis.  A system to provide continually
updated and  refined monthly data, using periodically published
information, was also formulated as part of this effort.
     Long- and short-term historical S0_ emissions are depicted in
Figures 1 and 2, respectively.
1980 Emissions Inventory
     The contents of the 1980 NAPAP Emissions Inventory (Version 5.0)
and corresponding Eulerian Modeling Inventory (Version 5.2) are shown in
Figure 3.  Compilation of these products required the integration of
several unique, but related, work efforts, as shown in Figure 4.
     The 1980 NAPAP Emissions Inventory, representing the most
comprehensive and highest quality emissions data available for the 1980
base year, was completed.  The emissions inventory was compiled, starting
with the 1980 "snapshot" inventory, from EPA's National Emissions Data
System (NEDS).  Updates were made to address known deficiencies in the
NEDS data.  These included substitutions of specific data with
information from other inventories or data bases that were believed to
be more reliable (e.g., replacement of fuel data for major utility
boilers using 1980 Federal  Power Commission data).  Emission factors and
corresponding emissions estimates for a number of pollutants not
contained in NEDS were also developed and incorporated.  Data covering
Canada were added, and improvements were made to methods used to
calculate area source and highway .-ehicle emissions.  Systematic quality
control checks were also completed for all significant data items in the
emissions inventory, and estimates of uncertainty were made.
     The importance of the utility industry has been recognized by Task
Group B,  which is responsible for not only developing estimates of
current emissions from the utility sector but also for projecting future
emissions.   Because of different but overlapping needs, Task Group B has
developed a single data has* that will  meet the utility-related data

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 needs  of  all  NAPAP task groups, the NAPAP Utility Reference File
 (NURF).   The  NURF consists of four component files:  the master unit
 data file (containing information on dll electric utility generating
 units), the fuel specific emissions file (containing emissions
 information by  fuel and input), the stack parameters file (containing
 stack  information on a unit-specific basis), and the announced unit file
 (containing unit-specific information on units coming on-line or
 converting to coal-firing after 1980).   The NURF was utilized to derive
 and  verify emissions data from the utility sector in the 1980 NAPAP
 Emissions Inventory.
     As previously stated, one of the most extensive applications of the
 1980 NAPAP Emissions  Inventory is to support development and testing of
 the  RADM.   For this purpose,  the 1980 NAPAP Emissions Inventory
 (Version 5.0)  had to  be further resolved temporally, spatially, and by
 component species (Version 5.2).
     Annual emissions had to  be allocated to hourly profiles for a
 typical weekday, Saturday, and Sunday in each season; county-level area
 sources and minor point sources had to  be spatially resolved to modeling
 grid cells; N0x emissions had to be split into NO and NO^;  TSP
 emissions  had  to be assigned  to alkalinity classes; and VOC emissions
 had to  be  apportioned into 30 photochemical  reactivity classes.
     Development of a methodology and a computerized data base for
estimating the uncertainty associated with the 1980 NAPAP Emissions
 Inventory  was  also  undertaken.   A workshop was held during which expert
opinion was solicited and a modified Delphi  method was applied to arrive
at quantitative estimates for the auxiliary data needed to calculate the
uncertainties  of emissions values.   Methodologies are now being
developed  for  the use of expert opinion to generate the auxiliary data
needed  to  calculate emissions uncertainties for the NAPAP 1985 base year.
1985 Emissions Inventory
     FY 86 activities have been focused on tl^e development of the
1985 NAPAP Emissions  Inventory.   Much of the work that went into the
development of the  1980 inventory will  be drawn upon to create the 1985
 data base, as  shown in Figure 5.  One important departure from the
 approach used  to develop the  1980 NAPAP Emissions Inventory is the

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enlistment of  individual state agencies to supply new 1985 emissions
data  for the NEDS  system, specifically for the NAPAP effort.  Previous
efforts have started with NEDS "snapshot" files which did not
necessarily represent the best data available from the states.  As a
result, a major  state interface/assistance component will be involved.
      In addition,  efforts related to development of the 1985 data base
will  include:  incorporation of 1985 Canadian data, 1985-specific
temporal allocation factor development, enhancements to spatial
allocation and speciation data, verification tests to support emission
factor refinements, and an enhanced QA program.
RADM  Field Evaluation Emissions Inventory
      Another focus area for FY 86 relates to a proposed field study for
validating the Eulerian Regional Acid Deposition Model  (RADM).  This
would entail development of an "episodic" emissions inventory for
pre-set intensive  study periods including collection of actual (rather
than  typical)  hourly emission values using Continuous Emissions
Monitoring (CEM) for major sources, and accounting for phenomena such as
major forest fires, chemical spills, and process upsets.   The episodic
inventories ccjld  then be used with corresponding deposition and
atmospheric chemistry measurements to validate the RADM.

                               CONCLUSIONS

      Task Group  B has generated a number of data bases to fulfill its
stated objectives.  These include estimates of historic emissions back
to 1900 to support long-term trends analyses; estimates of monthly
emissions from 1975 through 1983 to support short-term trends analyses;
estimates of 1980 emissions on both an annual basis, and with the
necessary temporal, spatial, and pollutant species resolution to support
Eulerian modeling analyses; and estimates of uncertainty associated with
the 1980 NAPAP Emissions Inventory.  Work planned for FY 86 includes
development of an emissions inventory for the 1985 base year, and
development of an episodic emissions inventory to support field
validation of the RADM.

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Figure 1.   Overall trena  in  $02 and NOX  emissions  from 1900 to  1980

            for the U.S. and  by source category for each study year.
         CO


         O


         C
         O
          C
          O
          E
         u
             2.6
             2.4
             O.2
                                     /

                                               •v.
                                               &

                 ' f ' " f ' " i' ' " i' ' " i' ' " i' ' " i' ' " i* '-" i' ' " i' ' '* I

                 Jon  F»b Mor Apr  Moy  Jun  Jul  Auq S»p  Oc<  Nov  0»c


                                     Month
      Figure 2.   Monthly trends  in U.S. S02  emissions  for 1980.

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TEMPORAL
RESOLUTION
GEOGRAPHIC
DOMAIN/
RESOLUTION
POLLUTANTS
   1980 NAPAP
ANNUAL EMISSIONS
   INVENTORY

Annual/seasonal
48 Contiguous
states and
Canada with area
sources at the
county level
S00
               TSP
               Pb
               CO
               HC1
               HF
               NCx

               VOC
           1980 NAPAP EULERIAN
             ACID DEPOSITION
       MODELING EMISSIONS INVENTORY
Hourly emissions values for a
typical  weekday, Saturday,  and Sunday
for all  four seasons
48 States and Canada; separate
major point source file with minor
point sources and area sources
assigned to 63,000 20 x 20  km
grid eel Is
so2
so4
TSP:
 - Ca
 - Mg
 - K
 - Na
Pb
CO
HC1
HF
NO
                                  VOC:
                                   - Methane
                                   - Ethane
                                   - Ethylene
                                   - Propane
                                   - Propylene
                                   - N-butane
                                   - 1,2-butene
                                   - Isobutane
                 VOC (cont.)
                  - Isobutene
                  - Trans-2 butene
                  - Pentane
                  - Isopentane
                  - 2,3-dimetnylbutane
                  - Other alkenes
                  - Other alkanes
                  - Formic acid
                  - Acetic acid
                  - Other organic acids
                  - Formaldehyde
                  - Acetaldehyde
                  - Propionaldehyde
                  - Acetone
                  - Other ketones
                  - Other aldehydes
                  - Xylene
                  - Benzene
                  - Toluene
                  - Ethyl benzene
                  - Other aromatics
      Figure 3.  Contents of the 1980 NAPAP emissions inventories.
                                   10

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NAPAP UTILITY
REFERENCE FILE
   EMISSION
   FACTORS
STATE EMISSIONS DATA
FOR 1980
1

1 NAPAP EMISSIONS INVENTORY
| FOR 1980


.
1
f '
'
1

1
EMISSIONS INVENTORY FOR THE
EULERIAN ATMOSPHERIC MODEL
FOR 1980
  QUALITY
 ASSURANCE
UNCERTAINTY
 ESTIMATES
  Figure 4.  Major program components for developing  the
             1980 NAPAP Emissions  Inventory.
                             11

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     STATE
   ASSISTANCE
       1985
    NEDS FILES
SO?, MOX, CO,  VOC,
   PARTICULATES
    SOX/NOX
   ALLOCATION
    FACTORS
 VOC ALLOCATION
    FACTORS
HOURLY EMISSION
   PROFILES
                           INVENTORY
                       IMPROVEMENTS AND
                           ADDITIONS
 SPATIAL SOURCE
  ALLOCATIONS
                          1985 K'APAP
                      EMISSIONS INVENTORY
                           CANADIAN
                           INVENTORY
                           EMISSION
                           FACTORS
                         VERIFICATION
                             TESTS
                          UNCERTAINTY
                           ESTIMATES
                                                   QUALITY
                                                  ASSURANCE
      Figure 5.   Integration of activities for developing
                 the 1985 NAPAP Emissions Inventory.

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                 ASSESSMENT  OF  THE  FINAL

              1980NAPAP EMISSIONS  INVENTORY
                   Douglas A. Toothman
                Engineering-Science,  Inc.
                  10521 Rosehaven Street
                 Fairfax, Virginia   22030
               EFA Contract No.  68-02-3996

          Work Assignment Nos.  1,  2,  10,  and 11

          EPA Project Officer:   J. David  Mobley

      Air and Energy Engineering  Research Laboratory

           U.S. Environmental  Protection  Agency

      Research Triangle Park,  North Carolina  27711
                      Presented at:


Second Annual Acid Deposition Emission  Inventory Symposium

                Charleston, South Carolina

                   November 12-14,  1985
                             13

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                           ASSESSMENT  OF  THK r'INAL
                        1980 NAPAP EMISSIONS INVENTORY

                        oy:   Douglas A. Toothman
                             Engineering-Science, Ir.c.
                             Ka i rf ax ,  Virginia  22U30
                                   ABSTRACT


      A detailed  1980  base year emissions  inventory has  been  developed to
 support the needs  of  various tas'-: groups  within the. National Acid Precipi-
 tation Assessment  Program (NAPAP).  The emissions inventory  was compiled
 startinq with  the  1980 "snapshot" inventory fr0.1 EPA's  National Emissions
 Data  System (NL^iS)  which was converted  to Emissions Inventory System  (EIS)
 format.  Updates were made to address  areas whf>re the NEDS  inventory  was
 known to be deficient.   In addition to  S'JX, NOX, nor.-me thane V(XJ, T.^P,
 and CO which are included in NEDS, emissions estimates  fvr  S'J,j, N H ^,  to-
 tal VU_"
 emissions  estimates  for tne highway vehicle, res i i--n tial  wood c-j'ib'js t ion,
 and organic solvent use area source categories have been  improved.   Sys-
 tematic quality control checks have be?n  completed for  all  significant
 data  items  in   the  emissions  inventory  for major point sources.   The  most
 recent version of  the emissions inventory.  Version 5.0,  is  now b^ing  fi-
 nalized.   Therefore,  emissions data presented herein reflect Versions
 3.0 and 4.0 for which detailed summaries  are available.   Emissions of
SOX,  NOX,  and  VOC,  which are of primary interest for acid deposition
research,  are  27.1, 23.7,  and 23.3 million tons p~ r year, respectively.
Emissions  in the NAPAP  data  base agree  reasonably well  with  Work Group
38 and  EPA/OAQPS emissions trends estimates.  NAPAP fuel  use data show
reasonable  agreement  with  fuel  values in  DOE's State Energy  Data Report.
Version 5.0 of the NAPAP data base represents the he^r  detailed 1980
emissions  inventory presently available.

                                      14

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                         ASSESSMENT OF  THE FINAL
                       1980 NAPAP  EMISSIONS INVENTORY
                                INTRODUCTION

     This project required development of  a central, qua li ty -assured data
base of emissions of pollutants  of  interest for ao id deposition  research
and modeling.  The pollutants  believed to  b^ most important  in  acid depo-
sition processes — sulfur oxides,  nitrogen oxides,  primary  sulfate, vola-
tile organic compounds  (VO-Cs),  ammonia,  chlorides, fluorides, and others
— were addressed.  The data needed consist primarily of  emissions esti-
mates  for the 19HO base year with adequate geographic and  temporal detail.
The area covered includes  the  48 contiguous states of the  U.S.,  the Dis-
trict  of Columbia, and  the 10  provinces  and 2 territories  of Canada.
     The starting point for the 1980 NAPAP emissions data  base  was the
1980 "snapshot" data  file  of  the National  Emissions Data System  (NEUS),
maintained by the U.S.  Environmental Protection Agency  (EPA) at  Research
Triangle Park, North Carolina.   Activities to Create the initial detailed
NAPAP  emissions inventory  from the  1980 NEUS "sncirshot"  file began in Jan-
uary 1983,  The Fhiissions  Inventory System (EIS) was selected  to store
the NAPAP emissions data base.   A goal of  the initial conversion to EIS
was to maintain equivalency between emissions totals in  NEDS and EIS.

                                 DISCUSSION

     In an effort  to  improve  the quality of the initial  NAPAP  emissions
data base, updates were initiated to address areas where the NEDS inven-
tory was known  to  be  deficient.  The following updates  resulted in Ver-
sion 1.0 of  the  inventory  (11/29/83) and  include:
     o  Incorporating  latest  EPA emission factors (through Supplement  14
        of AP-42).
     o Substituting  other NEDS point source data that more represent
        calendar  year 1980 for 12 states.
                                      15

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     o  Updating  fuel  type,  quantity and quality, source classification
        code  (SCO, control  equipment and efficiency, and boiler capa-
        city  for  electric  utilities that could be matched in  the Pechan
        unit  inventory  (1980)  and calculating updated emissions using
        AP-42 emission  factors.
     o  Updating  seasonal  throughput for all boilers matched  in the
        Pechcin  unit inventory  using FPC Form 4 data  for 1980.
     o  Adding  seasonal factors  for area source emissions by category.
     Subsequent updates which  resulted in Version 2.0 of the  1980  NAPAP
emissions  inventory  (12/30/83) include:
     o  Updating  copper smelters  to reflect SOX emissions in Work  Group
        3B  inventory  (1980) .
     o  Substituting  plants  in Northeast Corridor Regional Modeling  Pro-
        ject  (NECRMP)  inventory  (1980) for those in  NAPAP except for
        power plants  updated with Pechan data and plants that exhibited
        no  improvement  i.n  SOX  emissions.
     o  Incorporating  throjgh  Supplement 14 emission factors  in NECRMP
        data  substituted.
     o  Correcting several problems with previous power plant updates.
     Additional updates made to  the emissions inventory in generating
Version 3.0  (6/27/fa4)  include:
     o  Updating  power  plant SOX  emissions to be consistent with Pecha •>
        plant inventory.
     o  Correcting NAPAP  as  appropriate to eliminate the largest fuel
        discrepancies between  NAPAP arj DOE's State  Energy Data Report
        (SEDR).
     o  Updating  area sources  to  incorporate data for 15 counties  pre-
        viously omitted.
     o  Making  additional  power  plant updates for consistency with
        the Pechan unit inventory,  to add plants/units not previously
        matched,  and  to better identify plant names.
     o  Revising  incorrect SCCs  associated with fuel discrepancies and
        power plant changes.
     In creating  Version  4.0 of  the data base (9/18/84), the  improvements
made include:
     o  Adding  sulfate  and ammonia emission factors, control  device data,
        and emissions.
                                     16

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     o  Eliminating roundoff error present  in  earlier emission factor
        files for point sources.
     o  Incorporating emissions estimates for  point  sources/pollutants
        that had an emission factor but no  emission  estimate in the file.
     o  Adding latitude/longitude and/or Universal Traverse Mercator ( UTM)
        coordinates for all point sources.
After some additional processing to put the data  base in the format needed
b/ GCA, this version of the inventory was supplied to GCA for generating
Eulerian model input.
     Version 5.0, the final 1960 NAPAP emissions  inventory, was scheduled
tor completion by October 31, 1985.  The additional  updates being made to
create Version 5.0 of the data base include:
     •-j  Incorporating 1980 Canadian point and  area source emissions data.
     o  Substituting improved 1980 utility  data  from the NAPAP Utility
        Reference File.
     o  Adding chloride, fluoride, and  lead emission factors, control
        device data, and emissions,
     o  Performing a systematic quality control  check for important data
        base items to identify missing or anomalous  data and correct as
        appropriate using average or  typical  values.
     o  Updating area sourre data for highway  vehicles,  residential wood
        combustion, and onianic solvent use to reflect improved data/
        procedures  for calculating VOC emissions.
     o  Adding  total VOC emissions to  the  inventory  for  point and area
        sources  (previous emissions reflected  non-methane VOC only).
     Emissions  summaries of  the 1980 NAPAP  emissions data base are pre-
 sented  in this  section.  Table  1 shows  the  difference in emissions for
 the five  most  important pollutants from the four existing versions of
 the data  base.   Little difference exists between Versions 3.0 and 4.0  for
 SOX, nox,  and  VOC.   Table  2  indicates  that SOX emissions are dominated by
 electric  utilities,  primarily  from coal-fired generating stations in the
 eastern U.S.   For  NOX,  the  largest sources  are transportation  (mostly
 highway vehicles),  electric  utilities,  and industrial combustion.  VOC
 emissions result largely  from  miscellaneous sources   (including organic
 solvent use,  gasoline service  stations, and forest wildfires), transpor-
 taticn, and other  industrial processes.   The geographic  breakdown of SO
                                     17

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emissions  in Table  3  shows  that EPA Regions 5 and 4 are the largest con-
tributors, and  the  eastern  31  states  account for over 82% of total emis-
sions.  Regions 6,  5, and 4 are the highest NOX emitters, with the eastern
J1 states  accounting  for about 64%  of national emissions.  Regions 5,  4,
and 6 contribute  the  largest amount of VOC emissions, and the eastern 31
states account  for  about 66% of nationwide emissions.  Table 4 indicates
that nearly all VOC and about 6H%  of  NOX emissions are released below 120
feet.  Nearly 4U% of  all SOX is released above 480 feet.   Table 5 identi-
fies source category  contributions  to nationwide sulfate and ammonia emis-
sions.  Electric  utilities  and industrial point sources account for over
80% of the total  sulfate emissions  while area sources,  primarily manure
field application,  contribute about 80% of the total ammonia emissions.
Table 6 summarizes  Canadian emissions by source category and indicates
that electric utilities have much  less influence than in the United
States.   Smelters and area  sources,  however, are more significant emit-
ters in Canada.

                                CONCLUSIONS

     The  point  and  area source inventory represents year 1980 well with
over 80%  of emissions of SOX/  NOX,  and VOC having an indicated year of
record of  1980.   Virtually  all significant 3OX and NOX emitting plants
are included in the NAPAP point source file.  Outside of the NECRMP do-
main, the  completeness of the NAPAP point source file for VOC is likely
to be inconsistent  depending on the thoroughness of the states.  All
point sources have  location coordinates and reasonable stack data in
Version 5.0.
     Fuel  summaries from NAPAP Version 3.0 and the SEDR show reasonable
agreement  with  NAPAP  quantities being generally higher.  Differences in
Version 5.0 of  the  inventory are likely to be less.  Emissions data in
NAPAP Version 3.0 show reasonable  agreement with emissions in Trends and
Work Group 3B.  Some  comparisons may  improve when Version 5.0 of the in-
ventory is created.
     Version 5.0 of the NAPAP emissions inventory represents the best
detailed 1980 emissions inventory  presently available.

-------
                           Table 1
                National Summary of Emissions
        fron all Versions of  the 1980 NAPAP Inventory
                       ( 1 O3 tons/year)
Pollutant
   SOX
   NOX
   VOC
   S04
   NH3
 1 .0

27,916
22,905
22,582
                         Emissions  Inventory Version
 2.0

27,784
23,198
22,520
 3.0

27, 1 1 1
23,667
23,269
 4.0

27,222
23,833
23,307
   947
 4,250
                           Table  2
              NAPAP  Emissions  by Source Category
                       ( 106  tons/year)
    Electric  Utilities
    Industrial  Combustion
    Residential/Commercial  Combustion
    Non-ferrous Smelters
    Other Industrial  Processes
    Transportation
    Miscellaneous
    Total
                                        27.1
                                                NO
                                                       VOC
17.3
3.7
0.9
1 .2
3.0
0.9
0.1
8.1
4.5
0.7
Neg
1 .0
9.1
0.3
0.1
1 .0
0.1
Neg
4.5
8.0
9.6
                                               23.7   23.3
                              19

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                 Table  3

        NAPAP Emissions by  Region3
             ( 1 fl6 tons/yea r )
                                NOV      VOC
LPA Region 1            0.7      0.6      1.2
EPA Region 2           1.2      1.2      1.8
EPA Region 3           3.8      2.3      2.1
EPA Region 4           6.5      4.1      4.0
EPA Region 5           7.9      4.8      4.5
EPA Region 6           2.3      5.3      4.0
EPA Region 7           2.0      1.8      1.4
EPA Region 8           0.8      1.2      0,9
EPA Region 9           1.5      1.7      2.4
EPA Region 10          0.4      0.7      1.0
31 Eastern States5     22.3     15.1     15.3
Nation3	     27.1     23.7     23.3

d  Includes Continental  U.S.  only.
b  Includes tier of  staces  from Minnesota
   south to Louisiana  and all states east.
                 Table  4

 NAPAP Emissions by Release  Height Range
            (percent of  total)

     Range  (ft)    SOX     NOX     VOC
0-1 20
1 21-240
241-480
>480
Total ( 106
tons/year)
26
1 4
20
40

27.1
68
8
1 0
1 4

23.7
99
1
0
0

23





.3
                    20

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                        Table 5
            National Summary of Sulfate and
          Ammonia Rnissions by Source Category.
                    (1O3 tons/year)
                  Category
                                             Emissions
                                                    NH-
Point Source

     Electric Utility Boilers
     Industrial Boilers
     Commercial/Institutional Boilers
     Industrial Processes
     Total
Area Source

     Stationary Fuel Combustion
     Mobile Fuel Combustion
     Field Application of Manure
     Anhydrous Ammonia Fertilizer
       Application
     Beef Cattle Feedlots

     Total

Grand Total
448
172
 25
149
794
561
 63
  3
219
846
1 18
35
0
0
0
153
947
16
0
3,31 1
53
24
3,404
4,250
                        Table 6

    Summary of Canadian Bnissions by  Source Category
                    ( 1 O3 tons/year)

                               Pollutant Emissions
Source Category
Electric Utilities
Non-Ferrous Smelters
Other Industrial
Processes
Industrial Combustion
Area Source Stationary
Combustion
Transportation
Mi seel lane ous
Total
sox
844
1,507
1 ,754

21 3
577

151
65
5,111
NOX
235
	
114

34
31 3

1,181
259
2,1 36
voc
5
	
417

<1
52

878
2,231
3,583
SU4
18
29
87

6
43

5
1
189
NH3 Alkaline
15
— —
20 96

1
3

<1
<1 6,840
22 6,955
                            21

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      nFVELOPMFNT OF THE NAPAP UTILITY PFFERENCE FILE
                            by

     Edward H. Pechan, James H. Wilson, Kristin Graves
              E. H. Pechan & Associates, Inc.
                    5537 Henipstead Way
               Springfield, Virginia  22151
               EPA  Contract No. 68-02-4070
                   EPA Project Officer:

                      J.  David Mcbley
      Air and Energy Engineering Research Laboratory
           U. S. Environmental Protection Agency
       Research Triangle  Park, North Caroline  27711
                      Presented at:

Second Annual Acid Deposition Emission Inventory Symposium
                Charleston, South Carolina

                   November 12-14, 1985,
                             22

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         DEVELOPMENT OP THE NAPAP UTILITY REFERENCE FILE

    Edward H. Pechan,  James H. Wilson, Jr.,  and Kristin Graves
                 E.H.  Pechan & Associates,  Inc.
                            ABSTRACT

     Emissions from electric utilities account for a large share
of total acid  deposition precursor emissions.   The importance
of the utility industry has been recognized by NAPAP  through
many  of  the  activities of NAPAP1s  Task Group B  (Man-Made Sources),
which has sponsored work in both  developing estimates of current
emissions from  the utility industry and projecting  future emissions.
Different components of NAPAP have overlapping but not identical
dati needs; the  purpose of this  project was to develop a single
data  base  that  would  meet the  utility-related data  needs of
all NAPAP task  groups.  Because existing data files were inadequate
for  this  purpose,  Task Group B requested  that E.H.  Pechan &
Associates,  Inc.  (Pechan) develop  a single, comprehensive utility-
related  data  file.   This paper documents  the resulting  data
system,  designated  the NAPAP Utility Reference File  (NURF).

-------
         DEVELOPMENT OP THE NAPAP  UTILITY REFERENCE FILE
                          INTRODUCTION

     Different components  of  NAPAP have overlapping  but not
identical  data needs;  the purpose of this project was to develop
a  single  data base that would meet the uti1ity-related  data
needs  of  all NAPAP task groups.   Existing  data files developed
under  Task Group  B  sponsorship were inadequate  for  this purpose.
For  example, Version  4.0 of  the  ?.980  NAPAP emissions inventory
(Toothman,  1984),  between its point source and area  source compo-
nents, includes only anthropogenic sources of major acid deposition
precursor  pollutants  for that  year.  As another  example, the
Unit Inventory (Pechan, 1983) was developed to meet data requirements
of the Advanced Utility Simulation Model (AUSM);  the  Unit Inventory
contains unit-specific  information for only a  subset of generating
units,  however.   In response to  the needs  of  NAPAP, Task Group
B  requested that  E.H.  Pechan & Associates, Inc.  (Pechan) develop
a  single,  comprehensive utilitv-related data  file.  This data
base,  designated  the  NAPAP Utility Reference  File  (NURF), will
be used as an input  to  Task Group B utility emissions models.

                          DISCUSSION

     Figure 1 provides an  overview of  the NURF  data  system.
NURF  comprises four component files:  the master unit data file
(containing information on all electric  utility  generating units),
the fuel specific  emissions file (containing  emissions information
by fuel  and unit),  the stack parameters file  (containing  stack
information on a  unit-specific basis), and the announced unit
file (containing unit-specific information on units  coming on-line
or converting to  coal-firing after 1980).  In addition, as  shown
in Figure 1, three files were derived from NURF  and  made available
for distribution:  the NAPAP emissions inventory updates file
(containing corrections and addendums  to Version  4.0  of the
1980 NAPAP emissions inventory) ,  and  information for AUSM, including
a  1980 generating Unit Inventory  (an updated version  of the
existing  file containing unit-specific  information  on  larger
generating units  and  aggregated  information on smaller units)
and the  announced  inventory  (containing information  on units
coming on-line or  planned for conversion to coal  after 1980).

     NURF was  developed  using  information  from Version 4.0 of
the  1980  NAPAP  emissions inventory,  the Unit Inventory, and
new data;  additional  updates were  obtained from  a  variety of
sources.   Table 1  lists major data inputs to NURF.   In developing
NURF,  the  greatest  reliance was  placed on data available from
public sources,  especially files available in machine-readable
form.   A variety of  processing techniques were required to format

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                                                Figure 1

                                  OVERVIEW  OF NURF ELEMENTS
ro
CJl
                    NURF Component
                         Files
                      Master Unit
                       Data File
                     Fuel Specific
                     Emissions File
    Stack
Parameters  File
                       Announced
                       Unit  File
                                         NURF Derivative Files
                                                a




Input to 1 980
NAPAP Emissions
Inventory,
Version 5.0

1
Input to I 	
                                                       AUSM
                                                                          1 980 Generating
                                                                          Unit  iventory
                                                        Announced
                                                         Inventory
                        existing plants emitting S02, NO , or TSP

                        existing plants aggregated

                       cplanned plants (or conversions)
               Note:  The three NURF derivative  files were made available for distribution.

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                                                                        Table 1

                                                               Major Data Inputs to NURF
CT>
Mame
EIA Form 759
FPC Forr, 423
FPC Forn 6?
FGDIS
NAPAP Inventory
Generating Unit
Reference File
EPA State
Implementation
Plan file
NERC planned plants
NERC coal conversions
DOE coal conversions
Pechan nuclear plant
status
NO control update
AWL firing data
IX££i
A
A
A
A
A
A
A

M
M
M
M

M
A
Lfii'fiLj
Plant
°lant
Boiler,
Boiler
Boiler
Unit
Unit

Uni t
Unit
Unit
Unit

Unit
Url t
                                                                     tfLLiliil
Fuel consumption and genernticr,

Cost and quality of fuels

Fuels cor.surr.ed, control equipment,
firing typo, and tot ton type

SO- scruttor data

Stack para-^ters

Year online, year retired, capacity


TSP, SO   and NO  Emission
Limits          x


New plants

Plants converted or planning
conversion to coal

Plant: converted or planning
corversion to coal

Status of planned nuclear units
                                                                                       NO  control  measures

                                                                                       Suppl'vnental  data  on  firing  typ^s
                                                                                       and  botton  type
                            •ArAutonated

-------
the available  information from these sources into a single consistent
data system.

     Other data elements  (e.g.,  heat rate and  capacity  factor)
were simply not  available from standard sources and,  therefore,
had to be  calculated  from data  that were available.  For  those
cases in  which  the calculated values were unreasonable, judgements
were made as to which of the input values were the most accurate;
other data were  adjusted  on a unit-specific basis so that  all
resultant values were reasonable.

     Because of the wide range of  types of data processing required
to create  NURF, a combination of  programming languages and  meth-
odologies  was  used  in  its development.  Initial data reduction
of the larger  data  files  was performed by a series of programs
written  in Programming Language/I (PL/I).  These  larger  files
were reduced  to  one record per  unit  (or plant  if a plant-level
file).   The reduced files were converted to a  consistent  format
using the  Statistical  Analysis  System  (SAS).   These SAS  files
were then combined and manipulated using a series of  SAS programs.
Examples  of the processing  required include calculation of default
state average  fuel quality  data and assignment of plant technology
codes.   The result  of  these manipulations was  a final  NURF in
SAS format.   The  final processing steps converted the NURF data
in their  component  file form into the set of  derivative  files
which were discussed earlier.

     Development of NURF  was a multi-step process.  The  first
step  was to  identify  the universe  of units  to be included.
Because  the coverage of the major  contributing data files differs,
it was necessary to compare several data files on a plant-specific
basis in  order  to develop the best possible universe of  facilities.
Conflicts  between these files occurred in many cases.    These
had  to  be resolved on a  case-by-case basis.   In  cases  where
a conflict occurred,  if two or  more  files contained  consistent
information,  those data  were chosen.  Otherwise, preference
was given  to  the  U.S.  Department of  Energy's  (DOE)  1980 Form
67 data  (U.S. DOE,  1980b) and  the Generating  Unit Reference
File  (GURF --  U.S.  DOE,  1981b),  both of which  contain the most
recently  updated information for 1980.

     Operating characteristics  such as  total  generation  and
total fuels consumed  for  generation  were  obtained from  DOE's
Form 4 (U.S.  DOE, 1980a).  Form  4 is a monthly  data base;  for
use in NURF,  however,  the monthly data for 1980 were aggregated
into annual totals.   Form  4 data  are  reported by plant and  prime
mover.  For example, a plant having both  steam  and combustion
turbine  units would  have  fuel use and generation data provided
for each  of these two prime movers.

     Unit-specific  operational  data for  1980  were estimated
by applying 1980  unit  shares computed from 1980 Form 67 data
on fuel  use and generation to the corresponding data elements
from the 1980 plant  and prime mover  totals from Form 4.  This


                               27

-------
method was  adopted to correct erro-rs  associated with the  use
of incorrectly  reported units on Form 67 submissions.   Because
the Form  67  data  were used only to  compute shares of validated
totals, unit errors in Form 67 data were  not carried through
to NURF.

     Fuel quality  data were obtained  from the Federal Power
Commission  (FPC)  Fcrro 423  (U.S. DOE,  1981a).  For units with
no reported  Form  423 information, state average data  obtained
from Form  423 were  used.

                          CONCLUSIONS

     NURF is  a  central repository  of  data for  utility operations
and emissions,  making analysis of the  electric utility  sector
convenient.   The  largest sources of generated power and  sulfur
dioxide emissions have been thoroughly  covered.  In addition,
data on all  large  units  (including  fossil-fired, nonfossil-fired,
existing,  and planned) are provided  in a comprehensive manner.

     The major user files derived  from NURF are inputs to Version
5.0 of the 1980  NAPAP  emissions inventory and the 1980 generating
Unit  Inventory,  an  input  to AUSM.  Due  to data coverage  and
desired data base size considerations, both of these derivative
files  have  been segmented  into components  comprising large  and
small  generating  units.  The size cutoff  utilized in  the Unit
Inventory is more restrictive than  that used to update Version
4.0 of the 1980  NAPAP  emissions inventory because the Unit  Inventory
is used as  the  basis for projection of  emissions and  fuel  use
in AUSM;  detailed projections of the activity of smaller units
cannot reasonably be made.  For example,  the 1980 generating
Unit  Inventory  includes unit-specific data on only 30 percent
of all  fossil-fired units, while Version 5.0 of the 1980 NAPAP
emissions  inventory contains detailed  data on 62 percent of
all fossil-fired  units; because  the  units represented in  detail
in these  data files are the larger units, these files have more
extensive coverage  of generating  capacity, generation, and emis-
sions.  For  fossil-fired  generating  capacity, 92 percent of
the total  is represented in unit-specific  data in the 1980 generating
Unit Inventory and  96  percent of  the total is included in Version
5.0 of the  1980  NAPAP emissions inventory file.  Generation
and emissions coverage is  almost complete  for Version  5.0 of
the 1980  NAPAP  emissions inventory  file and is extremely high
(more  than 98 percent) for the 1980 generating Unit  Inventory.  Note
that the  Unit Inventory also includes  nonfossil units, which
are not included in  the NAPAP inventory-

     Table 2  provides some summary statistics  on NURF's  coverage
of generation capacity,  generation, and emissions, by  fuel  and
plant  type.   Fossil-fired units  account for more than 75 percent
of capacity  and generation,  and  100 percent  of emissions.   Table
2  also shows that the proportion of coal-fired generation is
larger than  the proportion of coal-fired capacity; the  opposite
is true  for  oil-fired units.  As expected,  coal-fired units


                                28

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                                                     Table 2



                                        Summary Statistics by Plant Type
Plant Type
Coal steam
Oil steam
Gas steam
Oil nonsteam
Gas nonsteam
TOTAL FOSSIL
Ifciclear
Hydroelectric
Other
TOTAL
Capacity % of
(W) Total
242,700 42
67,600 11
93,500 16
29,300 5
24,400 4
457,500 78
48,900 8
81,500 14
900 0
588,800 100
Generation % of
(TWh) Total
1,171,000 51
217,000 10
338,000 15
7,000 0
21,000 1
1,754,000 77
233,000 10
287,000 13
5,000 0
2,279,000 100
S02 % of
(10 3 tons) Total
	 — ^
16,070 91
1,320 8
120 1
10 0
0 0
17,520 100
0 0
0 0
0 0
17,520 100
NOX % of
(103 tons) Total
5,200 79
400 6
750 12
40 1
100 2
6,490 100
0 0
0 0
0 0
6,490 100
TSP % of
(103 tons) Total
570 88
60 9
20 3
3 0
2 0
655 100
0 0
0 0
0 0
655 100
Note:  Percentages calculated from detailed  data.

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account for  the majority of emissions.

     NURF was  compiled from every major publicly  available data
file.  By matching  and  combining this information,  the development
of NURF  gathered all  relevant  information into  one data file.
Discrepancies  that existed  in  the past between  data  bases are
resolved in NURF;  the result  is  a cohesive and  comprehensive
electric utility operations and  emissions data  file.  Because
NURF  is  a composite of the  best  data available  from  a number
of sources,  it does  not exactly match any other  individual file.
Aggregate measures of key variables are in excellent  agreement
with  published statistics,  however.  NURF is  important  as an
input to NAPAP's emission  efforts,  as well as an  important utility
operations data base  in its own right.

                           REFERENCES

Pechan,  1983:   E.H.  Pechan & Associates, Inc.,  "Electric Utility
Unit  Inventory:  Database Technical Documentation,"  prepared
for University  of  Illinois at Urbana Champaign,  May 1983.

Toothman,  1984: Toothman, Douglas A., John C.  Yates, and Edward
J. Sabo,  "Status Report on the Development of  the  NAPAP Emission
Inventory  for the 1980  Base  Year and Summary of  Preliminary
Data," EPA-600/7-34-091 (NTIS No. PB8b-167930),  December 1984.

U.S.  DOE,  198Ca:   U.S.  Department of Energy, "Monthly  Power
Plant Report,"  EIA-759  data file, 1980.

U.S.  DOE, 1980b:  U.S. Department of Energy,  "Steam-Electric
Plant Operation and Design Report," EIA-767 data  file, 1980.

U.S.  DOE,  1981a:   U.S. Department of Energy,  "Cost and Quality
of Fuels for Electric Utility  Plants," DOE/EIA-0075(80),  May
1981.

U.S.  DOE,  1981b:   U.S. Department  of Energy, "Inventory of Powf-r
Plants  in the  United  States:  December 1980,"  DOE/EIA-0348(83),
1984.
                                30

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         DEVELOPMENT OF AN EMISSIONS INVENTORY TO

         SUPPORT TESTING OF THE EULERIAN REGIONAL

                   ACID  DEPOSITION MODEL
                   Frederick M.  Sellars
                  GCA/Technology Division
               Bedford, Massachusetts   01730
               EPA Contract No. 68-02-3997
                        Task  No.  9
                   EPA Project Officer:

                     J. David Mobley
      Air and Energy Engineering Research Laboratory
           U.S.  Environmental  Protection  Agency
       Research Triangle Park, North Carolina   27711
                      Presented at:

Second Annual  Acid  Deposition  Emission  Inventory  Symposium

                Charleston,  South  Carolina


                   November  12-14,  1985
                           31

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                DEVELOPMENT OF AN EMISSIONS INVENTORY TO
                SUPPORT TESTING OF THE EULERIAN REGIONAL
                          ACID DEPOSITION  MODEL
                      by:  Frederick M. Sellars
                           GCA/Technology Division
                           Bedford, Massachusetts  01730
                                ABSTRACT

     One of the most extensive applications of the National  Acid
Precipitation Assessment Program (NAPAP) Emissions Inventory is to
support development and testing of the Eulerian Regional  Acid Deposition
Model (RADM).  To accomplish this, the 1980 NAPAP Emissions Inventory
had to be further resolved temporally, spatially, and by component
species.  Annual emissions had to be allocated to hourly for a typical
weekday. Saturday, and Sunday in each season; county-level  area sources
and minor point sources had to be spatially resolved to modeling grid
cells; NO  emissions had to be split into NO and NO,,; TSP emissions
had to be assigned to alkalinity classes; and VOC emissions had to be
apportioned into 30 photochemical reactivity classes.  To create the
NAPAP Eulerian Modeling Emissions Inventory, sets of temporal, spatial,
and pollutant species allocation factors were developed and applied to
the annual  data.  This paper present., a discussion of the processes,
assumptions, and data sources used to generate the 1980 NAPAP Eulerian
Modeling Emissions Inventory and presents results of that effort.
                                   32

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                DEVELOPMENT OF  AN  EMISSIONS  INVENTORY  TO
                SUPPORT TESTING OF THE  EULERIAN  REGIONAL
                         ACID  DEPOSITION MODEL
                              INTRODUCTION

     The 1980 NAPAP Emissions  Inventory  contains  annual  emissions from
point and area sources,  with area sources compiled on a  county basis.
To support testing and development of the Eulerian Regional  Acid
Deposition Model  (RADM):

     •    annual  emissions had to be further resolved to hourly values;
     t    county-level area source data  had to be spatially  allocated to
          grid cells;
     •    NOX emissions  had to be split  into NO and N02J
     •    TSP emissions  had to be assigned  to alkalinity classes; and
     •    VOC emissions  had to be assigned  to photochemical  reactivity
          classes.
To create Version 5.2 of the 1980 NAPAP  Eulerian  Modeling Emissions
Inventory, sets of temporal, spatial,  and pollutant species  allocation
factors were developed and applied to  the annual  data contained in the
1980 NAPAP Emissions Inventory.   Development of a more efficient and
flexible data handling system, the Flexible Regional  Emissions Data
System (FREDS), was also required.   Development of the 1980  NAPAP
Eulerian Modeling Emissions Inventory, the  associated allocation
factors, and the  data handling system  is discussed below.
                                  33

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                               DISCUSSION

Temporal Allocation
     Temporal allocation of the NAPAP emissions data was accomplished by
applying a set of seasonal, daily, and hourly fractions to the annual
emissions totals to generate hourly emissions values for a typical
weekday, Saturday, and Sunday in each season.
     For area sources, temporal allocation factors were derived based on
oublished activity statistics (e.g., heating degree days, gasoline
Sales,  air traffic activity).  Where such data were unavailable,
patterns for similar studies were utilized or engineering judgement was
employed.
     For electric utilities in the Eastern United States, State and SCC-
specific hourly temporal factors were developed based on hourly power
plant  fuel use data previously collected for use  in EPRI's SURE Program.
The  SURE data were also used to derive SCC-specific patterns for the
rest of the  United States.  For other point  sources, point-specific
patterns were derived based on operating rate information contained in
the  annual inventory records.
     Since the NAPAP study area spans several time zones, temporal
allocation factors were adjusted to represent Greenwich Mean Time.
Adjustments  were alsf; made to reflect Daylight Savings Time during the
appropriate  seasons in applicable areas.
Spatial Allocation
     The NAPAP modeling grid system (Version 5.2) is comprised of 63,000
grid cells (210 rows, 300 columns) dimensioned 1/6° latitude by 1/4"
longitude (approximately 20 x 20 km).  Point source records in the NAPAP
Emissions Inventory contain locational information making their
assignment to grid cells straightforward.  Area source emissions are
allocated from counties to grid cells using  spatial allocation factors,
fractional multipliers that assign a portion of each county's emissions
to a particular grid cell.  Generally, since the  subcounty distribution
of emissions is unknown, emissions are apportioned on  the basis of the
known  distribution of some surrogate indicator.
                                    34

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     Spatial allocation factors were derived for population, housing,
 total land area, 10 land use classifications, and 1  composite land use
 category.  Population and housing counts from the 1980 Census were
 obtained by enumeration district.  Spatial  allocation factors were
 created for those two surrogates by assigning populations and housing
 units to grid cells based on the location of the centroid of each
 enumeration district.
     Land use data, derived from Landsat mosaic images, were obtained
 and  contain 10 land cover/use percentages for each NAPAP grid cell.
 These land use percentages were utilized with grid/county land area
 relationships to derive spatial allocation factors.   The final step in
 spatially allocating county-level emissions to grid cells was to assign
 the  most appropriate of the 14 possible surrogates to each of the 88
 area source categories.
 Species Allocation
     To be used in the RADM, three of the pollutants in the NAPAP
 Emissions Inventory. NO , TSP, and VOC, had to be further refined.
 NO   emissions had to be split into NO and NO,,, TSP emissions
 assigned to alkalinity classes, and VOC emissions broken down by
 photochemical reactivity class.
     Profiles of NO  emissions, referenced by Source Classification
                   A
 Code (SCC), were developed using patterns previously derived for the
 SURE and Northeast Corridor Regional Modeling Project (NECRMP)
 inventories.  Since the modelers desire the flexibility to test a number
 of different chemistries,  a more complex approach was necessitated for
 VOC  emissions.  Using primarily published information, a set of species
 profiles were developed.   Each profile provides a breakdown of a
 category's VOC emissions  into a typical  set of component species.  By
 distributing emissions to  individual species, the profiles become
 independent of any reactivity scheme,  providing the flexibility desired
 by the modeling  community.   To "speciate" emissions, two additional
 files were employed.   First,  the SCC Index  File matches each SCC with
 the most appropriate  profile.   Next, the Class Assignments File assigns
each of the  160  species contained in the profiles to one of the 30
photochemical  classes  specified by the modelers.  Alkaline dust emission
                                    35

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     Spatial  allocation factors were derived for population,  housing,
total  land area, 10 land use classifications, and 1  composite land use
category.  Population and housing counts from the 1980 Census were
obtained by enumeration district.  Spatial  allocation factors were
created for those two surrogates by assigning populations and housing
units to grid cells based on the location of the centroid of  each
enumeration district.
     Land use data, derived from Landsat mosaic images, were  obtained
and contain 10 land cover/use percentages for each NAPAP grid cell.
These land use percentages were utilized with grid/county land area
relationships to derive spatial allocation factors.   The final step in
spatially allocating county-level emissions to grid cells was to assign
the most appropriate of the 14 possible surrogates to each of the 88
area source categories.
Species Allocation
     To be used in the RADM, three of the pollutants in the NAPAP
Emissions Inventory, NO  , TSP, and VOC, had to be further refined.
NO  emissions had to be split into NO and NOp, TSP emissions
assigned to alkalinity classes, and VOC emissions broken down by
photochemical reactivity class.
     Profiles of NO  emissions, referenced by Source Classification
                   A
Code (SCO, were developed using patterns previously derived  for the
SURE and Northeast Corridor Regional Modeling Project (NECRMP)
inventories.   Since the modelers desire the flexibility to test a number
of different chemistries, a more complex approach was necessitated for
VOC emissions.  Using primarily published information, a set  of species
profiles were developed.  Each profile provides a breakdown of a
category's VOC emissions into a typical set of component species.  By
distributing emissions to individual species, the profiles become
independent of any reactivity scheme, providing the flexibility desired
by the modeling community.  To "speciate" emissions, two additional
files were employed.   First, the SCC Index File matches each  SCC with
the most appropriate profile.   Next, the Class Assignments File assigns
each of the 160 species contained in the profiles to one of the 30
photochemical classes specified by the modelers.  Alkaline dust emission
                                     35

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factors were used to  develop  allocation  factors  to  apportion TSP into
five alkalinity classes.   A list  of  species  contained in  the NAPAP
Eulerian Modeling Emissions Inventory  is  provided  in  Figure 1.
Eulerian Modeling Files
     In addition to development of allocation  factors to  address the
above requirements, a data handling  system capable  of creating  subsequent
versions of the NAPAP Emissions Inventory has  been  developed.   The
Flexible Regional Emissions Data  System  (FREDS), consisting of  six
primary independent subsystems written in the  command language  of the
Statistical Analysis  System (SAS), is  being  used to preprocess  EIS
formatted emissions data  for  use  in  regional scale  atmospheric
simulation modeling.   The function of  each module  and its relationship
to the system as a whole  are  presented in Figure 2.
     In addition to preprocessing annual  emissions  data in Emissions
Inventory System (EIS) Master File format and  allocating  these  emissions
by time, pollutant species, and location, FREDS  calculates emissions
uncertainty at any given  level of temporal,  species,  and  spatial
allocation.  For example, percent error  values can  be assigned  to annual
emissions which have  not  been allocated  in space,  time, or by pollutant
species.  On the other hand,  the  percent  error values can be assigned
for SCC level emissions which have been  fully  allocated.

                                 RESULTS

     Hourly emissions of  S0x, N0x> VOC,  and  NH3  for a typical
summer weekday, nationwide, are shown  in  Figure  3.  Figure 4 shows the
distribution of VOC emissions by  reactivity  class  as  a function of time
for a typical summer  weekday. Spatial distribution of SO  emissions
for 1600 Greenwich Mean Time  of a typical summer weekday  is depicted in
Figure 5.   (Note that, for ease of interpretation,  each grid cell
depicted in Figure 5  actually represents  24  of the  NAPAP  grid cells.)
                                   36

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                               CONCLUSIONS

     An emissions data base with the spatial, temporal, and species
resolution necessary to support development and testing of the
Eulerian Regional Acid Deposition Model (RADM) has been developed.
A corresponding data handling system, which addresses the extensive
requirements of the RADM, has also been developed and provides
substantial improvements in efficiency over the predecessor system.
                                  37

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TEMPORAL RESOLUTION:
GEOGRAPHIC DOMAIN/RESOLUTION:
POLLUTANTS
Hourly emissions values for a typical
weekday, Saturday, and Sunday for all
four seasons
48 States and Canada; separate
major point source file with minor
point sources and area sources
assigned to 63,000 20 x 20 km
grid colls
SO,
so4
TSP:
 - Ca
 - Mg
   K
 - Na
Pb
CO
HC1
HF
NO
N02
NH3
VOC:
 - Methane
 - Ethane
 - Ethylene
 - Propane
 - Propylene
 - N-butane
 - 1,2-butene
 - Isobutane
VOC (cont.)
 - Isobutene
 - Trans-2 butene
 - Pentane
 - Isopentane
 - 2,3-dirnethyl butane
 - Other alkenes
   Other alkanes
 - Formic acid
 - Acetic acid
 - Other organic acids
 - Formaldehyde
 - Acetaldehyde
 - Propionaldehyde
 - Acetone
 - Other ketones
 - Other aldehydes
 - Xylene
 - Benzene
 - Toluene
 - Ethyl benzene
 - Other aromatics
        Figure 1.  Contents of the 1980 NAPAP Eulerian Modeling
                   Emissions Inventory.
                                   38

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                        ANNUAL EIS
                      EMISSIONS DATA
               MODEL DATA EXTRACTION MODULE

Accepts EIS formatted annual emissions data and extracts
pertinent information only.  A SAS data file is created
for each user-defined industry group.  Separates major
point sources from minor sources and area sources based
on user-designated size cutoffs.
                             l
                TEMPORAL ALLOCATION MODULE

Matches each emission record with the appropriate set of
seasoi al, daily, and hourly temporal allocation factors
from  the Temporal Allocation Factor File.  Where a pattern
is not supplied, one will be generated based on operating
hours data contained in each EIS record.
                     SPECIATION MODULE

Matches each emission record with the appropriate set of
speciation factors contained in the Speciation Factor File.
Can provide 30 subspecies each for up to 15 pollutant
categories.  Resolves NO- into NO and NO;?, TSP into
alkalinity classes, and VOC into reactivity classes for NAPAP.

                 SPATIAL ALLOCATION  MODULE

Assigns point sources to grid cells based on latitude/
longitude.  Assigns area sources to grid cells using
spatial allocation factors based on surrogates (e.g.,
population, housing, land use) and matchings of area
source categories to most appropriate surrogate indicators.
                             i                         ~~	
                    UNCERTAINTY MODULE

Calculates estimates of uncertainty associated with the
emissions data and corresponding temporal, spatial, and
species allocation factors.
                             i
              NAPAP MODEL INPUT PREPROCESSOR

Accepts SAS emission records into which allocation factors
have been merged.  Applies allocation factors to emissions
as designated by the user.  Sorts and reformats as required
by the Regional  Acid Deposition Model (P.ADM).
    Figure 2.  Major components of the Flexible Regional
               Emissions Data System.
                            39

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  Q
CO Z
UJ <
  CO
           a  SOX
        i   +  NOX
           o  voc
           A  NH3
        t * ^
        >"**-** *
-------
            AJ.KANES  •_, ALKtNES
          :•? kCTHANE  & ORQAMC ACOS
0)
u
J
t~~,
s .
• 'I--.
-~."

c^rTi
• 'r ^ r - * ' *<
* *• • * '* *«
i". r-\ •"; p •; — •".
^rU-iH":!-
r~i
l ' „
; -«
                        (i  ^ 1 0 I I i z 1 1 I t 1 1 It, ' "• ! a 1 9 i<-' 21 ^2 2} 21
               HOUR (GMT) TYPICAL SUMMER WEEKDAY
      Figure 4.  Diurnal VOC distribution by reactivity  class  for a

                typical summer weekday, contiguous United  States.
                                 41

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LEGEND: SOX LHJ<5   iSiSSI 5-20
-20
       Figure 5.  SOX emission density (g-moles/hr/km2),
                 1600 GMT for a typical  summer weekday.

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   UNCERTAINTY  ANALYSIS  OF NAPAP EMISSIONS INVENTORY
                   Carnen M.  Benkovltz
              Brookhaven  National  Laboratory
                Upton. New York   11973


        EPA  Interagency Agreement  No.  DU89930122-01-1


                    EPA Project  Officer:

                      J.  David  Mobley
       Air and  Energy  Engineering  Research Laboratory
            U.S.  Environmental  Protection Agency
              Research Triangle  Park,  NC   27711


                  U.S. DOE Project Officer:

                      Edvird  C.  Trexler
                       Fossi1  Energy
                  U.S. Department  of  Energy
                  1000 Independence Ave.  SW
                    Washington,  DC 20460
                       Presented  at:

Second Annual Acid Deposition  Emission  Inventory  Symposium
                      Charleston,  SC
                   November  12-14,  1985
                                43

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              UNCERTAINTY ANALYSIS OF  NAPAP  EMISSIONS INVENTORY

                             Carmen M.  Benkovitz
                       Brookhaven National Laboratory
                                  ABSTRACT

     A major goal of Task Group B is  the  development  and  maintenance of
detailed inventories of anthropogenic emissions  to  support  acid deposition
research.  Estimates of the uncertainties of  the  emissions  values are an
integral part of any inventory developed.   Detailed  quantification of these
uncertainties in the scale required by NAPAP  researchers  has  never been
attempted before.  Methods used to estimate emissions  were  studied, and sta-
tistical methodologies were derived which will provide  the  best estimate of
the uncertainties associated with these emissions values.   These methodolo-
gies do not rely on any assumptions as to the statistical properties of the
data needed to quantify the emissions uncertainties.  Auxl'iary data needed
to estimate the uncertainties have been identified.  A  basic  framework com-
puter software has been developed to allow the calculation  of  the uncertain-
ties associated with the emissions values in  the NAPAP  inventory.  A work-
shop was held during which expert opinion was solicited, and  the Delphi
method was applied to arrive at quantitative estimates  for  the  auxiliary
data needed to calculate the uncertainties of emissions values  for the NAPAP
i960 base year.   Statistical formulations have been developed  to incorporate
these data into  the  methodologies selected to estimate  the  uncertainties
associated with  the  emissions  values.   Development of the computerized data
base and calculation of the  emissions  uncertainties are proceeding.   Meth-
odologies are  being  developed  for the  use of  expert opinion to  generate the
auxiliary data  needed to calculate  emissions  uncertainties  for  the NAPAP
1985 base year.   Calculation  of  the  1985  base year uncertainties  is  expected
to follow the  1985 data base development.
                                      44

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                                 INTRODUCTION

     A  major  goal  of  Task  Group  E  is  the development and maintenance of
detailed  inventories  of  anthropogenic emissions to support both assessment
of  the  effects  of  acid  deposition  and the development, evaluation, and use
of  long range  transport  and  transformation models for acid deposition
research.   Estimates  of  the  uncertainties of the emissions values are an
integral  part  of  any  inventory  developed.  The  objectives of this project
are:

      1.   To develop  a methodologies framework to assess the uncertainties
associated  with the  emissions  data as presented in the NAPAP emissions
inventory.

      2.   To develop  and  implement  a prototype software package to calculate
the  uncertainties  associated with  the emissions values of the NAPAP emis-
sions  inventory.

      3.   To develop  the  data base  needed to calculate the uncertainties
associated  with the  values for  the 1980 base year emissions.

      4.   To develop  the  data base  needed to calculate the uncertainties
associated  with the  emissions  values  for the 1985 base year.
                                  DISCUSSION

      The  NAPAP  emissions  inventory  was based on the National Emissions Data
 System  (NEDS)  currently operated by the Office of Air Quality Planning and
 Standards (OAQPS)  of  EPA.   NEDS  provided the basic data froir which all other
 levels  of aggregation or  disaggre^ation will be calculated.  The basic NEDS
 data  are  statistical  averaged  parameters which allow the calculation of
 yearly  emissions  of  the five  criteria  pollutants (particulates,  SOX,
 NOX,  hydrocarbons, and  CO)  on  an individual source/process basis for point
 sources and  on  a  county level  for area sources.  Current plans call for the
 application  of  spatial,  temporal,  and  species disaggregation algorithms
 which will be  based on  disaggregation  factors (or modifications  thereof)
 developed for  the  Northeast Corridor Regional Modeling Project (NECRMP).
 Higher  levels  of  aggregation will be calculated as sums of the basic NAPAP
 data.

     For  each  individual  point source/process, yearly emissions  are esti-
 mated using  one of the  following methods:

     1.   Stack  tests  or other  emission measurements

     2.   Material  balance

     3.   Calculated using federal  (AP-42)  emission factors, where emission
 factors are  the rate  at which  a  pollutant  is released as a result of •rme
activity
                                         45

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     4.   Guess

     5.   Calculated using special emission factors.

     Emissions estimated using Methods 3 and 5 are calculated using  the
equation:


     EM =   E  (EF1)(A1)(Fl)  (O                                      (1)
           i=l

where
     EM  = total emissions from a point source of a given pollutant
      P  = number of processes contributing to emissions from point  source

     EF^ = emission factor for process i
      AJ = ash or sulfur content of fuel used by process i  (if appropriate)

      Fj = material or fuel throughput for process i

      C  = (1-control efficiency of control equipment) for  a given pollutant

     Yearly emissions for area sources are calculated by geographic  county
using th'i equation:


     EMC =  E  EMa =  T.  (EFa) (Aa) (ACa) (ADa)                           (2)
           a=l       a=l

where

     EMC = area source emissions for county c

      A  = number of activities contributing to emissions in county  c

     EMa •» area source emissions from activity a for county c

     EFa = area source emission factor for activity a (this parameter can
also be  county specific)

      Aa - ash or sulfur content of fuel used in activity a (if  appropriate)

     ACa  = appropriate measurement of level of activity a  in county c

     ADa = adjustment factor for area source category

     Several previous projects have addressed the problem of assigning,  in
statistical terms, quantitative values to the errors in emissions data.
Final reports from the following projects were reviewed.
                                        46

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      1.  Weighted  Sensitivity Analysis of Emissions Data, project conducted
         by  IBM  Corporation under contract to the Office of Air Quality
         Planning  and Standards (OAQPS), EPA, July 1973.

      2.  Source  Inventory and Emission Factor Analysis (SIEFA) project con-
         ducted  by PEDCo - Environmental Specialists, Inc., under contract
         to  OAQPS, September 1974.

      3.  Emissions Inventory for the SURE Region, project conducted by GCA
         Corporation under contract to the Electric Power Research Institute
         (EPRI). April 1981.

      4.  Emissions,  Costs and Engineering Assessment, Work Group 3B,
         US-Canada Memorandum of Intent (MOI) on Transboundary Air Pollu-
         tion,  June 1982.

      5.  Preliminary Evaluation of  Acidic Deposition Assessment Uncertain-
         ties,  project conducted by Argonne National Laboratory (ANL) under
         contract  to the U.S. Department of Energy, November 1982 (prelimi-
         nary  report).

      All these  projects have based  their calculations on the statistical
 formulas for error propagation as derived for "small" values of the errors;
 i.e.,  the  Taylor series expansion included only the first derivatives of the
 function.   Some  of the error values used in subsequent calculations have
 been  as high as  80-90% of the mean.

      In calculating  the mean squared error of emissions estimated such as
 those  above, we  take the stance that the component parts of each expression
 are  themselves  estimated, and that  these component estimates have known (or
 estimable)  expected  values and variances.  Further, the estimation errors of
 the components  are independent of one another.  The mean squared error of
 the emissions  estimate then follows from simple formulas giving variances of
 algebraic  combinations of random variables;  e.g., for N independent random
 variables  U^,...,  UN:

                                     = £V(Ui)                           (3)

                              n E2(Ut) + V(Ui)  - uE2                  (4)

     Since  the  errors  of estimation are presumably independent across geo-
 graphic space,  the mean squared error of the  estimate of an aggregate is
 simply the  sum  of  the  mean squared  errors of  its components.

     The second  objective of this project addresses the design and implemen-
 tation of  the basic  framework of computer software needed to calculate
 uncertainties associated with yearly emissions values for both point and
 area sources.  The conceptual .-sign is independent of the software system
 used to support  the  NAPAP inventory;  the design and implementation of the
 software modules will  allow portability between computer systems and will be
as independent as  possible of the current NAPAP inventory software system.
Outputs generated  by  this software  include values for the uncertainties of
                                         47

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emission, at the point, plant, county, state, or national  level  for  point
sources and at the couaty, state, or national level for area  sources.

     Uncertainty values associated with each parameter used  in  calculating
emission values are expected  to be applicable to whole  classes   of  these
parameters rather than just to individual sources.  To avoid  needless
repetition of data (with  the  associated increase in storage  costs and  the
ever present danger of errors at update times), a file with  uncertainty
"profiles" was designed.  When the data are developed, this  file will  con-
tain ail the variance information needed to calculate  the  uncertainty  value
associated witl. the yearly emissions of a point source or  an  area source
category.  Each uncertainty profile will be identified by  a  unique code; at
retrieval  time the appropriate uncertainty profiles can be referenced  to
allow  the  calculation of  uncertainty values associated with  the  reported
emissions.  Figure I presents a  schematic of this design.

     Given the wide range of  elements  requiring uncertainty  estimation for
eventual use in estimating the uncertainty of the emissions  values in  the
1980 NAPAP Emissions Inventory,  the use of a panel  of  experts was considered
as an  approach to begin the task of building the data  base needed to perform
these  calculations.  As the initial activity of Objective  3  for this
project, an uncertainty workshop concept was formulated to convene a panel
with expertise in many of  the elements  included in  an  emissions inventory
uncertainty analysis.  The 1980  NAPAP  Emission Inventory Uncertainty Work-
shop was held at  the EPA  Air  and Energy Engineering Research Laboratory,
Research Triangle Park, North Carolina, on May 7, 1985.  The  panel was
queried  on individual  uncertainty estimates  for the elements  discussed above
which  are  part of  the  emissions  estimation process.  The Delphi technique
was applied to elicit  the experts' opinions  in a systematic  manner leading
to useful  results.  This  technique involves  iterative  questionnaires admin-
istered  to individual  experts; feedback of results  accompanies  each itera-
tion of  the questionnaire.  This process continued  until a convergence of
opinion  was reached.  The end product  is the consensus of  experts, including
their  commentary, on each of  the questionnaire items.
          NAPAP Emissions
          Inventory
          Data Files
          Uncertainty
          "Profiles" File
                                                 Emissions Reports
                                                  -  emissions values
                                                  -  uncertainty values
                                  Figure  1
                  Software to Calculate Uncertainty Values
                                         48

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     For each  uncertainty  value desired, the workshop participants were
asked  to estimate  p  in  the statement:   "90% of the data fall within p% of
the mean."  Table  1  summarizes the results of the workshop.

     To allow  the  use  of  the values developed in the workshop with Equations
(3) and (4)  the  concept of "fractional error" was developed.  Suppose 9 ~ N
(9, a ) so  that the quoted  phrase above is equivalent to:

                      Pr f (l-p) 9 <_ 9 _< (1+p) 01  - 0.9

              zo
that is, p = — where,  for the normal  distribution, z - 1.6448.  We call p

the "fractional  error  associated with  *} as an estimate of ^ . "

     Fractional  errors  may be developed for algebraic combinations of inde-
pendent random variables  as follows:

                        N             2                 N
                                   >        for X -   T.  Vl            (5)
         1-i            1-1                           i-l

                N                                      N
      P2  -  z2    n   (1  + k2P2.)  -L            for X -   n  I'l             (t>)
               i-1          bl                         i-l

      (Note that the  relation  between p and the variance depends on the
normal assumption, and also that the product of normal random variables is
not  norma I. )

      Table 2  presents the distribution of confidence rating values of the
point source  emis'lon factors  by pollutant.   Uncertainty profiles were
developed  based on  the Delphi  results, and a subset of the NAPAP I960 base
year  Version  3  major  point source  file was used to perform initial calcula-
tions.   The  subset chosen Included data for  the state of Delaware and for
the District  of Columbia.  Preliminary results Indicate that, for annual
point source  emissions,  calculated uncertainties are in the range of 20-100%
for  individual  point  sources and in the range  5-14% at the state level.
Uncertainty  profiles  for annual emissions from area sources are currently
being developed; uncertainty calculations will follow.

     The use  of expert teams will  be extended  in Objective 4 of this pro-
ject.  A draft  plan for  the development of the uncertainty values for the
1985 data  base  has been  prepared.   A finer breakdown of source categories
and an increased number  of pollutants are to be considered in the 1985 base
year exercise.  Four  expert teams  have been  identified; these teams will
address  the utility,  industrial combustion,  Industrial processes, and trans-
portation  sectors.  Expert opinion will be obtained via individual inter-
views using  the most  appropriate formulation of probability encoding tech-
niques.   A classical  statistical approach will be followed -- explicit
specification of an underlying  model followed  by derivation of the problem
                                         49

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                           Table 1
Proposed Uncertainties for the NAPAP 1980 Base Year Inventory
Uncertainty Range (%)

Parameter
Fuel S content
Point source emission factors
Method 1 (stack tests)
2 (material balance)
3 (AP-42 emission factors)
confidence rating A
B
C
D
E
5 (state emission factor)
4,6,7,0 and blank
Point source production throughput
Control equipment efficiency
Area source emission factors
Mobile sources
"Other" sources
Area source activity level
Mobile
Other
Point source temporal apportionment
Seasonal profiles
Dally profiles
Hourly profiles
Area sources temporal apportionment
Seasonal profiles
Daily profiles
Hourly profiles
Area sources spatial apportionment factors
Chemical speciatlon factors
N0/N02
voc

SOX


25
10

10
25
50
75
100
25
100
15
25

*
25




10
25
50

10
25
50
25



•Apply same criteria as for point source emission

NOX


25
25

10
25
50
75
100
50
100
15
25

50
25




10
25
50

10
25
50
25




VOC


25
50

10
25
50
75
100
50
100
15
25

100
100




10
25
75

10
25
75
25



Across all
Pollutants
10

















25
25










25
100
factors.
                                 50

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                                 Table 2



Emission Factor Confidence Level (from EIS Point Source Emission Factor File)


I
1 I
I
2 I
I
3 I
I
41 27 I
I
5 I I 8
I
I 	 I....
0 10
PERCENT

I
1 I
I
2 I
I
3 I
I
41 18 I
I
	 +
5 I I 6
I
I 	 I....
0 8
PERCENT
(
PERCENT 1
Sulfur Oxides

134 I 40.6

90 I 27.3

71 I 21.5

8.2

2.4

	 I 	 I 	 I 	 I
20 30 40 50

Nitrogen Oxides

104 I 34.7

88 I 29.3

84 I 28.0

6.0


2.0

	 I 	 I 	 I 	 I
16 24 32 40

                                                              CUMULATIVE
                                                            (Continued)

-------
Table 2(continued)
                                                               CUMULATIVE
                             	PERCENT	PERCENT	
                     Volatile  Organic Compounds
                                                        14.8     14.8
  I

II          111 I
  	+
  I
  	,	+
21                                           369 I    49.1    63.9
  	,	.	•».
  I

31                  172 I                              22.9    86.8
  	+
  I

41       83 I                                         11.1    97.9
  — — — — — —	=• — •*•
  I
  —+
5 I I 16                                                2.1   100.0

  I
  I	I	I	I	I	I
  0        10        20        30        40        50
  PERCENT
                                            52

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solution ii"der  the  assumptions  of  the  model.   Towards this end,  a documenta-
tion packet is  being  compiled  to  be  sent  to  participants on expert teams
prior  to the  interviews.   All  appropriate  definitions,  assumptions,  and
statistical questions  will  be  addressed  in the packet.
                                  CONCLUSIONS

     Strict  estimation  of  the  uncertainties associated with the emissions
values as  presented  in  the  NAPAP  emissions  inventory requires  the explicit
specification  of  the  sources  of  uncertainties in each method used to esti-
mate  these emissions  and  of the  underlying  statistical model and assumptions
to  be  used in  estimating  the  desired uncertainties.   The development of the
auxiliary  data  needed for  the  calculation of  uncertainties associated with
the  1980  base  year  emissions  had  to be  carried out within restricted time
and  resource bounds.  This  exercise provided  a basic framework within which
to  refine  the  techniques  being developed to estimate the uncertainties of
the  1985  base  year  emissions.
                                 BIBLIOGRAPHY

 Benkovitz,  C.M.,  "Framework for Uncertainty Analysis of the NAPAP Emis-
      sions  Inventory,"  EPA-600/7-85-036,  NTIS-PB86-112570 (September 1985).

 Ditto,  F.H.,  L.T.  Gutierrez,  T.H.  Lewis,  and L.J.  Rusbrook.  Weighted Sensi-
      tivity Analysis  of Emissions  Data:  Volumes I and II.   EPA-450/3-74-022
      a  and  b,  NTIS-PB258413 and 258414, 1973.
Klimm,  H.A.  and  R.J.  Brennan.
      EPRI-EA-1913,  1981.
Emissions Inventory In the SURE Region.
Knudson,  D. ,  M.  Davis,  J.  Shannon,  D.  Sisterson,  S.  Viessman,  M.  Wisely, and
     R. Whitfield.   Preliminary  Evaluation of Acidic Deposition Assessment
     Uncertainties.   ANL/EES-TM-XXX (Draft),  1982.

Office  of  Air Quality Planning  and  Standards, U.S.  Environmental  Protection
     Agency,  "Compilation  of  Air Pollutant Emission  Factors,"  third edition
     (plus  supplements  8-15),  AP-42,  NTIS-PB275525  (1977).
Office of Air Quality  Planning  and  Standards,  Environmental Protection
     Agency.  Source Inventory  and  Emission Factor Analysis.   Volumes I
     II, EPA-450/3-75-082  a  and b,  NTIS-PB247743 and 248829,  1974.
                                         and
Rivers, M.E. and K.W. Rit;j«fcl  (Eds.).   Emissions,  Costs and Engineering
     Assessment Work Group  3B.   United  States-Canada Memorandum of  Intent
     on Transboundary Air Pollution,  1982.

Toothman, D.A. , Yates, J.C. and  Sabo,  E.J.,  "Status Report on the Develop-
     ment of the NAPAP Emission  Inventory  for the 1980 Base Year and Summary
     of Preliminary Data,"  EPA-600/7-84-091,  NTIS-PB85-167930 (December
     1984).
                                        53

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         SESSION  2:  DEVELOPMENT OF NAPAP EMISSION  INVENTORIES  FOR
                          ANTHROPOGENIC SOURCES  (continued)

Chairman:   John Bosch,  Chief
           National Air Data Branch
           U.  S.  Envircnmental Protection Agency  (MD-14)
           Office of Air Quality Planning and Standards
           Pesearch Triangle Park, NC  27711
                                    54

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APPLICATION OF THE NAPAP EMISSIONS INVENTORIES TO EULERIAN MODELING
                                 By

                           Joan H. Novak
              Atmospheric Sciences Research Laboratory
                U.S. Environmental Protection Agency
            Research Triangle Park, North Carolina 27711

                                and

                         Paulette Middleton
              National  Center for Atmospheric Research
                           P.O. Box 3000
                      Boulder, Colorado 30307
                           Presented at:


     Second Annual  Acid Deposition Emission Inventory Symposium

                           Charleston, SC


                        November 12-14, 1985
                                  55

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                                 ABSTRACT



     This paper presents the  schedule  for development and evaluation  of

Eulerian Acid Deposition Models as part of the National Acid  Precipitation

Assessment Program and  discusses  the critical need to reduce uncertainties

in emissions  inventories  to  provide  more  reliable  modeling  results  for

policy decision  making.   A  strong  recommendation   is  made  to  expand,

improve, and standardize quality  assurance procedures  for  emission inven-

tory development  and  to  incorporate  knowledge  gained  through  modeling

sensitivity studies in  ranking emissions inventory development activities.
                                INTRODUCTION



    One of the primary goals of the National Acid  Precipitation Assessment

Program (NAPAP)  is  to develop a  comprehensive  Regional  Acid  Deposition

Model  (RADM)  suitable for assessing source-receptor relationships.   RADM

also forms the  scientific basis  for  development  of a  series  of  simpler

"engineering  models" useful  for addressing policy and  assessment  questions

NAPAP  has  established the following schedule  for development  and  evalua-

tion of these Eulerian acid deposition models.


   February  1986     Preliminary  Evaluation of the  First  Generation
                     Regional  Acid  Deposition Model  (RADM)

   October 1986       Testing dnd  Preliminary Assessment of  a sulfur
                     deposition Engineering Model
                                   56

-------
   October  1987       Testing  and  Evaluation of  an  Advanced  Engineering
                      Model  Operational  For Multiple  Species

   January  1988       Operational  Second  Generation RADM

   March  1989         Evaluation of  Second Generation  RADM
     NAPAP  has  planned  two major assessments  designed to  provide decision

makers  with  scientific information necessary for developing  acid deposi-

tion  control   strategies.   Both the  Euleriai  models  and  the emissions

inventories  will  play  an  important  role  in  th,>  1987  and 1989  assessments.

The  1987  assessment  will  use  an  unevaluated  bet of models  for  preliminary

regulatory analysis,  whereas  the 1989 assessment  will  use the evaluated

models.   Thus  a  major field  study has  been proposed  for  1987  through

early 1988 to  collect  data  necessary  for model  evaluation.  Knowledge of

uncertainty  both  within  the  model  and   each  associated   input data  set

is required  to assess  confidence  in model  predictions.   This paper will

focus on   uncertainty  in  the  enissions   data  base  as  related  to   these

Eulerian modeling efforts.



                                 DISCUSSION



    From a modeler's viewpoint,  uncertainties in emission  inventories  can

be categorized into two types: 1) uncertainties associated with errors or

inadequacies in the  data  base, and 2) uncertainties  associated  with  the

representativeness of  typical  daily  emissions   patterns   for  any  parti-

cular day being modeled.  Both the  emissions  inventory developers and  the
                                    57

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 modeling groups have begun to  address the  first  type  of uncertainty, but



 from different perspectives.   The developers  have been primarily concerned



 with improving  and  verifying those  raw  data elements  which  are  used in



 estimating annual point  and  county  level  emissions.   Those  elements in-



 clude  emissions  factors,  fuel  utilization and quality, production acti-



 vity,  and others.  They have  also been concerned with improving procedures



 and data necessary to  provide the temporal,  spatial,  and  species  resolu-



 tion required by the Eulerian  models.  Most  of the quality control tests



 have been  performed  on  these  individual  data elements and  efforts  are



 underway to  associate  a  level  of uncertainty with  each  of the individual



 elements comprising  the  final  emissions estimates  at point,  county  and



 grid 1evel.








    The modelers, on  the other hand, primarily  work  with the emissions



 inventories  in  their   most  resolved  form  - hourly  gridded  emissions.



 Their  quality control  tests search mainly for  individual  grids that appear



 to be  inconsistent  with  their surroundings,  subregions of  the  modeling



 domain that  appear unexpectedly high or  low,  VOC  species ratios that seem



 inconsistent with ambient measurement data and unexpected temporal  pat-



 terns  within  a  subregion.   Both  the developers  and  the modelers  have



 compared the NAPAP inventory  with other inventories  with somewhat  differ-



 ent results  because  of the  different  frames  of  reference.   Generally,



 the State totals for  individual species favorably agree  with  other inven-



 tories, or  discrepancies  can  be explained  by differences  in  methodology.



 However,  the modelers have found  that even when  State totals agree there




are sometimes significant  differences in  the  spatial or  temporal  patterns




of the  gridded emissions,  and at times differences  in  the relative magni-
                                   58

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tudes of  the reactive  species.   This  contradiction  is often  caused  by



errors  in the State emissions which have cancelled out in the State total.



Thus  it  is  important  for  the  developers to  begin  to  incorporate  into



their quality control  procedures more  analytical tests typically performed



by the  modelers.   In addition, it  is  important for the modelers to have a



better  understanding  of the quality  control  procedures  and  estimates  of



inherent variability  of the  individual  data  elements used  in  computing



emissions.







      Uncertainties in emissions  introduced by the question of representa-



tiveness are crucial  for some of  the proposed model  evaluation studies.



The  RADM will  be examined  in an episodic mode; thus, any major deviation



of the  estimated  typical  hourly emissions from  actual  emissions  for  the



particular days  being  modeled  has  the potential  to  influence  the  model



results.  Additional   burden is  then  placed  on the  inventory  developers



and  modelers  to  ensure  that  there are  no  atypical  operations  in  major



sources during the modeling periods.  For studies of the first  generation



RADM existing information on the major SOj point  source emissions will  be



used to  check  the representativeness  of  the  NAPAP  emissions.   Since  the



field study  is still  in the planning  stages more  options are available to



reduce  uncertainty in the emissions for the second generation RADM studies



Some of the  choices  include  acquisition  of  data on  any  anomalous  plant



operation during  the  period of  interest,  installation  and  operation  of



continuous emissions  monitors  (CEM)  on major  sources,  the  collection  of



actual hourly  fuel  use  or  production data,  improved activity  data  for



area source emissions  estimates,  etc.   All of  these options involve signi-
                                     59

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ficant  additional   cost  beyond  the production  of  a  typical  oase  year



inventory.   Therefore,  there  is  a  definite  requirement  to  rank  data needs



to most  effectively  accommodate  improvements  in  the  base  inventory  as



well  as the specialized needs of episodic model studies.   In response to



this need,  modeling studies  using  RADM  are currently being  performed  to



gain a better understanding of the  sensitivity  of  the model  to  uncertain-



ties in  emissions.   Attention   is  being given  to  spatial   and  temporal



variability in all  of the major  chemical species, and  speciation of VOC.



These sensitivity studies should  provide  information useful to  optimize



the data collection activities  and to  reduce  uncertainties in  critical
areas.
                               CONCLUSIONS








     In order to confidently use emissions inventories in the development,



evaluation, and application of large scale Eulerian  models  like RADM, it



is essential  to have  an  understanding  of the  quality  of the  input data



bases.  Standardized  quality  assurance and uncertainty estimation proce-



dures must be established  by the  emission data  base developers to provide



emissions inventories  that  are  reliable and directly useful  for a variety



of NAPAP applications.  Current modeling  sensitivity studies will provide



feedback to  effectively   rank  future  emissions  inventory  improvement



activities.
                                    60

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       HISTORIC EMISSIONS OF S02 AND NO  SINCE I99C

            BY STACK HEIGHT RANGE AND BY SEASON
                            by
                   Gerhard Gschwandtner
           Pacific Environmental Services, Inc.
                   1905 Chapel Hill Road
               Durham, North Carolina  27707
                EPA Contract No. 68-02-3887
                     Assignment No. 11

                   EPA Project Officer:

                      J. David Mobley
      Air and Energy Engineering Research Laboratory
           U. S. Environmental Protection Agency
       Research Triangle Park, North Carolina  27711
                      Presented at:

Second Annual Acid Deposition Emission Inventory Symposium
                Charleston, South Carolina

                   November 12-14, 1985
                             61

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                               ABSTRACT



     Historic emissions of sulfur oxides and nitrogen oxides were



estimated  for each state of the conterminous United States.  The



emissions  were estimated by ir>ai vicijal source category on the state



level from 1900 to 1980 for every fifth year and for 1978.  The source



categories included power plants,  industrial boilers, industrial



processes, commercial and residential heaters,  natural gas pipelines,



highway vehicles,  off-highway diesel engines, and all other anthropogenic



sources.   These emissions were calculated from salient statistics



indicative of fuel consumption or  industrial output,  estimations of



average statewide  fuel properties,  and estimations  of emission factors



specific to each source category.   The emission  estimates were then



aggregated to show the emission trends by state,  region,  and all



states combined.



     This paper summarizes  the national  historic  emission trends by



emission release  (stack)  height and  by season.  The  paper outlines



the approach  taken and presents general  results.
                                62

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             HISTORIC EMISSIONS OF S02 AND NOX SINCE 1900



                             INTRODUCTION



     Sulfur dioxide  (SOj) and nitrogen oxides (NOX) are considered



primary precursors of acidic precipitation.  The anthropogenic



emissions of these pollutants are suspected causes of many biological



and  chemical effects observed in recent years.  Understanding the



historic emission trends is important to understanding the development



of acid-precipitation-related problems and causes of observed



environmental effects.



     Average emission rates for each study year were calculated for



individual  source categories for each state.   The source categories



are  listed  in Table  1 according to the fuel consumed.  These categories



represent all types  of boilers, furnaces, engines, processes, and



other anthropogenic  emission sources.  The basic steps involved in



calculating state emissions have been described in detail  by



Gschwandtnerl and by Gschwandtner et al.2  The emissions by source cate-



gory were totaled by year to provide an estimate of overall national



emission trends.



Analysis by Release  (Stack) Height



     The percentage distribution of national  emissions was then esti-



mated for each source category according to four broad ranges of stack



heights.  In the case of electric utilities,  individual power plant



emission estimates and stack height data were used to determine the



national distribution by height from 1950 to 1980.  For earlier years



and for other sources, a general trend in the percentage of emissions



by stack height range was estimated based largely on engineering judg-



ment.  It was assumed that the percentage emissions of each category



changed linearly over time.   The percentages estimated for each year
                                  63

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         TABLE  1.   FUEL TYPES AND EMISSION SOURCE CATEGORIES
Bituminous Coal:
Anthracite Coal:

Residual  Oil:




Distil late Oi1:
Natural Gas:
Wood:
Gasoline and Diesel
Fuel :
Other:
Electric Utilities
Industrial Boilers and Space Heaters
Commercial and Residential Uses
Steam Railroads
Coice Plants

All Uses

Electric Utilities
Industrial Boilers and Space Heaters
Commercial and Residential Uses
Vessels

Electric Utilities
Industrial Boilers and Space Heaters
Commercial and Residential Uses
Railroads
Vessels

Electric Utilities
Industrial Boilers and Space Heaters
Pipeline Compression  Stations
Commercial and Residential Uses

Electric Utilities
Industrial Boilers and Space Heaters
Commercial Heating
Residential Wood  Stoves  and  Fireplaces
Highway Vehicles
Off-Highway Vehicles
Vessels
Wildfires
Cement Plants
Copper, Lead,
Mi seellaneous
Miscellaneous
                                      and  Zinc  Smelters
                                      Industrial  Processes
                                      Other  Sources
                                  64

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were then multiplied  by  the  total  emissions of  each category.   These

results provide  a  general  indication  of  the national  trend.

Analysis by  Season

     The seasonal  emissions  were  also estimated  for major  source

categories.   These  estimates were  based  on monthly fuel data available

for only certain years,  and  an  assumed percentage distribution  of  the

emissions by  season  over time.  The distribution for  each  category

was weighted  by  the  historic emission estimates  to yield an average

seasonal distribution for each  study  year for all categories combined.

                                DISCUSSION

Distribution  by  Release  (Stack) Height

      Figure  1 shows  the  overall national trend  of SU^  and  NOX emissions

by  stack height  range.   This analysis does not  include stack exit

velocities or atmospheric mixing  heights, which  are also important

considerations.  The  analysis in  this study suggests  that  more  S0£

emissions were released  into the  atmosphere from stacks taller  than

24'J ft* than  from  stacks  shorter  than this height since about 1945.  By

1980,  approximately  30 percent  of  the SOj emissions were emitted above

480 ft, for  example,  compared to  only ab"ut 5 percent  above this height

in 19bO.  In  19bO, six power plants reported ? maximum stack height greater

than 480 ft.  Not only have the  percentages increased,  but  tot?l national

S0£ emissions  also increased and  peaked  around  1970.   The  percentage of

the total  S02 emissions  released  below 120 ft has generally decreased

over the study period.   The  distribution of NOX emissions  has histori-

cally remained constant,  although  on the national level the total

emissions  have steadily  increased.  Approximately 60  percent of the

total  NOX  emissions in 1980  were  released from ground  level sources;

predominantly from transportation  sources.
(*)  1 ft = 0.3048m
                                   65

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                                                            STACK HEIGHT, ft
      1 ton = 9O7.18 kg
      1 ft = 0.3048 m
1900     1910     1920     1930     1940     1950     1960     1970
         Figure 1. Total national S02 and NOx emissions by stack height ranges.

                                      66

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     Analysis  of  the electric  utility  category alone  suggests  that,  in



 the  1950's and 60's, most  of  the S02 ana  NOX emissions  from  this cate-



 gory were released  below 480  ft --  mostly  between 240 and 480  ft.  Sy



 1980, about  50 percent  of  the  total S02 emissions and 40 percent of



 the  NOX  emissions  from  this source  category were released above 480  ft



 as a result  of the  trend toward taller  stacks.  Since the emissions



 from electric  utilities constitute  a large portion of the total national



 emissions in  recent years, as  shown by  Gschwandtner e_t  al ,^  they have a



 significant  effect  on  the  overall distribution of emissions  by release



 height.



 Distribution  by Season



     Table 2  presents  the  estimated percentage distribution  of emis-



 sions by season on  the  national level.  The percentage  of wintertime



 S02  emissions  appears  to have  decreased from about 35 percent of the



 total annual  emissions  in  1900 to about 26 percent of the total in



 1980.  This  gradual decrease  is largely a  result of switching from coal



 to fuel  oil  and gas for heating, and also  an increase in summertime



 fuel combustion by  power plants to  meet the demands of  refrigeration



 and air  conditioning.  The seasonal distribution is more pronounced on



 a regional level where climatic conditions deviate from the  national



 average.  NOX  emissions appear more evenly distributed  by season than



 S02 emissions.  This is primarily due  to an assumed distribution of



 highway  vehicle emissions  by season, and  the fact that  the major



 sources  of S02i which are  seasonally /ariable, emit less NOX.



     Figure 2  shows the trend  in the quantity of emissions by season



on the national level.  While  the S02  percentage distribution  shows a



gradual   change, the increase in the quantity of S02 emissions  is



more evident,  especially in the summertime.




                                     67

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                                TABLE 1.   PERCENTAGE  DISTRIBUTION OF EMISSIONS BY SEASON
                    Percentage S02 Emissions
           Year    Winter     Spring     Summer
01
en
Fall
Year
 Percentage NOX Emissions
Winter     Spring     Summer
Fall
19UO
1905
1910
1915
1920
1925
1930
1935
1940
1945
1950
1955
1960
1965
1970
1975
1978
1980
34.8
34.5
34.3
34.3
34.2
34.0
34.0
33.4
32.5
32.3
30.8
30.2
29.5
28.0
26.7
26.1
26.4
26.4
19.4
19.4
19.4
19.3
19.4
19.5
19.4
19.4
19.8
20.0
21.0
21.9
22.7
23.3
23.5
23.5
23.4
23.4
23.6
24.1
24.5
24.7
24.8
25.0
25.4
26.0
26.3
26.4
26.3
25.7
25.4
25.6
25.8
26.1
26.1
26.1
22.2
22.0
21.9
21.7
21.6
21.4
21.2
21.2
21.3
21.3
21.9
22.2
22.5
23.1
23.9
24.2
24.1
24.1
1900
1905
1910
1915
1920
1925
1930
1935
1940
1945
1950
1955
1960
1965
1970
1975
1978
1980
30.8
31.1
31.7
31.9
31.6
30.3
29.5
28.8
29.8
28.5
27.6
27.2
26.5
25.7
24.6
24.2
24.5
24.5
19.9
19.8
19.8
19.8
20.2
20.4
20.7
20.9
21.2
21.2
22.3
23.0
23.4
23.9
24.1
24.1
24.0
24.0
26.1
26.9
25.8
25.8
25.8
26.5
27.0
27.4
27.3
27.5
27.0
26.7
26.5
26.6
27.2
27.3
27.2
27.2
23.2
23.0
22.6
22.4
22.4
22.7
22.9
22.9
22.7
22.8
23.0
23.2
23.5
23.9
24.2
24.3
24.3
24.3
                                         Winter = December. January, February
                                         Spring = March, April, May
                                         Summer = June, July, August
                                         Fall   = September, October, November

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1900     1910      1920      1930      1940     1950     1960      1970     1980
         Figure  2. Total national S02 and N3x emissions by season.
                                      69

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                              CONCLUSION

     The historic emission estimates  presented  are  consistent in trie

estimating methodology used.   They  provide  a  basis  for studying the

relationship between emissions  in  the past  and  observed  environmental

effects including tree-ring growth  patterns,  material  damage,  and

acidic deposition.   The emission  trends shown in  this  presentation

should De considered the best available estimates at  this  time,  but

it should be remembered that,  as work in  this area  continues,  more

Defined estimates may be made.  The historic  emission  estimates  show a

definite trend in terms of the  total  nation by  stack  height range and

by seasonal  distribution.
                               REFERENCES

1.    G.  Gschwandtner.   Historic  Emissions  of S02 and  NOX  Since  1900.
     In  Proceedings:   First  Annual Acid Deposition  Emissions  Inventory
     Symposium,  EPA-60G/9-85-015  (NTIS PB  85-200004/AS),  U.S. Environ-
     mental  Protection  Agency,  Research Triangle Park,  NC,  pp   38-46
     May 1985.

2.    G.  Gschwandtner,  K.C. Gschwandtner, K. Eldridge,  "Historic Emissions
     of  Sulfur and  Nitrogen  Oxides in the  United States  crom  1900  to  1980,"
     Volumes I and  II.  EPA-600/7-85-009a  and 009b  (PB  8S-191 195/AS  and
     PB  85-191 203/AS), U.S. Environmental Protection  Agenc). Research
     Triangle Park, NC. April  1985.
                                   70

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          DEVELOPMENT OF MONTHLY EMISSIONS TRENDS

                     FOR RECENT YEARS
                            by

                       Di ane Knudson
                Argonne  National Laboratory
             DOE Contract No. W-31-109-Eng-38
                   DOE Project Officer:
                      Edward Trexler
                  Office of Fossil Energy
                U. S. Department of Energy
                      Washington, DC
                      Presented at:

Second Annual Acid Deposition Emission Inventory Symposium
                Charleston, South Carolina

                   November 12-14, 1985
                             71

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                   Development of Monthly Emissions  Trends
                               for Recent Years

                                  D. Knudson
                                   ABSTRACT
       As atmospheric transport  and  deposition  modeling capabilities increase
and  monitoring  data  are  accumulated,  it  becomes  desirable  to   also  have
representative  emissions  data.    This paper  describes  the  methodology and
results of an  effort  to generate state-total source category-specific monthly
S02  and  NOX  emission  estimates  for the  period   1975-1983.    These  data
complement other data bases and  support a  variety  of analytical efforts.  The
basis  of  the  monthly emission  estimates  are source  category-specific state-
total  S02  and NO   emission  values  from  the 1980  NAPAP  emissions   inventory.
Annual emissions from the  electric utility industry  are  allocated   to monthly
values using  actual monthly  fuel  use for  each year  in  the  period.   Annual
emission values  for other source  groups  were  apportioned  to  monthly values
using  data  which  provides  an  indication of  the  monthly  activity  for  each
source group in the inventory year (1980).   Annual state-total source category
emissions for  other years  in the  period  were derived  from  the EPA emissions
trends data.

       The  results indicate  that  intra-annual variability  of  SCK  and NO
emissions  for each  state depend  on  the  variability of   source   categories
contributing  most  to state  total emissions.    In  states with  S02  emissions
dominated  by   the  electric  utility  sector,  maximum emissions  occur  in the
summer and winter.   The  relative importance of these two peaks depends on such
factors  as   climate and  utility  prime   mover   and  fuel  mix.   Monthly NO
emissions variations are also  a function  of the variability of source groups
contributing  the most  to  total  state  N0x  emissions.   In  all  states, vehicle
fuel  consumption  contributes   substantially  to  total state  NO    emissions.
Monthly  variability of NOX  emissions  attributable  to this  source category
shows only small variability  in most  states.
                                       72

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                    DEVELOPMENT OF MONTHLY EMISSIONS TRENDS

                                FOR RECENT YEARS
                                  INTRODUCTION




       Evaluation   of   long-term  data  on  such  parameters   as   atmospheric




deposition,    biological    response,    geochemical    changes,    and   response




characteristics  of  other  receptor  systems  for  trends  is  facilitated  by




appropriate  emissions  data for  the specific  period.   In many  cases  accurate




evaluation  of the measured  deposition and/or response  of  a subject  receptor




requires  emissions  data  with  a  temporal  resolution matching  the  critical




period   of   the  receptor.     For   establishing   correlations   and   functional




relationships between  receptor  response  and emissions for  trends  evaluation,




monthly  emissions  estimates are sometimes  required.   The data  base  developed




in  this  project,  therefore, complements the commitment to collection  of  long-




term  deposition and  receptor  system response data.




       This   paper  describes  the  development  and   presents   an  overview  of




monthly  S02  and NOX emission estimates for the period 1975-1983.    Review  of




the  methodology will  address  the  utility  sector  separately  from all  other




source groups.  This is  because  of  the  generally large contribution of SC^ and




NO   emissions  by   the  utility  -.ector  and  because  the methodology  is  more
  X



detailed for  this source  category.   Portioning of  annual  state-total emissions




estimates for  the diverse  group  comprising  the nonutility sector uses a number




of  different  data  bases.   The  selection of the appropriate  monthly data base




for  allocation  of   annual  emissions  is  a  critical  step  in  the data  base




development.   A more thorough presentation  of  the methodology is  provided  in




Reference 1.




       The state-total  source category-specific monthly  S02  and NOX estimates




for all  years  in  the  period  1975-1983 are condensed into  two  summaries for
                                      73

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presentation.  Total  regional  seasonal S02  and NOX values  are presented for


Federal Regions 1 through 6 to illustrate  regional  emission trends.  Then, to


provide  an   indication  of  differences  in  source  category  contributions  to


monthly emissions  variability,  monthly source  category specific  S02 and N0x


emissions are presented for 1980  for Illinois and New York.




                                 METHODOLOGY


       The 1980 NAPAP  SOo  and  NO  emissions inventory  (version 3.0) provided


state-total  source category-specific emission values for  S02 and NOX>  A six-


digit  level  of  specificity of the  Source  Classification  Code  (SCC) was used


for  point  sources to  identify  the  major  source  category  (e.g.,   industrial


boiler)  activity   (e.g.,  combustion  and   incineration),   and  fuel  (coal  and


residual oil).   For  area  sources,  the  eight digit  code  unique  to the NAPAP


inventory was  used to  define  source groups.   The  apportioning  of the state


annual emissions used data bases  that provide some measure of activity for the


source category,  operation, and/or fuel  use on a monthly basis.

Utility Poinc Sources - All Years


       Computation of  monthly  862  emissions  for the electric  utility sector


used  plant  emission  values furnished  by  E.H.  Pechan  and Associates for the
               fy
years  1975-1982   in  combination with  monthly   fuel  consumption  reported  by


Energy Information Administration (EIA)  Form 759 "Monthly Power Plant Report".


Annual  emission   calculations  for  1983 were  performed  by  Argonne National

Laboratory according  to methodology developed by Pechan.


       Computation of monthly NOX  emissions  for this sector used  the monthly


fuel  use  from EIA  Form 759  with  plant-average  NOX emission factors.   The


emission  factors   were  derived   from   AP-42  firing  type  and  fuel-specific


emission factors  in  combination  with 1980  unit-level  fuel  use for firing of
                                        74

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coal, lignite, gas,  residual  oil,  and distillate oil in conventional  boilers;




internal  combustion  of  natural  gas  and  distillate  oil;  and  gas turbines.




These emission factors coincide with the fuel  use  categories  on Form 759.




Nonutility Sources,  1980




       Allocating  annual  SC>2 and  NOX emissions  to  monthly values  for  the




diverse  group  of  nonatility sources requires a number of equally  diverse  data




bases.   The  source  categories and  the  data  bases supporting monthly allocation




are  defined  in Table 1.




Nonutility Point  and Area  Sources  for  Other  Years




       Monthly SC^  and NOX emission estimates  for  nonutility  source categories




were  derived from national emission estimates  in the  EPA report,  "National Air




Pollutant  Emission  Estimates:   1940-1983.'    Values  from   that  report  for




source  categories  matching  those  used  for the monthly  emissions estimation




were  normalized,  with  1980  as   the  base  year.    This  provided fractional




national  emission  changes  relative  to  1980  for all  years in  the   period.




Therefore,  the monthly source  category  emission  fractions developed  for  1980




were  held constant  throughout the  analysis.




                                    RESULTS




       Figures  1  through  5  present seasonal  total  862  and NOX emissions  for




the  period 1975  through  1983 for Federal Regions  I and II, III,  IV. V,  and VI




respectively.    A  characteristic  apparent  in  all  regions   is   the  lack  of




seasonal  variability  in   NOX emissions  compared  to  S02.    This   is  probably




attributable to the  large  contribution of vehicle  fuel combustion  to  total NPX




emissions in most states,  and the lack, of variability in  monthly  vehicle fuel




combustion.




       For total  S02 and N0x  emissions  in  Regions I and II  (Figure  1),  there




is a  small  difference between S02  and NOX  emissions, with NOX  being  slightly







                                       75

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Table 1.  Data Sources for Estimation of Nonutility Monthly S02
          and NOV Fractions for Apportioning Annual Emissions
           Description
Industrial external coal combustion
Industrial external oil combustion

Commercial and Institutional external
   coal combustion
Commercial and institutional external
   oil combustion
Commercial, institutional, and industrial
   external combustion for space heating

Commercial, institutional, and industrial
   internal oil combustion
Industrial chemicals:  sulfuric
   acid, plastics, organic chemicals,
   explosives, carbon black, printing
   ink
Food product processing
Primary metal:  c  ".e manufacturing,
   steel production, copper smelters,
   zinc, and other primary metals

Secondary smelting:  o^uminum, copper
   lead, etc.

Mineral products:  glass, fiberglass,
   gypsum products, cement, brick,
   pottery
In-process fuel use
Petroleum refining
Wood and paper products
   (including Kraft pulping)
Crude oil and natural gas extraction
   (including gas sweetening)

Solvent use
Solid waste disposal

Industrial internal gas combustion
 Data Source or Approach for
Estimating Monthly Fractions
Quarterly Coal Report
Adjusted FRB monthly produc-
   tion indexes

Quarterly Coal Report

Uniformly distributed3
Local climatological data -
   heating-degree-day
   accumulation

Uniformly distributed3
FRB monthly production indexes
   for SIC 2819; inorganic
   chemicals

FRB monthly production indexes
   for SIC 209:  miscellaneous
   food preparation
FRB monthly production indexes
   for SIC 331:  basic steel,
   coking, mill production;  SIC
   333-6,9:  nonferrous metals
FRB monthly production indexes
   for SIC 333-6, 9:  non-
   ferrous metals
FRB monthly production indexes
   for SIC 326:  concrete and
   miscellaneous clay
FRB monthly production indexes
   for SIC 326:  concrete and
   miscellaneous clay
FRB monthly production indexes
   for SIC 291:  petroleum
   refining
FRB monthly production indexes
   for SIC 261:  pulp and paper
FRB monthly production indexes
   f
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      Table 1 (Cont'd)
                                                Data Source or Approach for
                 Description                    Estimating Monthly Fractions
      Incineration and open  burning               Uniformly distributed3
      Miscellaneous  area sources0                 Uniformly distributed3
      Diesel and gasoline vehicles                1980 Highway Statisticsb


      aAnnual  data  assumed  to  be uniformly  distributed  throughout  the year,
        due  to  lack of monthly data.
        Nox  only
      cRailroad  locomotives, military  aircraft LTO's,  civil  aircraft LTO's,
        commercial  aircraft  LTO's, coal  vessels,  diesel  oil vessels,  residual
        oil  vessels,  gasoline  vessels,   solvent  purchased,  gasoline marketed,
        unpaved   road  travel,   unpaved  airstrip  LTO's,  construction,  wind
        erosion,  land tilling, forest wild  fires, managed  burning, agricultural
        burning,  frost control,  and structural  fires.
 less.   SOn emissions  have  been relatively  constant,  while NOX emissions  are

 increasing  slightly.   Winter is the  season  of peak emissions for S02 and  N0x

 for the region  through  the  entire  period.

       Region   3   (Figure   2)   shows   a   small  502   trend   downward,  and  no

 discernible  NO  trend.   N0x emissions  are  about  50 to 60%  of regional  S02

 emissions  for  all  years in  the  period.  Winter is  the peak  season for SO-,  and

 NO  for all years  except 1983,  in  which  summer  is  the peak  emission  season.

       Region  IV  shows  a  steady  decline  in S02  emissions  from a  maximum in

 1977.   There  is  little change  in t,'0x emissions  through the period, with  NOX

 being about 50% of the  S02  emissions.

       In  Region  V,  S02 emissions  have  decreased  steadily since  1977 to  a

value  about  double  the NOX  emissions  in 1983.   NOX emissions have changed

little  throughout  the  period.    Winter  is  the  peak  season for  NOX and  S02

emissions for all years  in  the  period.


                                         77

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M
      600-1
      500-
      400-
   r>
   c

   •2  soo-
z o

o
c
o
*5>
io
     200-
      100-
             75     76     77     78     79    80    81

                              Season and Year
                                                      82
 Figure 1   Regions 1 and 2 Seasonal SO  and NO   Emission Totals for

           the Period 1975-1983.      L       x
                                 REGION 3
c
to

in

'E
      lOOO-i
       800-
•O p


§1



C?"o



•5 ^


O
  O

 .O
       600-
       400-
       200-
              75    76    77    78    79    80

                                Season and Year
                                                  81     82
 Figure 2  Region 3 ^Seasonal  S02  and N0x Emission Totals  for  the

-------
                                 REGION 4
 n

 o
      2000-T
      1500-
 O £
 >"o
 O o


 "5
 c
 o
 'o>
 c
 or
1000-
 500-
                                      scx
              75     76     77     78     79     BO

                               Season and Year
                                            81
82
                                                             83
   Figure  3   Region A Seasonal SO  and NO  Emission Totals for the Period
             1975-1983.                   x



                                REGION 5
 c
 o
 'in
 m
      2500
      2000-
      1500
O o
z o  1000

"5
c
o
 0
ot
io
500-1
                                     SO,
             75     76     77    78    79    80


                              Season and Year
                                           81
                                                 82
 Figure 4  Region 5 Seasonal SCK and NO  Emission Totals  for  the

           Period 1975-1983.           X

-------
                               REGION 6
     1500-1
 5
 w
 CM
O
1000-
o  .2
O
O
EC
^
"o
 500-
                                     so,
            75    76    77    78    79    80
                              Season and Year
                                           81
82
 Figure 5  Region 6 Seasonal SO. and NO  Emission Totals for the
                                       X
           Period 1975-1983.
                                  80

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                    New York
                         linn.
                 MAMJ JASOND
J  F
                           CD Industrial Coal
                           EZJ Industrial Oil
                             Industrial Process
                             Miscellaneous
                             Utility Oil
                             Utility Coal
                      Illinois
         ttO-,
             JFMAMJJASOND
                                        CD Industrial Coal
                                        ZZ3 Industrial Oil
                                          Industrial Process
                                          Miscellaneous
                                          Utility Oil
                                          Utility Coal
.Figure 6 Monthly 1980 SO  Emissions by Source Category for
        New York and Illinois.
                           81

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                        Mew York
        J   F
                                                 CD  Vehicle
                                                 E3  Industrial Fuel
                                                 E33  Industrial Process
                                                 Q  Miscellaneous
                                                 EZ  Utility Oil & Gas
                                                 •I  Utility Coal
                         Illinois
   100
                                                  CH Vehicle
                                                  E2 Industrial Fuel
                                                  ESS Industrial Process
                                                  HZ) Miscellaneous
                                                      Utility Oil & Gas
                                                      Utility Coal
Figure 1  Monthly 1980 NO   Emissions by Source Category for
          New York and Illinois.

-------
        In  Region  VI,  NOX emissions  are roughly a factor of  two higher than S02




emissions.   Neither SC>2 nor NOX emissions have  changed significantly over the




period  of  interest.   There  is  a slight winter peak for both pollutants for all




years except 1983,  for  which summer is the  season for maximum S02 emissions.




        Figures  6  and  7 present   1980  monthly  source  category  SC^ and  NOX




emission  estimates for  Illinois  and  New York,  respectively.   In  both  states




the  utility  sector contributes the  most to  SCK emissions.   In Illinois monthly




variability  in utility  coal  combustion dominates the  total  state  monthly S02




emissions  variations.   In  comparison, utility coal derived  SC^  emissions for




New  York have  little variability  through  the year.   The  variations  in  total




New  York  ttate SC^ emissions is largely attributable  to utility oil combustion




fluctuations.   In  New  York,  source  categories  defined as  industrial  oil and




miscellaneous   also  have   substantial  contributions  to   total   state   SO-,




emissions,  but show little  monthly  variability in SO*? emission rates.




        Monthly emissions of N0y  also  show  differences between  the  two  states




(Figure 7).   NOX  emissions  in Illinois are  clearly  dominated  by utility  coal




combustion   and   vehicle fuel use.    The  vehicle  source  category  is   the




overwhelming  contributor  to  NOX  emissions  In  New   York   State.    However,




coincident  minimum monthly  NOX  emissions  for the utility  oil,  miscellaneous,




and  industrial  oil  combustion  categories  combine   to  yield  a  state-total




minimum NO  emission rate   in the  late  spring to early  summer  period,  even




though  vehicle-related  emissions  are  not  at  their minimum  during these months.









                                  CONCLUSIONS




       Monthly  state-total  S02 and NOX emissions  by  source category  for the




years 1975-J983  have been  prepared.   The  allocation  of   annual  emissions  to




monthly values used  a diverse set  of  data describing  source category-specific
                                        83

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fuel  use  or related  activity.   Definition of the  monthly  data base used  for




allocation is the critical step in the development  of the monthly  data.




       General  regional  patterns  of  monthly  S02  and  NOX  emissions   are




dependent  on  the  characteristics of  each  region.   In the northeast  (Regions




I-III),  S02  emissions have decreased  slightly while NOX  emissions have  been




increasing through  the  1975-1983  period.   In these regions winter  is  the  peak




S02 and NOX emission  season.   Region  IV has experienced a significant  decline




in  S02 emissions  and little  to no  increase  in  NOX,  with  summer being  the




season  of maximum  emissions  for  both  pollutants.   Region  V has  shown  the




largest decrease  in S02  emissions,  with little change in NOX emissions  across




the period.   Winter is  the  season of  maximum S02 and NOX emissions  for  Region




V.   The relative portions and  trends  in S02 and NOX  emissions for Region  VI




are  distinctively  different  from the  patterns  in  the  eastern  regions.    In




Region  VI,  N0x  emissions   are  roughly  a  factor  of  two  higher  than   S02




emissions, with  neither showing  any  trend  through the  period.   Unexpectedly




for  Region VI,  winter  is  the  season  of peak  S02  and NOX  emissions for  all




years  in  the  period,  except   1983.   In  1983,  S02  emissions peaked  in  the




summer.




       Generalizations   of  state-level   monthly  emissions  variability   are




impossible to make.   The pattern of monthly  S02 and NOX emissions  dopends  on




the  relative  contributions  of  source   categories  in  each  state  and their




monthly emission pattern.




                                ACKNOWLEDGEMENT




       This  research   has   been  funded   as   part  of   the  National   Acid




Precipitation Assessment  Program's Man-Made  Sources  Task  Group  by the  U.S.




Department of Energy  Office  of Fossil  Energy.   The DOE  Project Officer  was




Edward  Trexler.     Special  thanks  is   given   to  Marylynn  Placet  of  Argonne




National Laboratory  for her  assistance  in  methodology development and  data



base selection.



                                         84

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                                  REFERENCES
1.   Knudson, D,A.  "An  Inventory of Monthly  Sulfur Dioxide Emissions  for  the
    Years 1975-1983," ANL/EES-TM-277 (April 1985).

2.   E.H.  Pechan  and Associates,  "Estimates  of Sulfur Dioxide  Emissions  from
    the Electric Utility Industry," EPA 600/7-82-061a and b (November 1982).

3.   U.S.  EPA  "National Air  Pollutant  Emission  Estimates,  1940-1983,"  EPA
    450/4-84-028 (December 1984).
                                       85

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             APPLICATIONS  OF  EMISSIONS  DATA IN
                THE  NAPAP  ASSESSMENT  REPORT
                      Paul  Schwengels
                Office of Air and Radiation
           U.S.  Environmental  Protection Agency
                       Presented at:


Second Annual  Acid Deposition Emission Inventory Symposium

                Charleston,  South Carolina
                   November 12-14,  1985

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        APPLICATIONS OF EMISSIONS DATA IN THE NAPAP ASSESSMENT REPORT
                            By:  Paul Schwengels
                         Office of Air and Radiation
                    U. S. Environmental  Protection Agency

                                  ABSTRACT

     A great deal of emission^ data has  been assembled for use in the
forthcoming NAPAP Assessment Report.  This includes natural and man-mac'e
sources of a number of relevant chemical  species or classes in both the
United States and Canada.  Emissions data will  be used in the report in
several ways.  First, an emissions section will  summarize best available
information on substances of interest, compare natural and man-made levels
provide regional distributions and comparisons,  and evaluate national and
regional trends in man-made emissions where possible.   In addition,
emissions data have been used to support analyses and  modeling for the
atmospheric processed and materials damage sections of the report.  This
paper briefly describes the various data sets which have been assembled to
meet these different needs in the assessment.  It identifies the different
types of data needed to support different types  of analyses or comparisons.
Uncertainties and limitations in available data  and their impact on
assessment will be reviewed, as well as  data improvements needed to support
improved assessments in the future.  Some preliminary  approaches to analysis
and presentation of data being considered for the Assessment Report will
also be discussed.
Note:  The text of this paper was not available at the time of publication
       of the proceedings.
                                     87

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            OVERVIEW OF  THE  DEVELOPMENT  OF  THE
              1985  NAPAP EMISSIONS  INVENTORY
                     Charles  0. Mann
           U.S.  Environmental  Protection  Agency
       Office of Air  Quality  Planning  and  Standards
                      Presented  at:

Second Annual  Acid  Deposition  Emission  Inventory  Symposium

                      Charleston,  SC


                   November 12-14,  1985
                             88

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                      OVERVIEW OF THE DEVELOPMENT OF THE
                        1985 NAPAP EMISSIONS INVENTORY
                                   ABSTRACT
      The  National  Acid  Precipitation  Assessment   Program   (NAPAP)  needs  a
 current and detailed  emissions  inventory  to  support its activities.  To meet
 this  objective,  NAPAP and  the  United  States  Environmental  Protection  Agency
 (EPA)  have  selected  1985 as  the base year for the  inventory.  Data collected
 by  the States  during  1985  for  the National  Emissions  Data  System (NEDS)  will
 be  used to  develop the NAPAP emissions inventory.  The  NEDS was selected to
 permit the  design  of a data collection program that  will  meet  NAPAP's require-
 ments  for both  quality assurance and  spatial,  temporal, and species  resolu-
 tion.   Ensuring  the  accuracy of  more  than  4 million  items  of  data that the
 States will  collect  for  NEDS is a challenging task.  To meet this challenge,
 EPA has developed  a  five part  management  strategy.   This strategy emphasizes
 the high  priority  of the  NEDS  in 1985, establishes EPA and  State accounta-
 bility for  the  NEDS  data, delineates  quality  assurance procedures for the
 data,  provides  financial  assistance to States  that require  it,  and  ensures
 that  participating State  and EPA personnel  clearly understand  the NEDS data
 requirements.  This  management  strategy  will   result  in the development  of
 NEDS  data that will have unparalleled  quality.
                                 INTRODUCTION
     The National  Acid  Precipitation  Assessment  Program  (NAPAP)  requires
emissions data for three reasons:   to support atmospheric modeling, to explore
relationships between  sources  of  emissions  and  receptors of acid deposition,
and to facilitate examination of regulatory alternatives.  The reliability of
NAPAP's activities  in  these areas  can  be no  better than the data  on  which
they are based.  Thus, to produce  reliable  results,  these activities must be
founded on the development of a comprehensive emissions inventory with a high
degree of quality  control  and  of  species, temporal,  and  spatial  resolution.

     As illustrated in Figure 1, the basis for NAPAP's estimates of anthropo-
genic emissions will be  the  1985 emissions inventory  conducted  by the States
for the National Emissions  Data  System  (NEDS).   This system is maintained by
the National   Air  Data  Branch  of  the  U.S.  Environmental  Protection  Agency
(EPA).  The goal of this  project  is to  ensure  the  best ever development of a
NEDS data  base to  meet  NAPAP's  needs  for  1985  emission  inventory  data.
                                        89

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                                  DISCUSSION


     The NEDS  is a  computerized  system  which accepts,  stores,  and  reports
source data  and  emissions  data  for  both  point  and  area _ sources.   Point
sources are  considered to  be stationary  sources of pollution  that  emit  at
least 100 tons  annually  of  particulate  matter,  sulfur  dioxide   nitrogen
oxides, or  reacti e  volatile organic  hydrocarbons,  or  that  emit  at  least
1UUU tons annually of  carbon monoxide.   Area sources are  considered  to  be
stationary sources  with emission  rates below  these  thresholds  and all mobile
souses of  particulate  matter,   sulfur  dioxide,  nitrogen  oxides,  reactive
volatile organic hydrocarbons, or carbon monoxide.

     Point source data are  collected  by  both  State and local  air pollution
control agencies.  The data  are  obtained  for each  source  at  an individual
plant through  questionnaires,  visits,  and  emission tests.   For  an  average
plant  a  State  must   collect,  check,  and  report 350  items of  data.  After
conducting quality  assurance checks on the  data, States enter  the data onto
forms or computer tapes compatible  with  NEDS  and transmit  the  data to their
EPA Regional Offices.  States are required to make  an annual   report to EPA
for all of the sources meeting the above  criteria.

     Area source data are  developed  by  EPA's  National   Air  Data  Branch.
Development of  the  area  source  data  relies  upon  published  information for
calculating area source activity  levels,  such as quantities of  fuels distri-
buted to  States,  vehicle-miles   travelled  by  motor vehicles  and  so  forth.
State level  data  are  allocated  to  counties  using  employment,   population,
or similar  statistics.  Emissions are calculated using emission factors from
standard EPA references such as AP-42 and the MOBILE3 highway vehicle  emission
factor model.

     The major thrust of the  1985 data collection  effort is to ensure  a high
quality, timely  point  source  data submittal  by  the States.   In  deciding to
use  198b NEDS emissions data for NAPAP's purposes, r_PA  recognized  that careful
management would be  needed to  superimpose  NAPAP's data  requirements  on the
State emissions  inventory  process.   The  management   strategy  that  EPA has
developed to  help  the  States  meet  NAPAP's  requirements  consists  of five
elements:

      0  Emphasizing priority:   emphasizing  the  importance  of  meeting the
        NAPAP data requirements  to managers in State offices and  EPA  Regional
        Offices;

      0  Establishing accountability:  establishing  a  network  of  managers in
        the State  offices  and EPA Regional Offices  that will   be  responsible
        for the NEDS data;

      0  Ensuring accuracy:  establishing quality control procedures for prep-
        aration and submittal of  the source and  emissions data;
                                         90

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     0  Assisting States:   pinpointing and  eliminating  any  State  resource
        constraints; and

     0  Establishing communication:   ensuring  that  all   participating  State
        and EPA personnel understand the NAPAP requirements 1or the emissions
        data to be col 1ected.

     The first element  of the  strategy was to  establish the priority for the
1985 State  NEDS  inventory.   This has  been  accomplished  through  a memorandum
from EPA Adninistrator  Lee  Thomas  to  State Air Program  Directors  and  to EPA
Regional Administrators.  This letter  urged State and EPA Regional  assistance
to produce  an  accurate  and comprehensive  emissions inventory.   The  letter
alsu empnasized the high priority that EPA attached to tne^e goals.  To focus
additional  attention on these goals within EPA, the Administrator's Strategic
Planning and Management System for fiscal  year 1986 includes NEDS performance
milestones for managers in the Regional Offices.

     The second element  of  the strategy was to  establish accountability.   A
network of  managers  responsible for  ensuring  the quality and  scheduling  of
the emissions  data  was  established during  August and  September  198b.   This
network will  consist  of individuals in both  Regional  Offices and  State Air
Program Offices.   Accountability  for  EPA managers  is  further  emphasized
through the performance milestones mentioned above.

     The third element of the strategy is  the most challenging one.  Ensuring
the accuracy of more  than  4 million items  of  source and emissions data that
will be collected  during  1985  is a difficult task  under the  best  of circum-
stances.  Given the limited resources  typically encountered  in  the  State air
program offices,  the  task   of  selecting  appropriate quality  assurance  pro-
cedures is  nade  even more  complex.   The  quality assurance  procedures  that
NAPAP and  EPA  are to  employ  attempt  to  strike  a  balance  between  vigorous
investigations and limited  State  resources.  States  and  EPA  Regional  Offices
will oe provided with written guidance  concerning  the quality assurance checks
that NAPAP will conduct.  This  will not only focus attention both on critical
elements in the NEDS data and on appropriate calculation  procedures, but will
also minimize errors.  Also, Regional  Officec  will be provided with copies of
computer programs  designed  to  check  the  data  submitted by  the  States  for
potential  errors.    When  questions about  the  data  are   raised,  the  Regional
Offices will  contact the States to resolve any problems.  Finally, NAPAP will
perform its quality  assurance  checks  on  high-priority  data  items  to  ensure
that errors have  been  corrected  by  the State  and  Regional  Office  efforts.
NAPAP will  also cross-check the data  received  wi ch independent  data sources,
such as U.S.  Department  of Energy data  for individual electric utility plants.

     The fourth element  of  the  strategy  is assisting  the  States.   F.PA has
allocated  $500,000 from Clean  Air  Act  Section  105 air quality grants to help
States that need  extra  resources.  A similar amount of assistance as contract
support is  to  be  provided   from  NAPAP  funds.   The  resource  assistance  plan
is discussed in detail   in  the  paper by David Johnson,  titled Assistance to
States In  the Development of the 1985  NAPAP Emission Tnventory.
                                        91

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     The final   element   of  the  management  strategy  is   communication.   On
July 30  1985, OAQPS transmitted written guidance to each  EPA  Regional  Office
Air Program Director which discusseo three  initiatives being taken to  ensure
that the network of  State  and  EPA personnel  responsible for the  NEDS emissions
data understand both their roles and the data collection requirements.   These
initiatives include the  organization  of telephone  conferences to coordinate
work between EPA  personnel  in  OAQPS  and  in the  Regional   Offices,  and  the
preparation of written quality assurance guidance  for EPA and State personnel.
A workshop for State and Regional  project managers was held  on  October  24  and
25.  OAQPS will maintain contact with the Regional and State project  managers
throughout the  remainder  of   the project to  follow  up on  specific  problems
that develop.

     Work is also planned to  improve the methodology for  calculation of NEDS
area source  emissions  to ensure that  all   significant source categories  of
emissions are  accounted  for.   Development  of  an  improved methodology  for
highway vehicles  is also anticipated.   This  is necessary to  improve  the
accuracy of the emissions estimates for this source  category   which  accounts
for about one-third of  national  NOX and VOC  emissions.   The new methodology
will produce  better estimates  of   vehicle-miles  travelled  to be  used with
MOBILE3 emission factors to  calculate emissions.

     Finally, the NEDS  point and  area   source  data  developed  by  the  States
and NADB will  be  processed   by  NAPAP to produce the  spatial, temporal,  and
species resolution  of emissions  needed   by  NAPAP.  The procedures for  accom-
plishing this have been  described by Fred Sellars  in the paper titled  Develop-
ment of an Emissions Inventory to Support Testing of the Eulerian Regional
Acid Deposition Model.
                                  CONCLUSION
     The management strategy developed  by  EPA  represents a strong  commitment
to achieving NAPAP's goals  for  a 1985 emissions  inventory.  This  effort has
the highest priority of  any emission  inventory  project  conducted  since the
initial  development of  NEDS  in the  early  1970's.   To  achieve the desired
goals will  require an  intensive and coordinated effort  by  the  States and EPA,
The expectation is  that  the inventory data  developed  will be the  best ever
during the  time NEDS has  been in existence.

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                  STATE EMISSIONS INVENTORIES
                        1985 NEDS FILES
                S02,  NOX,  CO,  VOC,  PARIICULATES
   STATE
 ASSISTANCE
 EMISSIONS INVENTORY
  SYSTEM FOR POINT
  AND AREA SOURCES
   SPECIES
 ALLOCATION
   FACTORS
INVENTORY IMPROVEMENTS
     AND ADDITIONS
CANADIAN
INVENTORY
EMISSIONS
FACTORS
HOURLY EMISSION
    PROFILES
SPATIAL SOURCE
 ALLOCATIONS
  DOE DATA
                             VERIFICATION
                                 TESTS
                              UNCERTAINTY
                              ESTIMATES
                                QUALITY
                               ASSURANCE
                 1985 NAPAP EMISSIONS INVENTORY
                (INCLUDES 40 POLLUTANT SPECIES)
         Figure 1.   Relationship Between State and NAPAP
                    Emissions Inventories for the 1985 Base Year
                                   93

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                ASSISTANCE TO STATES IN THE

                  DEVELOPMENT OF THE 1985

                 NAPAP EMISSION INVENTORY




                            by

               David Johnson and Mark Hodges
                Technical  Guidance Section
           U. S.  Environmental Protection Agency
       Office of Air Quality Planning and Standards
       Research Triangle Park, North Carolina  27711



                    EPA  Contract No.


                   EPA Project Officer:
           U.  S.  Environmental  Protection Agency
       Research Triangle Park,  North Carolina  27711
                      Presented at:

Second Annual  Acid Deposition Emission Inventory Symposium
                Charleston,  South Carolina

                   November  12-14, 1985
                              94

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                                 ABSTRACT
     The Environmental  Protection Agency (EPA)  is  working  with  the  State
and Territorial Air Pollution Program Administrators  (STAPPA) Acid  Rain
Committee to identify the capabilities and  needs  of  States  with  regard to
cevelopnent of tne 1985 National  Acid Precipitation  Assessment  Program
J.APAP; emission inventory.  A survey nas  been  distributed  to the  States
asKing them to determine what level  of inventory  effort  they could  provide
for 1985 given their current resources and  activities  and  what  types  and
levels of support are needed to ensure the  desired information  can  be
collected and submitted.  The results of the survey  will be used in
determining wnat type of assistance will be provided with  the additional
fjnds available for tnis project.
                                       95

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 Introduction

     The 1985 NAPAP emission inventory effort  will  call  on States to make
 a concerted effort to collect and submit emission-related  data.   However,
 since trie emission inventory development and maintenance activities and
 capabilities vary across the States, it is  necessary to  determine what
 assistance or support mignt be needed to enable all  States to produce
 consistent and high-quality emission inventory information.   Once these
 needs are determined, an appropriate strategy  to provide the assistance can
 be developed based on program goals and available resources,

 Background

     In June 1985, the Administrator of the U.S. Environmental  Protection
 Agency  (EPA) wrote to each State Environmental  Director  explaining the
 importance of the 1985 emission inventory and  the role of  States  in the
 development of the inventory.  The Administrator said that he was giving
 the 1985 inventory project a high priority  within EPA, and he urged the
 State Directors to also give the project high  priority in  their  States.
 The Administrator also commented that he realized that the inventory
 cevelopnent activities and capabilities varied across the  States  anc that
 trie critical needs associated with producing consistent  and  nign-quality
 emission inventories snould oe identified.   Once these needs were identified
 ways of satisfying tnese needs and solving  major problems  should  be
 determi ned.

     The Administrator stressed his desire  to  work  closely with  the States
 in aeternining their inventory capabilities and needs.  He stated that
 EPA's interface with the States would be through the STAPPA  Acid  Rain
 Committee, chaired by Mr.  Jim Hair.bright (head  of the Pennsylvania air
 program).  Staff of EPA first met with the  STAPPA committee  in April 1985
 to discuss the objectives  of the 1985 inventory project  and  how  EPA and
 STAPPA could work together to identify and  address  Stace inventory needs
 and concerns.  The STAPPA  committee and EPA agreed  that  a  greater'effort
 within the existing National  Emission Data  System (NEDS) context  could
 produce a worthwhile improvement in emission inventory information and
 that an appropriate way to determine the capabilities and  needs  of States
 would be through a survey.

     A survey was developed and mailed by STAPPA to the 48 contiguous
 States  and the District  of Columbia in July 1985.  The primary goals of
 the survey were to determine (1) what level of inventory effort  the States
 could provide for 1985,  given their current inventory activities  and
 resources and (2) what types and levels of  support  were needed to ensure
the States could provide the desired emission  inventory information.
                                    96

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-.esults CT~ tie STAPPA Emission Inventory Survey

     Tne survey drew an effective and widespread  response  from the  States.
Cut of tne -? surveys that were mailed, 42 had been returned  by October  17,
l'-S5.  Figure 1 snows the response in each EPA Region,  which  illustrates
cr, effective response to the survey across the country.  It  was also
evident mat nany States gave considerable time and effort  in  preparing
tneir  responses, with some States providing detailed estimates of man-hour
and material needs associated with the 1985 effort.  The following
ciscussion summarizes the results of the survey.

     Inventory Capabilities With Current Resources - The first primary
question of tne survey asked whether States would be able  to  provide  by
J'jly 1, 1986, the 1985 emission data for various  sources given the  States'
curnent inventory activities and resources.  States were asked to specify
v/netner they would be anle co provide emission data needed  for (a)  all,
'b' more tnar naif, (c) less than half, or (d) none of  the  sources  grouped
by jollutant and size categories.  The responses  of the States are  summarized
   r~,;ures 2-b.  Figure 2 illustrates that over two-thirds  of  tne States
cojld  provide the emission-related information tor all  sulfur  dioxide
"SI^.1  sources greater tnan 2,500 tons per year 'TRY) with  current resources,
?'. er rial* could provide tne data for SO? sources  greater than  1,000 TRY;
ana c.'er a tnird could provide the data for all S0£ sources greater than
I'.i-j TPr witnout needing additional assistance.  The most significant
cnan.je in tne distribution occurs when the size cutoff  is  lowered to  100
T^Y.   Considerably fewer States are able to provide data for  all sources
emitting more tnan 100 TDY of S0£, and most States could provide the  data
*•";.- only a portion or none of their sources.

     Figure 3 illustrates an almost identical  pattern in the  capability
of States regarding sources of oxides of nitrogen (NOX).  The  similarity  in
Figures 2 and 3 shows an expected pattern, which  is apparent  also for
sources of volatile organic compounds (VOC's), particulate  matter (PK),
and carbon monoxide (CO), that reflects the increasing  demands on State
resources as the size cut-off becomes smaller.  However, the  similarity
in a State's capabilities regarding S0£ and NOX sources also  results  from
the considerable overlap in sources; that is,  most sources  of  SOp emissions
sre also sources of NOX and vice ve^sa.

     Figure 4 snows the capabilities of States to provide  the  emission
data for VOC sources.  Figures 5 and 6 ->how the capabilities  of the
States to provide the emissions data fo  sources  of particulate and
carbon monoxide.  Although the patterns in the capability  of  States to
provide data for these sources are quite similar  to the patterns illustrated
in Figures 2 and 3 for SO;? and NOX, acrus: the board there  are fewer
States capable of providing data for al1 sources  of VOC, PM,  and CO in
the particular size categories.
                                     97

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  Figure  1.    SURVEY RESPONSES RECEIVED
                1985  NAPAP EMISSIONS INVENTORY
co
                           8
RESPONSES
   10
    9
    8
    7
    6
    4
    3
    2
    1
    0
                          EPA REGION  NUMBER
  Based upon 42 of 49 possible responses.
  October- 3O. 19R5
                 fe
x>
.-.-x
                          tx-^d  :<1  i>x

                                                           No reponse received
                                                        tV\
                                SResponse received

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  Figure  2.
VO
VO
STATVS
 45

 40

 35

 30 £•
    r
 25 F-
    I-
 20 [-

 .15 F.

 10 r.
    »-
  5 "•
ABILITY TO PROVIDE 1985 EMISSIONS
DATA FOR  S02  SOURCES
 (  NAPAP Emissions  Inventory  )
               IT * \ v  v ' V
                  \ \ \ \
                       \ x
               \
                                \ '  N '  N.
                              \
                              \
                                       \
                                                     ~.V\
                                                           F N
                                                           k  J
                                                      data
                                               100% Of  •ju.'.it'Ll;'/
                                                 vicio  u,ita fj
                                                    of ;iw;jfi.(.i

                                                   U:  cKit.i f»j:
                                                    Of S5uuri'.f;
                                                   Jt;  dcitei fo,
        jn -I.: jf -ili i.uvoii.'h. :•;.

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  Figure  3.
O
o
ABILITY  TO  PROVIDE 1985 EMISSIONS
DATA FOR NOx  SOURCES
 ( NAPAP  Emissions Inventory )
              NOx > 2500 tpy   NOx >  1000 tpy   NOx > 100 tpy

                         SOURCE SIZE CATEGORY
                                                             Provide data for
                                                             100% of sources
                                                             Provide data for
                                                             > 50% of sources
                                                             Provide data for
                                                             < 50% of sources

                                                             Provide data for
                                                             0% of sources
  Based upon 42 of ^9 total possible r-esponses

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Figure  4.
      STATES
       45
       40

       35

       30

       25

       20

       15

       10

        5

        0
ABILITY TO PROVIDE  1985  EMISSIONS
DATA FOR  VOC  SOURCES
 (  NAPAP Emissions  Inventory  )
             VOC > 2500 tpy   VOC > 1000 tpy   VOC > 100  tpy

                         SOURCE SIZE CATEGORY
Based upon 42 of 49 total possible responses.

October 30.  1985
                                                Provide  data for
                                                100% of  sources
                                                Provide  data for
                                                > 50% of sources
                                                Provide  data for
                                                < 50% of sources
                                                Provide  data for
                                                0% of sources

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    Figure 5.
o
PO
ABILITY  TO PROVIDE  1985  EMISSIONS
DATA FOR PARTICULATE MATTER SOURCES
 ( NAPAP  Emissions Inventory )
                PM > 2500 tpy    PM > 1000 tpy    PM > 100 tpy

                          SOURCE SIZE CATEGORY
        upon 42 of 49 total possible responses.
                                                             Provide data for
                                                             100% of sources

                                                             Provide data for
                                                             > 50% of sources
                                                             Provide data for
                                                             < 50% of sources

                                                             Provide data for
                                                             0% of sources

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o
Co
          Figure  6.   ABILITY  TO  PROVIDE  1985  EMISSIONS
                        DATA FOR CARBON  MONOXIDE  (CO)  SOURCES
                        ( NAPAP  Emissions Inventory  )
        STATES
          40
          35
          30
          25
15


10


 5
                         \

                      \
                      \
                                        *T^
                                                - -4
                                                >
                     CO > 2500 tpy        CO > 1000 tpy

                          SOURCE  SIZE CATEGORY
  Based upon responses from 40 of 49 total
                                                  ' ";Provide data for
                                                  :> ..\ 100% of sources
                                                  •'' ~; Provide data for
                                                  ':. ,.'> 50% of sources
                                                  ^•T7>Provide data for
                                                  K'.-..J< 50% of sources
                                                     Provide data for
                                                     0% of sources
          necnnn'

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     It sno.ild be noted that these figures are based on the number of
3tatfs"r-es;,e cifferent.  For example,  Figure 7 illustrates the number of
sources and emission points associated with  the States' ability to provide
e-.issicn cata for sources emitting more than 2,500 TRY of SOj.  In this
case, considering either the number of State responses or the associated
plants or points'would seem to have the same implications for the coverage
of emission sources.  However, for NOX (see  Figure 8), the implications
are efferent depending on whether State responses or number of plants or
points are used.  Still, neither of these figures show what portion of
tr.e total inventory would be accounted for,  which could have other
^-plications for resource allocation.  All of these variables will need
to be considered as further evaluation of the surveys occurs.

     In acdition to oeing asked about their  being able to provide the
;ssired emission information,  States  were askea whether they could also
...,	. -,._, ^vission estimates with their S02 and NOX sources.  Figure 9
•  • ;5f = tes ''c-.' HC"_; Steles could  confirm the emission estimates they
         a: 1 ^ to c-> e", 01 for sources  emitting more than 2,SOU TRY of SC^.
          e, of tne 26 States  that would b.e  able to develop emission
£it:-,£.tes for all sources emitting over 2.5UU TRY of SOj, 21 would be
aL.le to confirm t'icse estimates and five States would be able to confirm
tie estimates of only a portion or none of those sources.  Figure 10
i  "i: jstrat&s similar confirmation capabilities regarding SG£ sources
er-ittirg more than 1,000 TRY.   The responses regarding NOX sources were
similar.  One indication of these  figures is that almost all States that
would be able to estimate emissions for all  their sources would be able
to confirm tnose emissions, whereas those" States who could estimate
emissions for only a portion of tneir sources would be able to confirm
emissions for only a portion of those sources.

     Amount and Type of Assistance Needed -  If a State would need assistance
in providing the 19R5 emission inventory information that was needed, it
was asked to determine the amount  of  assistance (in man-hours and material
costs)  that would De needed to (a) develop and confirm emission estimates
for sources emitting more than 2,500  TRY of  SO? or NOX; (b) develop
emission estimates for sources emitting more than 100 TRY of SO?, NOX, or
''••'".;  and 'r] -e/^0p emission  estimates for  sour.es emitting more than
i'Ju TRY of ?\\ or l.Juu TRY of  CO.   Figure 11 presents the total requested
assistance associated with these three levels of inventory development.
Of the total  S2.05 million requested, about  20 percent or 5410,000 would
Dr: needed to develop and confirm emission estimates for sources emitting
Tore than 2,500 TRY of S02 or  NOX.  Over half of the amount requested
w:uld^he used to develop the emission estimates for sources emitting more
t1^  1'JO 1DV of SOj, NOX, or VOC,  and about  a fourth would be needed for
-••
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 Figure  7.   ABILITY TO  PROVIDE  1985 EMISSIONS
              FOR  S02 SOURCES  >2500 TRY
              ( NAPAP Emissions Inventory )
PERCENT OF TOTAL
   100% r
                                         Provide data for
                                         100X of sources

                                         Provide data for
                                         > 50% of sources

                                         Provide data for
                                         < 50% of sources

                                         Provide data for
                                         0% of sources
                           105

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Figure 8.   ABILITY TO  PROVIDE  1985  EMISSIONS
             FOR NOx SOURCES  > 2500 TRY
              (  NAPAP Emissions Inventory  )
PERCENT OF TOTAL
   100X
     90


     80


     70


     60


     50


     40


     30


     20


     10


     0
Provide data fop
100% of sources

Provide data for
> 50% of sources

Provide data for
< 50% of sources

Provide data for
0% of sources
                           106

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      Figure 9
STATE RESPONSES
     30


     25
     20


     15


     10


      5


      0
ABILITY TO  CONFIRM 1985 EMISSIONS
FOR  S02 SOURCES  > 2500  TRY
 ( NAPAP Emissions Inventory  )

                              R vConflri 100X of
                                 Confirm > SOX of
                                 sources
                                 Confirm < 50% of
                              Sii sources
                                       none of
                                 sources
                                                   Provide data fnr
                                                   100X of sources

                                                   Provide data for
                                                     50X of sources

                                                   Provide data for
                                                   < SOX of sources
I                                                    Provide data for
                                                    OX of sources
             STATE  CAPABILITIES  TO  PROVIDE
              DATA    (  Numbers  of  States )
                                 107

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      Figure  10
ABILITY TO CONFIRM  1985 EMISSIONS
FOR  S02 SOURCES  > 1000 TRY
 ( NAPAP Emissions Inventory )
STATE RESPONSES
     25


     20


     15


     10


      5


      0
                                 Confirm none of
                                 sources
                                 Confine > SOX of
                                 sources
                                 Confirm < SOX of
                                 sources
                                ! Confirm 100X of
                               _ sources
                                                      Provide data for
                                                      100X of sources

                                                      Provide data for
                                                      > SOX of sources

                                                      Provide data for
                                                      < SOX of sources

                                                      Provide data for
                                                      OX of sources
            STATE CAPABILITIES  TO  PROVIDE
              DATA   ( Numbers  of  States )
                                   108

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            Figure 11
LEVEL OF ASSISTANCE REQUESTED  TO
DEVELOP 1985 NAPAP INVENTORY
>100 tpy S02/NOx/VOC~55X^
                                                   >2500 tpy S02/N0x~20%
                                                 PM and CO--25X
                          Total Assistance Requested =
                                 $ 2. 052, 688

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     A'- ir.r^rtant indication from tnese numbers is that, based on the
 •.••-.-.-. =1 State calculations, available funds (about SI million) could
 •.:"::ariv support tne level of assistance needed to ensure the development
 :'" e~:ssi;^ in. entries o* sources emitting more than 2,500 TPY of 502 or
 vjx.   nowever, the remaining funds do not appear sufficient to ensure
 aae^ate coverage o* sources emitting more than 100 TPY of S02, NOX, VOC,
 zr ?'•'  or l.OOJ TPY of CO.  Subsequent evaluations will  determine whether
 tne  assistance needed can be provided in a way to produce considerable
 cost savings, whetner the data and inventory needs should be modified, or
 wnetier additional funding sources should be sought.

     T?i s a-.e tvpe o'~ information on assistance requested has been summarized
 cr> a Regional sasis.  Figure 12 shows that acquiring emission data for
 so,rces"e~itv>.3 -lore than 100 TPY of S02, NOX, or VOC accounts for the
 largest portion of requested assistance in almost all EPA Regions.

     It is interesting to note that the 20 percent of requested assistance
 fjr  nevelopiny e^ssi'jn aata for the large 502 and NOX sources would help
 =•-,„'= tiat o.er j'j percent of S02 point source emissions ana over 80
 .-'_--.; a*' '. jr po^"-t soijrce emissions are ccvered in the -'nventory effort.
 5:-.  r'-j'e lj.  •':•- fie jtner na^cj, tne assistance requestea for S02. NOX,
 c_nj:  v^C sources ^rtr.ter than 10'J TPY would be associated with less than
"..Percent of t^c S02 point source emissions and less than 20 percent of
 f=  '.0A e:--,-; ssi 3rs.  It is important to add, nowever, that tnis later
           : also address about 95 percent of tne VOC point source emission
     As e>,;;e:tec, tne level  of assistance needed generally increases with
*."e r'-"t:er of so^-ces ?. State has, although there are exceptions.  Figure
1 •* ""i^strates tne req'jestea assistance for developing the inventory for
sources err.tting nore than 2,500 TPY of 862 and NOX as a function of the
ij-ner of those sources in the State.  Further evaluation reveals that
tie cost ^er source is widely variable and, if any trend can be discerned,
it is generally constant over the range of the number of sources per
State.  Fi^'jre 15 shows the wide range for cost per source associated
w-tn the assistance requested for sources emitting more than 2,500 TPY
SO? or ;,0r.  A similar graph for developing the inventory of sources
e' ittiry nortf tnan ijj -PY of 502, NOX, VOC, or PM or 1,000 TPY of CO is
s'uwn in Figure 16.  A slight downward trend is shown by the regression
ana1ys-is, rut the >:ide range in costs per sources is apparent.

     States indicated tnat most of the assistance needed would involve
aata eaiting and quality assurance activities, data collection from the
screes, or data processing to enter the data into the State files.
Mgure 17 illustrate  the responses of the States, given the seven categories
listed.  States also  indicated a preference for receiving direct supplemental
-r2nt assistance as opposed  to contractor support.  See Figure 18.
                                    110

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          Figure  12
LEVEL OF  ASSISTANCE  NEEDED FOR
1985 NAPAP INVENTORY EFFORT
 ( by EPA  Region )
% OF TOTAL REQUESTED
       10
                            v   vi
                            REGION
           VII VIII  IX
X
                                                       > 2500 tpy
                                                       S02 or NOx

                                                       > 100 tpy
                                                       S02. NOx or VOC
                                                       > 100 tpy PM and/or
                                                       > 1000 tpy CO
October 17. 1985

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          Figure 13.    COVERAGE OF  EMISSIONS  INVENTORY  AT
                          TWO  LEVELS OF  ASSISTANCE
  PERCENT  Or TOTAL
        100

        90

        80

        70

        60

5       50

        40 L

        30

        20

        10
                              0

                    > 2500 tpy         MOO and <2SOO tpy +

                          SOUrlCrJ S1ZK CUT-OFr
 *   Point sources only.  (1980 NAPAP  Inventury)
 +   > 100 tpv VUG
 October 16.  1985
Percent of Total
Funds Requested

% Total S02 *

% Total NOx x

1. lotal VOC
> 100 tpy

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        Figure  14.    NUMBER OF  S02  AND  NOx  SOURCES
                       > 2500 TRY  vs.  LEVEL OF
                       ASSISTANCE REQUESTED *
LEVEL Or ASSISTANCE REQUESTED  ( $ ) .
    25. 000 r

               *
20. 000
15. 000
10. 000
  5000

    o
     0
    ^    *   :

      *
• ^ i   '   i  •  i
  10   20    30
                        *

                       ,-*
                             i
                            -10
                                                 *
-1
70
                               bO    60    70    80

                   NUMBER Or  SG2 AND NOx SOURCES

Overlap may nave occurred in adding S02
                                                       $ as  f (# sources)
90    100

-------
        Figure  15.
          COST PER  SOURCE
           (>2500 TRY S02 or  NOx)
          AS  FUNCTION OF NUMBER OF SOURCES  *
COST PER SOURCE  ( $ )
      600 r
      500
      400
      300
      200
      100
       0
                           A
  A
                    A
             A
                           A
                   A
 ....A.
 A
                                             -A-
                                             A
                   A
                     A
    A
                        A
                                   A
           A
        o
10
                20   30   40   50    60   70   80

                  NUMBER OF S02 AND NOx SOURCES
Overlap may occur in adding SO2 and NOx
90
                                             Cost per source
                                            (as f (#  sources))
                                                 	A	
100

-------
Figure  16
COST  PER SOURCE ( $ )
      1000 r
      900 -

      800 -

      700

      600

      500

      400

      300

      200

      100
          O
        O
       O
  b    o
   - o
      O
                      COST PER SOURCE,  TOTAL  INVENTORY
                       (  MOO  tpy  S02,  NOx,  VOC and PM,  and
                      >1000 tpy CO )
                O
          o
                  GOO
                                                            Cost per source
                                                           (as f (# sources))
O
              i . . . . i . . .
        0
                  TOTAL NUMBER OF SOURCES  (by State)
  Overlap may occur  in adding S02 and NOx
  t*ni innPQ

-------
                 Figure  17.    TYPES  OF  ASSISTANCE NEEDED
                                    (  1985  NAPAP  INVENTORY  )
                    DATA PROCESSING TO ENTER
                    DATA INTO STATE SYSTEM/
                    FILES - 22%
     DATA PROCESSING TO
     PRODUCE NEDS SUBMITTAL -
     9%
    SOFTWARE CHANGES TO STATE
    SYSTEM TO PRODUCE NEDS
    SUBMITTAL - 4%
                                                               OBTAIN DATA FROM
                                                               SOURCES - 21%
OTHER - 6%
                   DATA EDITING/QUALITY
                   ASSURANCE - 23%
                                                           CALCULATION OF EMISSIONS
                                                           ESTIMATE - 15%
42 of 49 total possible responses received

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Figure  18.
ASSISTANCE  REQUESTED BY  STATES FOR
1985 NAPAP  INVENTORY
 ( by Type and Amount )
   Section 105—68%
                                 Section 105—75%
                              Other—9%
                            Both—9%
               Contractor—15%
       PROPORTION OF STATES REQUESTING
          ASSISTANCE. BY MECHANISM
                                                              Other—IX
                                                             Both—18%
                                      Contractor—6%
                           AMOUNTS REQUESTED.  BY
                                MECHANISM

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     Alnost all States noted that they would not be able to submit the
.lislr&a cata significantly before July 1, 1937.  Nineteen iI3; States
in-icatea t^at tneir requests ^or assistance would oe reduced if two or
t.-iree accifio.nal  months were allowed for their subnittal.  See Figure 19.
Eignt of inese 19 States were able to estimate a total reduction in
resource requirements of about $325,000; the other States did not provide
estimates of reductions.

Process for Providing Assistance

     The survey responses will  be used to determine the types and levels
or assistance needed by States  to provide the desired  emission data.
-!.>out SI million (S500K in Section 105 funds and S500K in NAPAP funds)
are available to provide direct  financial  assistance to States or to
ueveiop appropriate contractor projects to satisfy the needs of tne
States.  In addition to the survey responses, follow-up discussion with
States and Regional  Offices will  be used to identify alternative approaches
*or providing tne assistance needed.  The alternative  approaches will be
•'•-I/1-;wec wit'; tni STn^PA committee, and a final  plan for providing tne
*;si5tenct '."11 be ctveloped.  By December 1935, appropriate grant
-.•'•i":~er.ts to States sroulc be made and contractor projects  should 3e
developed.
                                    118

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•JO
              Figure  19
        OF STATES

         25 r
          20
          15
          10
WOULD ADDITIONAL TIME REDUCE

RESOURCE  REQUIREMENTS ?
                                    15
  fx>x-^x^:^x^
  ^.,\>-S,y^\
  ^X--;\'X<-:
  f\ \ •«. xX \ . . yx ' y **
  rvX^c/vA^Xi-c-^
                   Yes
K&M^&S^

     No
                  Not Applicable

-------
       SESSION 3:   FORMULATION OF MAN-MADE  POLLUTANT EMISSION FACTORS

Chairman:   Dale Pahl
           Air and Energy Engineering  Research  Laboratory (MD-61)
           U.  S.  Environmental  Protection Agency
           Research Triangle  Park,  NC   27711
                                     120

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           DEVELOPMENT OF NAPAP EMISSION FACTORS

                 FOR ANTHROPOGENIC SOURCES
                            BY
                       J.B. Homolya
                    Radian Corporation
                      P.O. Box 13000
             Research Triangle Park, NC  27709
                EPA Contract No. 68-02-3994
                  Work Assignment No. 32
                   EPA Project Officer:
                      J. David Mob ley
       A1r and Energy EnglneMng Research Laboratory
                Research Triangle Park, NC
                       Presented At:

Second Annual Add Deposition Emission Inventory Symposium

                      Charleston, SC



                   November 12-14, 1985
                           121

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     DEVELOPMENT OF NAPAP EMISSION FACTORS FOR ANTHROPOGENIC SOURCES
                            BY:  J.B.  Homolya
                           Radian Corporation
                                ABSTRACT

     The NAPAP emissions  Inventory  activities from 1980 to  1985  have
Included  the  development of  anthropogenic emissions  Inventories  to
support  the formulation  and testing  of  an  Eulerian  atmospheric
transport,  transformation,  and  deposition model.  The  model  requires
high levels of species* temporal, spatial, and  sectoral  resolution for
emissions Inventory Input parameters.   A numhar of the pollutant species
Included  1n the  Inventory  development  required  the  formulation  of
source-categorized  emission  factors   which   were developed   from
assessments of data  available in the  literature.   To date,  detailed
emission  factor  assessments have been  prepared  for  primary sulfates,
ammonia, hydrochloric acid,  and hydrofluoric  acid.  For  certain source
categories,  the  assessments  were  compared  with  additional   stack
measurements conducted to address data gaps or to verify the  quality of
the emission factors.  An assessment  of alkaline dust emission factors
has pointed to  the need  for  both detailed chemical  composition  and
particle size distribution  data to  support emission factor  development.
Ongoing  research is  addressing  this  need and   providing  further
development of VOC emission  factor data needed to support the 1985 NAPAP
emissions Inventory.

                              INTRODUCTION

     The Eulerian acid deposition model currently being developed  by the
National Center  for Atmospheric Research  requires emissions data  based
on certain chemical  species  which act as direct  acidic emissions to  the
atmosphere, scavengers of primary or  secondary  adds  1n  the atmosphere,
or catalysts  1n  atmospheric  transformation  processes.  Most of   the
chemical compounds or  classes of  compounds needed for  input into the
modules describing chemical  transformation and deposition processes
                                    122

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are  non-criteria  pollutants.   Because  of this, limited  Information  is
available  concerning  emission  factors  for  most  of  these  species.
Therefore, an  anthropogenic  emission  factor development program within
NAPAP was designed to formulate appropriate  emissions  Inventories using
the  best  pollutant  speclatlon  data  available.   Emission  factor
development was  Initiated In  1983  with  the preparation  of  emission
factor assessments for primary sulfate ,  ammonia,  hydrochloric add,  and
hydrofluoric add.   These species  were  selected  because they are the
priority  pollutant species required  for  use 1n  both Lagranglan modeling
projects  and the preliminary development of the Eulerian model.
     The  assessments  began with  a  review  of  a compilation  of  data
available 1n the  literature.   Where  data  were  Incomplete,  a  series  of
emission  tests were conducted  at  the Department of Energy, Pittsburgh
Energy Technology Center.  To date,  emissions tests have been conducted
for  bituminous  coal  combustion  omissions  of  HC1,  HF,  and  primary
sulfate.
     During  1985   preliminary  assessments  were performed  on  the
development of  point  source  alkaline  partlculate  emission  factors.
Emphasis  was given to  the consideration of  particle  size distribution
and  the  chemical   cctnposltlon  of  the  alkaline  fraction of  total
particulate emissions.   Further,  source categories  were Identified which
require the development  of VX emission  factors.   Priorities  have been
assigned and Incorporated 1n an implementation  plan for data  gathering.
     This paper summarizes the current  results of the  NAPAP  emission
factor development program by presenting tabulated  estimates  of  emission
factors derived for  the above species.   The estimates  are  provided
according to  source  classification  code  (SCO  format  and  Include
emissions calculations for 1980.
                                  123

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                        PRIMARY SULFATE EMISSIONS

     Sulfur present 1n fossil  fuels  1s emitted to the atmosphere mainly
as  SO  .   However,  some  of  the sulfur  1s oxidized  further  1n the
combustion  process and  1s emitted as primary sulfate  compounds.   The
largest source of primary sulfate emissions (PSE) is from the combustion
of  coal  and oil.  The  amount of  primary sulfates  emitted  from  a
particular  combustion  source  is  dependent  on a  number of  factors
including  fuel  type  and  composition,  combustion  equipment   design,
operating parameters,  and emissions controls.
     A  significantly  higher conversion  of fuel  sulfur to  primary
sulfates occurs during oil firing as compared to coal firing.  Enhanced
PSE from oil combustion are  due to the low ash,  fast burning  properties
of fuel oil.  Also, many  residual oils contain high  levels of vanadium
which can catalyze the formation  of SO.  in a furnace.
     Sulfates are  formed  in combustion processes  1n both the  flame
region and  downstream in  the heat transfer  section.  The major primary
sulfate formation mechanisms include oxidation of S0_ to SO.,, hydration
of SO, to H_SO., corrosion  of  boiler internals by H_SO., and  conversion
of metallic oxides 1n fuel  ash to  particulate sulfates.   In  combustion
flames, the predominant  sulfate  formation  mechanism 1s  reaction  of
molecular oxygen to form  SO-.  The final  SO.,  concentration leaving the
flame zone  depends on 0_  concentration, cooling  rate,  and  the location
and rate of mixing of  excess air.
     Increased PSE can be  affected by the heterogeneous catalytic
oxidation of S0_ by metals,  metal  oxides, and soot  suspended 1n  the
stream of  combustion  gases  or deposited  on  boiler  internal  surfaces.
Residual   fuel  oils from Venezuela  and  the  Middle East contain
significant amounts of  vanadium  which  1s liberated as V^O,.  during
combustion.   V_05  has  been  used  extensively  in  the chemical
manufacturing  Industry,   as  an   oxidation  catalyst.   The  major
constituents of coal  fly  ash, S102 and  Al^.  are only  weak catalysts.
     SulfuMc add is  formed hy reaction  of  SO, with  water  vapor 1n
combustion product gases.  The acid can adsorb on ash or soot particles,
condense on cooler parts  of  the combustion  equipment,  or be  emitted  to
the atmosphere as a mist.   The SO.-to-H.SO.  conversion  is temperature-
and moisture-dependent.
                                  124

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REVIEW OF AVAILABLE PRIMARY SULFATE EMISSION FACTOR DATA BASES
     Prior to  the  current  need  for NAPAP Task Group B  to  Inventory PSEf
two  separate environmental program  activities have Included  assessments
of PSE factors for use 1n emissions Inventory development.  The Electric
Power Research Institute sponsored  a sulfate regional  experimental  study
which  included a  summary  of  existing measurements  data  on  primary
sulfates and  recommended  generalized  emission  factors  for a  number of
source categories.  Many of the factors were based upon an extrapolation
of a limited  data  set for uncontrolled fossil  fuel  combustion  sources
along with data contained 1n the EPA Emission Factor  Guidelines (AP-42).
     The United States/Canada Work Group 36 (WG 3B)  prepared an emission
Inventory  report  1n  accordance with  the Memorandum  of  Intent on
Transboundary  A1r  Pollution  of August  1980.   The report  Included  a
study   of  U.S.  and  Canadian  PSE  using  factors  abstracted from the
literature  along  with  unpublished  emissions  data  from  Canadian
measurements obtained from the use of a variety of sampling and analysis
methods.
     Following review of the EPRI and WG 3B sulfate  emissions data  sets,
an extensive literature review was conducted to Include al• contemporary
PSE  measurements  data in  a final   analysis  and tabulation of emission
factors appropriate for the NAPAP emissions Inventory.   Where available,
all  field measurements  using  the controlled condensation  system (CCS)
procedure were considered as  the   prime  data  set.   Emissions  data
acquired through the use of methods other than CCS were Included only  1f
multiple  measurements  yielded  precise   data.    Sulfate   emission
assessments were aggregated for different point  sources within  the  same
source category  only  1f  fuel  composition  and  emission controls were
similar.
     PSE factors recommended for use 1n the NAPAP Emissions  Inventories
are  listed 1n  Table  1.   The factors are  reported for  source  classifi-
cation codes  (SCCs)  and  reflect  sulfate emitted as  SO.   (molecular
                                                        4
weight = 96)  based on the chemical  analyses  of   source test  samples.
Much of the  current  data  set  1s  for  fossil fuel combustion 1n the
Industrial  and  utility  sectors which contribute  most  of  the regional
mass emissions of  primary  sulfates.   Table  1 also contains an estimate
of the uncertainty for each emission factor.  The estimates are based on
a Qualitative assessment of the representation of available  source  test
                                   125

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TABLE 1.   PRIMARY SULFATE EMISSION FACTORS FOR NAPAP EMISSIONS INVENTORY
Source category
Electric Utilities - External Combustion
Eastern bituminous coal
Western bituninous coal
Lignite
Residual oil (>li sulfur content)
Industrial - External Combustion
Eastern bituminous coal
Res i dual oi 1
Ccwiercial/Institutional - External Combustion
Residual oil (<-lX sulfur content)
Space Heating - External Combustion
Distil late oi 1
Industrial Process - Cheaical Manufacturing
H2S04-contact process
Industrial Process - Prinary Metals
Primary copper smelters
NEDS Source
classification
code (!,CC)
1-01-002
1-01-002
1-01-003
1-01-004
1-02-002
1-02-004
1-03-004
1-05-001-05
3-01-023
3-03-005-1
3-03-005-2
3-03-005-3
3-03-005-4
Control device
ESP
ESP and FGD
ESP
ESP and FGO
ESP
Fuel oil additive
Multiclones
Multiclones and FGO
Mult (clones
Multiclones and FGO
Fuel oi 1 additive
None
Deoister
ESP
ESP
ESP
ESP
Prinary sulfatei* Uncertainty
emission factor range*
0.385 Ib/ton
0.250T
1.290
0.761
1.951
5.439 lb/1,000
gal Ions
2 646 Ib/ton
0.462
5.296 lb/1,000
gallons
2.616
25.07 lb/1,0005
gal Ions
5.65 lb/1,000
gal Ions
0.100 Ib/ton
acid produced
22.5 Ib/ton
concentrated ore
1.08
5.76
15.66
A
C
8
C
C
B
8
C
0
D
C
C
B
C
C
0
0
                               (continued)
                                  126

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                                           TABLE  1.    Concluded
Sourct category
Industrial Process - Primary Petals (Cont'd)
Primary zinc smelters
Primary aluminum smelter
Iron production
Cokt
Industrial Process - Wood Products
Kraft pulp «i 1 1
Sulfltt pulp mill
Wood/bark wastt
Industrial Process - Mineral Products
Cement manufacturing
Cypsjmi rianufacturing
NEDS Source
classification
code (SCO
3-03-030
3-04-001
3-03-008
3-03-003
3-07-001
3-07-002
1-02-009
3-05-006 and
3-05-007
3-05-015
Control device
ESP
ESP
ESP
Baghoust
ESP
ESP
Hulticlones
ESP
ESP
Primary sulfateit
emission factor
55.5 Ib/ton
processed
0.5X of SO,
2. OX of SO,
0.320 Ib/ton
coal charged
»
**
3.6 Ib/ton
bark
TT
§*
Uncertainty
range*
0
0
0
0
c
c
0
D
0
Industrial  Process  -  Petroleum  Industry
  Fluid  crackers

  Sulfur recovery Claus plants
3-06-002

3-01-032
                                                                        ESP

                                                                        None
15.0 lb/1,000
 barrels 011
  2.8 Ib/ton
   produced
 * Estimated Mission factor uncertainty.   Assumes  that  90S of  the values for an individual  source He  within  the
   wan uncertainty estimates.   Corresponding values  are:  A =  tlOX; B = t25X; C = i50X;  and 0 = t75X.
 r Emission factor based on averagi sulfatt scrubbing efficiency of 35X.
 i Emission factor applicable cnly to low sulfur content  (0.3X  S) resiaual fuel  oil.
 I Total sulfate Missions for kraft pulp Bills  estiMted as B5X of NEOS total particulate missions  from  kraft
   recovery taoilers.
•• Total sulfatt Missions fro* sodluvbtst sulfite Bills estimated as 70X of NEDS SO, emissions;  for calciua-bas*
   sulfitt "ills tstiMted as 2SX of NEDS SO, Missions.
tT Total sulfatt Missions froe ceewnt kilns estimated as 5.6 Ib/ton of cemnt on an uncontrolled  basis.   Average-
   particulate control efficiency fro" N€OS data assused to apply in order to calculate actual Missions.
H ToUt sulfatt frot) gyptut) plants estimated as 56X  as  NEDS actual particulate Missions.
H  Although tt It  EPA policy to utilize  ••trie  untti. non-*»tr1c units have bewn used In this paper  since.  th«
    NAPAP emission  factor file  It In non-attr1c  unit*.  For conversion froa non-**tr1c units to oetric  units not*.
    that 1 Ib  - 0.4S3  kg and  that 1  ton (non-e»tr1c)  • 1  short ton - 2000 Ibt - 0.907 m*tr1c tons.
                                                          127

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data to the assignment of SCC-level factors.  Improvements are needed 1n
the  data base  for  low  sulfur  residual-oil-fired  industrial  and
commercial  boilers which  represent  a  significant  source of  sulfur
emission in major metropolitan areas in the eastern  U.S.   Also,  sulfate
emission  from  the pulp and  paper  Industry needs  further  refinement.
Pulp mill operations are concentrated  in  the acid deposition sensitive
Northeast and  represent a  major  SCL  and particulate source contributor
in the southeastern United States.

                       HYDROCHLORIC ACID EMISSIONS

     Table 2 lists the sources of hydrochloric acid emissions along with
emission factors  and estimates of  emissions for 1980.   Coal  combustion
is  the  largest   source   of  HC1  emissions,   accounting  for
467,000 ton/yr.
     Coal  is  formed over  eons  from successive  layers  of  fallen
vegetation.  As vegetation  accumulates,  physical  and chemical changes,
such as  loss  of  water and  volatile  matter,  occur.   Over time,  the
vegetation  turns  from  peat  to  lignite, the  earliest  stage  in  the
formation of coal.   As  lignite  is compressed with  deeper burial, the
heat ai Delated with the compression drives off volatile components.  As
more volatile components are  driven  off,  the rank  and  quality  of the
coal increase from lignite to subbituminous, bituminous, and anthracite.
The chlorine concentrations of domestic  coals vary over a large range.
The coal fields with  the highest chlorine content  are  in  the Illinois
basin.    The molecular form  of  chlorine   in  coal  is  not clearly
understood.  Chlorine  in coal exists  in  both  organic  and Inorganic
forms.   Although  1t has been  shown that chlorine occurs  in  coal  1n a
form more  volatile  than  sodium chloride,  no  correlation  has been
developed between the  molecular form  of  chlorine 1n  coal  and   its
combustion products.

COAL COMBUSTION IN UTILITY BOILERS
     There  are  three principal   types  of  coal-fired utility  boilers:
stoker-fired,  cyclone  furnaces,  and pulverized-coal-fired  (PC-f1red).
Of  the  three  types currently used,  PC-fired  is the most  common.
Scrubbers,  electrostatic  predpitators  (ESP), cyclones,  and  baghouses

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                                TABLE 2.  MAJOR  SOURCES  OF HYDROCHLORIC ACID EMISSIONS
ro
I-D

Source
Coal combustion
Utility and Industrial
bituminous
lignite
Commerc 1 al / 1 nst 1 tut 1 onal
anthracite
bituminous
lignite
Incineration
Municipal refuse
multiple chamber
single chamber
conical design- refuse
Industrial wastes
multiple chamber
single chamber
controlled air
conical design-refuse
Liquid wastes
Emission factor*
(Ib emitted/unit)


1.9
0.01
3.07
1.48
0.351


5.0
5.0
5.0
5.35
5.35
5.35
5.35
1.19
I960
Emissions
(ton/yr) SCC
467,000

1-01, 02-002
1-01, 02-003
1-03-001
1-03-002
1-03-003
75,000

5-01-001-01
5-01-001-02
5-01-005-07
5-03-001-01
5-03-001-02
5-03-001-03
5-03-001-04
NA
SCC units


ton burned
ton burned
ton burned
ton burned
ton burned


ton burned
ton burned
ton burned
ton burned
ton burned
ton burned
ton burned
ton burned
        * Although 1t Is EPA policy to utilize metric units, non-metric units have been used In this paper since the
          NAPAP emission factor file 1s 1n non-metric units.  For conversion from non-metric units to metric units note
          that 1 Ib ** 0.453 kg and that 1 ton (non-metric) = 1 short ton = 2000 Ibs = 0.907 metric tons.

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are  used  frequently  as flue  gas  control  techniques.   These control
devices are  effective  for  different pollutants and  often are used  in
combination.  An ESP or a  baghouse has no  demonstrated effect on HC1
emissions.   However,   alkaline  materials   are  sometimes  used  in
conjunction with a baghouse to remove sulfur compounds.  This could  also
result in a removal of HC1.
     Cyclones or centrifugal separators also are used  in  the control  of
particles from utility boilers.  Cyclones are assumed  to  have no effect
on HC1 emi ssions.
     Wet  scrubbers also  are used  to  remove particles  from  flue  gas
streams.  A  wet  scrubber  can use  a variety of  methods to  wet the
contaminant particles  in order to  remove them from the gas stream.  The
efficiency of a wet scrubbing device for HC1 emissions control should be
greater than  that  ?.   a baghouse  or ESP.    One  study demonstrated an
80 percent efficiency for HC1 removal  from bituminous-coal-fired utility
boi1ers.
     Gaseous  sulfur  compounds typically are removed  from  flue  gas
streams by flue  gas  desulfurization  (FGD) systems.   In FGD,  the sulfur
compounds are reacted with  an alkaline  substance.    The resulting
compound  then is removed  from  the flue gas  stream.  HC1 should  be
removed from  flue  gases  with FGD  systems;  however,  little  data  are
available to quantify the removal  efficiency.

COAL COMBUSTION IN INDUSTRIAL BOILERS
     Industrial boilers are smaller than utility boilers and  are used by
industry to  provide  steam  or  hot  water.  Only  10 to 15 percent  of the
industrial boiler  coal consumption 1s used  for  electricity  generation.
Coal burning  Industrial boilers are classified by heat transfer method,
arrangement of heat transfer  surface,  and fuel  feed  system.   The  three
types of heat  transfer systems  are watertube,  flretube, and  cast  iron.
Most  newly   Installed  Industrial   boilers  are  e.ther  watertube  or
firetube.   Fuel  feed  systems are  the  same  as  discussed under utility
boilers—stoker,  cyclone,  and PC-f1red.  Emission factors for HC1 have
not been  developed for industrial  boilers.   Emission factors  developed
                                   100

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for utility boilers can be used for Industrial boilers when the type  of
boiler and  fuel  are the same.  A1r pollution control technologies  for
industrial  boilers  are the  same as  those  discussed under  utility
bollers.
COAL COMBUSTION IN RESIDENTIAL BOILERS
     At the present time»  approximately  1 percent  of  the  nation's homes
are heated  with  coal.   Lignite is  burned for residential heating  in
North Dakota  only;  anthracite combustion is limited to  northern  states
east of  the Mississippi Riven with  64  percent  in Pennsylvania;  and
bituminous  coal  is  burned  In every  state except  Connecticut*  Delaware.
Maine, Maryland, New Hampshire, New Jersey,  North  Dakota, Rhode Island,
and  Vermont.   HC1  emission  factors   have  been  reported  as
60.5xlO~9, IZO.OxlO"9,  and 35.1xlO~9  Ib/Btu for  bituminous, anthracite,
and lignite combustion, respectively.

INCINERATION
     HC1   is emitted  during  the  Incineration of  wastes  containing
chlorinated hydrocarbons, chlorine-containing plastics such as polyvlnyl
chloride, and chlorine  or  chlorides,  often  1n the  form  of common  salt.
Incineration  1s  a  combustion process  used to change  the chemical  or
physical   characteristics of  waste  by  oxidation which, even under  ideal
combustion conditions,  results in  Inorganic solid  residues  and exhaust
gases.
     HC1   is emitted  as a result of  incomplete  combustion from three
types of  incinerators:  !1) municipal  incinerators that burn public
garbage;   (2)  municipally   owned  Incinerators  that  burn   primarily
Industrial wastes; and  (3) Incinerators  that  burn  liquid  wastes such  as
polychlorlnated waste, waste oil, and various other hydrocarbon 'liquids.
Emissions from the  public  Incineration  of  apn-   dmately  30x10  tons of
collected refuse  1n the United  States  1n  1.   produced estimated
emissions of 75,000 tons of HC1.   The emission factor for this source 1s
calculated as 5 Ib HCl/ton of refuse burned.
     Emission  factors  for  municipally  owned  Industrial  waste
Incinerators range from 2.0  to 7.0  Ib HCl/ton of wastes   burned with  a
mean value  of 5.35  Ib/ton.   Several sources were  tested  for  emissions
                                   131

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from Incineration of liquid wastes.   Emission factors from the test data
ranged  from  0.72 to  1.61  Ib  HCl/ton of  waste burned with  a mean
uncontrolled emission factor of 1.19 Ib/ton.

                       HYDROFLUORIC  ACID EMISSIONS

     Table 3 shows the major HF emissions sources and provides a summary
of  total  emlsslonst  emission  factors,  and  applicable SCCs.   Coal
combustion  1s  the  largest  source of HF  emissions*  accounting  for
58,000 tons/yr.  Fluorine present 1n coal  1s  converted to HF during the
combustion process and emitted to the atmosphere.  The effectiveness of
emissions controls for HF  1s  assumed to be similar  to that  discussed
previously for HC1.

PRIMARY ALUMINUM INDUSTRY
     The base ore for primary aluminum production 1s bauxite* a hydrated
oxide of  aluminum consisting  of  30  to 70 percent alumina  (AI^O,)  and
lesser amounts of Iron,  silicon,  and titanium.  Bauxite ore 1s first
purified  to  alumina  by the Bayer process,  and then  the  alumina  1s
reduced to  elemental  aluminum.  The production of  alumina  and the
reduction of alumina  to  aluminum are two  separate  processes,  seldom
accomplished at  the same  location.   Fluoride  emissions  from  primary
aluminum production  are from the reduction process only.
     Fluoride emissions  from  primary aluminum  production occur  1n the
gaseous phase as HF  with  a small  amount of silicon tetrafluorlde (S1FJ,
and  1n  the partlculate  phase as cryolite (Na-AlF,). The  ratio  of
gaseous to partlculate fluorides  varies with  the particular emission
point within the process.
     The principal points of HF emissions are the primary and  secondary
emissions from the potrooms housing  the reduction cells and,  1n the case
of the  prebake cell,  the  emissions  from the  associated  anode  bake
plants.   HF  emissions from  bauxite  grinding  and aluminum  hydroxide
production are negligible.  The manufacture of anodes for prebake  cells
emits HF from the fluorides 1n the recycled anode butts.
                                    132

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                                   TABLE 3.  MAJOR SOURCF.S OF HYDROFLUORIC  ACID  EMISSIONS
CO
CO

1980
Emission factor* Emissions
Source (lb emitted/unit) (ton/yr)
Coal combustion
Utility
bituminous
lignite
Industrial
bituminous
Commercial/ Institutional
anthracite
bituminous
lignite
Primary aluminum production
Anode baking furnace
Prebaked reduction cell
Prebaked fugitive emissions
Vertical Soderberg stud cells
Vertical Soderberg stud cells
fugitive emissions
Horizontal Soderberg stud cells
Horizontal Soderberg stud cells
fugitive emissions
Gypsum ponds
58,000

0.23
0.01

0.62-0.81

0.13
0.17
0.063
13,300
0.52
4.9
1.2
0.6

4.9
1.9

2.2
1.275 6,400
sec


1-01-002
1-01-003

1-02-002

1-03-001
1-03-002
1-03-003

3-03-001-05
3-03-001-01
3-03-001-08
3-03-001-03

3-03-001-10
3-03-001-02

3-03-001-09
3-01-016-02
SCC units


ton burned
ton burned

ton burned

ton burned
ton burned
ton burned

ton produced
ton produced
ton produced
ton produced

ton produced
ton produced

ton produced
tons P 05
produced

           • Although  It  Is  EPA policy to utilize  metric  units,  non-metric  units  have  been  used  In  this  paper  since  the
            NAPAP  emission  factor  file Is In non-metric  units.   For conversion  from non-metric  units  to metric units, note
            that 1  lb  =  0.453  kg and  that 1  ton (non-metric)  =  1 short ton =  2000 Ibs =  0.907 metric  tons.

-------
     All three types of reduction cells emit HF from  thermal  hydrolysis
of volatilized  bath  materials,  particularly  cryolite.  The reaction of
solid and vaporized fluorides at elevated tenperatures  occurs primarily
at the  point  where the hot gases escape through vents  1n  the crust  at
the cell  surface.   The hydrogen required for  the  formation of HF  1s
supplied 1n part from water vapor in the air.  Other sources  of hydrogen
Include residual moisture  1n  the alumina and  bath  raw materials  and
hydrocarbons  in the  carbon anodes.   The  HF emission factor for prebake
cells 1s the sum of the HF emission factors for the anode baking furnare
and the prebake reduction cell.

                            AMMONIA EMISSIONS

     Most  ammonia   emissions  result  from natural  and  biological
processes, primarily through the decomposition of  organic matter such as
dead  plants  and animal and  human  excrement.  Other  natural  sources
Include forest  fires  and  volatilization from  land  and ocean  masses.
Table 4 lists the  major sources  of  ammonia emissions.   Emission  factors
are given along with the total estimated emissions.

AMMONIA FROM LIVESTOCK WASTES
     The major  sources of  ammonia  emissions  from  the  production  of
livestock  Include  beef production  operations and  manure  spreading.
Production of  beef cattle can  be   divided  Into  four  stages:  calf
production, backgrounding,  finish feeding, and slaughtering.  The wastes
excreted by cattle grazing on pastures or range  areas are  disperse,
allowing the soil  to assimilate  the excrement.  However, manure produced
In feedlot situations  must be removed and processed  because of space
restrictions.   Animal  manure  contains complex carbohydrates,  protein,
and fats which are metabolized Into simpler compounds by microorganisms.
In the presence of  oxygen,  the end  products of metabolism are heat, 00^,
and H_0.  This  process, called  aerobic metabolism,  1s  dependent upon
temperature,  oxygen, and moisture.    In the absence  of oxygen, anaerobic
metabolism occurs with ammonia as an end product.
                                    134

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                                       TABLE 4.  MAJOR SOURCES OF AMMONIA EMISSIONS
o
n



Source
Livestock wastes
Manure field application
beef cattl 9
dairy cows
hogs
broilers
other chickens
Beef cattle feed lots
Coal combustion
Ammonium nitrate manufacture
Neutral izer
Solids formation

Emission factor*
(Ib emitted/unit)


34
71
7.5
0.47
0.47
2.1
2.0

0.86-36.0
0.54-33.4
I960
Emissions
(ton/yr)


1,900,000
390,000
240,000
920,000
56,000
24,000
525,000

3,100-130,000
920- 57,000


sec


NA
NA
NA
NA
NA
3-02-020-02
1-02, 02, 03

3-01-027
5-01-027


SCC units


per animal
per animal
per animal
per animal
per animal
per animal
ton burned

ton produced
ton produced

          •Although  It  Is  EPA  policy  to  utilize metric  units, non-metric units have been used 1n this paper since the

           NAPAP emission  factor  file Is In  non-metric  units.  For conversion from non-metric units to metric units, note

           that 1  Ib »  0.453 kg and that 1 ton  (non-metric) 3 1  short ton = 2000 Ibs = 0.907 metric tons.

-------
     Anmonia  is  emitted  from  beef  production operations as a result of
 anaerobic  decomposition  and volatilization  of  cattle wastes.   Anaerobic
 decomposition occurs in  the solid manure beneath the  feedlot surface, in
 manure  stockpiles,  and  1n runoff holding ponds.  Feedlot disturbances,
 such as mounding and manure removal, greatly  increase  the release of
 ammoniacal  compounds to  the  atmosphere.   Although  25  to 40 percent
 moisture  levels  are necessary  on  feedlot  surfaces  for  aerobic
 decomposition, too much  rain  or  watering,  resulting 1n  puddling and  wet
 spots,   can  trigger  increased  ammonia production.   In addition, about
 half of the nitrogen that cattle  excrete  is 1n the  form  of  urea 1n
 cattle  urine.  The urea  In  urine 1s hydrol1zed to  ammonia  and  can be
 released to the atmosphere.
     The spreading of livestock  manure on  agricultural  land 1s another
 source  of  ammonia emissions.   Field experiments  Indicate that,  when
 dairy manure was  spread  1n the field preparation  for plowing  under,  an
 85 percent  loss  of total  ammonia by  volatilization  occurred.  The dairy
 manure  volatilization rate may  be  applied to other  types  of  domestic
 livestock  manure.   The  ammonia  emission  estimates  from  the   field
 application of  livestock manure given  in Table 4  were derived  by
 multiplying ammonia excretion  rates by  animal population levels for 1980
 and by   the 85 percent loss factor.   Manure from beef cattle 1s the major
 source   of  these  emissions.   The total  emissions  estimate  for   ammonia
 from field application of livestock waste is 3.5 million tons.
 AMMONIA NITRATE MANUFACTURE
     Ammonia nitrate is produced by mixing nitric add and ammonia 1n a
 reactor or  neutral 1zer.  Either  ammonia or  nitric  add  1s  emitted from
 the neutralizing depending upon which reactant 1s added in excess to the
 process.  Most plants today  operate the neutral1zer with excess ammonia.
 An 83 percent aqueous  ammonium nitrate solution  1s  produced  1n  the
 neutral  1zer and  may be  sold  for  use  as  a fertilizer  or further
 concentrated for use 1n solid  ammonium  nitrate formation.
 COAL COMBUSTION
     Ammonia emissions  from  coal  combustion were  estimated  from a
 limited set of measurements data.   An  emission factor of 2 Ib  NH /ton
coal  burned was  applied  to  all  external  combustion boilers  for
anthracite, bituminous,  and  lignite fuels.

-------
                     ALKALINE DUST EMISSION FACTORS

     Anthropogenic  point source alkaline  participate  emission  factors
have  been calculated  from available  alkaline dust  emissions  data
reported  by  Meteorological and  Environmental  Planning, Ltd. and  the
Ontario Research  Foundation.    The emissions  data  were based  on  the
Identification of major  anthropogenic  sources  of partlculate Ca. Mg, Na,
and K  emissions.  Total  partlculate emissions from these  sources  were
estimated  along  with the amount of the  alkali ir.etals  contained 1n the
partlculate.
     Table 5  1s  a summary  of  emission factors for each alkali metal
assigned to  Individual SCC  categories.  Tho basic assumption 1s that the
alkali metal  contents of U.S.  and  Canadian  partlculate emissions are
Identical.   For power  generation and  fuelwood  combustion,  the emission
factors  are  assumed to  be applicable  for utllltyi  Industrial,  and
commercial/Institutional  source categories.   Additional refinement of
the  emission factors  should  Include  estimates of the particle size
distribution of the  alkaline partlculate emissions to  assess the  degree
to  which  the  particles   remain  suspended  1n  the  atmosphere as   a
neutralization sink  for  add.

                              VOC EMISSIONS

     Although total  VOC   emissions  have  been  Inventoried  by  the   EPA
within the  National  Emissions  Data System (NEDS),  the  EuleMan  add
deposition model  requires that  VOC  emission  must  be  disaggregated Into
refined  component species.   VOC emissions  must be  classified  by
photochemical reactivity  with the flexibility of varying the assignments
to a class depending upon the modeling chemistry used.
     Several  major SCCs  have either Incomplete or no VOC emission  factor
and speclatlon data.   Available emission  factor data are being  reviewed
to develop  the best  approch  to  fulfill  the  1985  NAPAP  Inventory
development needs.  The  program will  pursue  priorities for VOC  emission
factor development  which  reflects  NAPV  needs  and schedules,  the
availability of existing data,  and  the most effective use of project
resources to fill  current Information  data gaps.
                                    137

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     TABLE 5.   ANTHROPOGENIC  POINT  SOURCE  ALKA1INE  PARTICIPATE EMISSION  FACTORS
              Generic tource  «**crlpt1on
                                                    Unit*
Percenttge of total pcrtlcuUte
 e*)tulon «» *n «lk«)l  Bet*!*   Uncertainty
    C«     Hg      N«    K       r*t1nj«
3-03-023
3-03-006
3-03-006
3-04-006
3 -OS -020
3-05-016
3-05-020
J -05-025
3-05-006
3-OS-OU
3-05-00*
3-07-O01

1-01-001
1-01-002
1-01-OO3
1 -O2-001
1-02-002
1-O2-003
1-03-001
1-03-002
1-09-003
3-40-001
3-40-002
3-40-003
1-01-00*
1-02-009
1-03-00*
1-05-002-0*
3-40-00*
5-02-002-01
5-01-001
S-O 1-002-01
5-01-O05-O7
5 -02-O01
Iron ore alr'ng and benedclatlon
Iron and tteal Industry
Ferroalloy Manufacture
MagnealuB production
Mining and rock quarrying
I IB* Manufacture
Stone procMiIng
Sand and gravel
CMBMMt Manufacture
Concrete hatch toy
Cl ay products aanuf actur*
Sulfata (Kraft) pulping

Poeer generation by utilities











Fuelvood coMbuitton





Municipal Incineration



Ton* pellet* produced
Ton* produced
Ton* produced
Ton* processed
Ton* raw aaterlal
Ton* 11 MB* tone processed
Ton* ra» Material
Ton* product
Ton* ceaent produced
Tjn» processed
Ton* Input to process
Air dry tons until eacited
pulp
Ton* burned











Ton* burned





Tons burned



0.49
3.98
1.06
23.81
5.77
35.89
14.36
0.65
28.50
46.00
0.85

0.12
1.62











0.05





0.57



0.24
1.66
1.45
13.90
1.69
5.01
4.12
0.^0
0.78
1.50
0.90

0
1.71











0.04





0.14



0
1.74
1.35
0
0
o.so
0
0
0
0
0

1.38
0.82











0.04





0.57



0
5.63
0
0
0
0
0
0
0
0
0

0
0.44











1.95





0.46



E
E
C
C
0
c
c
0
B
C
0

c
c











E





E



 •Cx*>pl*:  for SCC  3-03-023.  e»1»»1oo* of *lktUne c«)du*> ptrttcultt* 
-------
                                  CONCLUSIONS

     Emission factors have been developed for point and area sources of
primary sulfate, ammonia, and hydrochloric and hydrofluoric acids for use in
the 1980 and 1985 NAPAP emissions inventories.  Preliminary alkaline dust
emission factors have been developed for anthropogenic point sources from an
emissions data set prepared in Canada.   Alkaline dust emission factors are
needed which consider the particulate size distribution and neutralization
capacity of each mass/size fraction.  Considerable additions and improvements
are needed for VOC emission factors and the level of speciation required to
support the development of the Eulerian chemical  transformation modules.

NOTE:  Although it is EPA policy to utilize metric units, non-metric units
have been used in this paper since the NAPAP emission factor file is in
non-metric units.  For conversion from non-metric units to metric units, note
that 1 Ib = 0.453 kg that 1 ton (non-metric) = 1  short ton = 2000 Ibs =
0.907 metric tons.
                                      139

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                               REFERENCES
1.   Homolya,  J.   Primary  Sulfate  Emission Factors  for  the  NAPAP
     Emissions  Inventory.   EPA-600/7-85-037 (NTIS  PB86-108263),  U.S.
     Environmental  Protection  Agency,  Research  Triangle  Park, NC,
     September L985.

2.   Homolya,  J.   "Stationary  Source  Emission Factor  Development,"
     presented at the First  Annual  Add Deposition Emission Inventory
     Symposium, Raleigh,  NC, December 3-4,  1984.

3.   Anthropogenic Sources and  Emissions of Primary Sulfates in Canada,
     Ontario  Research  Foundation,   Contract  No. 47SS.KE204-1-0318,
     November 1981.

4.   Anthropogenic Sources and  Emissions of Alkaline Particjlate Matter
     1n Canada, Meteorological  and  Environmental  Planning  Ltd.,  and
     Ontario Research Foundation,  Contract No.  52SS.KE145-3-0403, April
     1984.
                                  140

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        SIZE SELECTIVE PARTICIPATE EMISSION FACTORS

                 FOR EMISSION INVENTORIES
                            by

                      Frank M. Noonan
         Air Management Technology Branch (MD-14)
           U. S. Environmental Protection Agency
           Monitoring and Data Analysis Division
       Office of Air Quality Planning and Standards
       Research Triangle Park, North Carolina  27711
                    EPA  Contract No.


                   EPA Project Officer:
           U. S. Environmental Protection Agency
       Research Triangle Park, North Carolina  27711
                      Presented at:

Second Annual Acid Deposition Emission Inventory Symposium
                Charleston, South Carolina

                   November 12-14, 1985
                              141

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                  SIZE SELECTIVE PARTICULATE EMISSION FACTORS
                            FOR EMISSION INVENTORIES
                              BY:  Frank M. Noonan
                        Air Management Technology Branch
                     U. S. Environmental Protection Agency
                                    ABSTRACT

     Size specific Particulate Matter  emission factors have  been developed by
the U.  S.  Environmental Protection Agency  (EPA)  ao  a  result  of  source tests
performed on eleven  major  source categories.   Within each  source  category,  a
number of individual process operations have  been  characterized by particulate
matter size distribution emission rate  measurements,  along with  levels of source
activity.  In addition, size specific  emission  factors have  been developed for
source categories  based on information  in  EPA's  Fine Particulate  Emission
Information System (FPEIS)  and in published  literature.

                                  INTRODUCTION
     In order to  implement size  specific Particulate Matter National  Ambient
Air Quality Standards, the  U.  S.  Environmental Protection Agency has been dev-
eloping data bases for  source  categories,  through the combined efforts  of the
Office Of Air Quality Planning And Standards (OAQPS) and the Office Of Research
And Development (ORD), mainly ORD's Air And  Energy Engineering Research Labora-
tory (AEERL).  The primary  purpose  of  this  data base development is to produce
particle size related emission factors for  these source  categories  to  be used
principally by States  in developing State Implementation Plans when a revised
Particulate Matter  standard is   promulgated  by  the Agency.   These  emission
factors also can be employed in developing emission inventories.

     This paper  summarizes briefly the  source categories  for  which particle
size emission factors have  been  developed and made  available  or are presented
In draft reports  now undergoing  external peer  review before their publication
in EPA's Compilation Of Air Pollutant Emission Factors,  AP-42.
                                      142

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                                   DISCUSSION

     Size selective  particulate  matter emission  factor  information,  resulting
from U.  S.  Environmental  Protection  Agency's (EPA)  emission factor development
program, is  presented  in  terms of two efforts; (1)  completion  of  source cate-
gory reports based primarily on EPA sponsored source testing of selected source
categories, and (2)  particle size distribution  and  emission factor information
for additional  source  categories developed  from  data in the  Fine Particulate
Emission Information System (FPEIS) and from open literature.

     This source catsgoriee selected for testing are given in Table 1.  Table 2
lists processes  within each   of  these major   source  categories  and  presents
particle size  distribution data  from  2.5  to 10.0  micrometers.   Fugitive  dust
particle size  emission factor data  for  urban  paved  roads, unpaved  roads  and
industrial paved roads  are presently available in  the Fourth Edition  of EPA's
Compilation Of Air Pollutant Emission Factors, AP-42.  The  other  source cate-
gory reports  listed  in Table  2  are  in  the process  of  external peer  review
before publication of their emission factors in AP-42.

     Table 3 presents a list of additional source  categories for which particle
size data and  emission factors are being developed  from data  in the  FPEIS  and
open literature.  These factors  are  presently in  draft form  for external  peer
review.

                                   CONCLUSION

     Particle size distribution  data  and  emission  factors  have  been  developed
for eleven major  source  categories  and  a  list of  sources for which  data is
available as a  result  of  EPA's efforts.   Particle size distribution data range
from 2.5 to  10.0  micrometers.   Upon publication  in AP-42, these data  may be
used by States for emission inveitory and modeling purposes.
                                       143

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TABLE 1.  INHALABLE PARTICULATE PROGRAM SELECTED SOURCE CATEGORIES
                           PAVED ROADS
                   INDUSTRIAL AND UNPAVED ROADS
                          IRON AND STEEL
                        METALLURGICAL COKE
                          IRON FOUNDRIES
                            FERROALLOY
             PRIMARY AND SECONDARY  NONFERROUS  METALS
                         CEMENT AND LIME
                        ASPHALTIC  CONCRETE
                         KRAFT PDLP MILLS
                            COMBUSTION
                               144

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           TABLE II.  PARTICLE SIZE CHARACTERIZATION OF MAJOR SOURCE
                              CATEGORIES PROCESSES
IRON AND STEEL

     A source category report  for  iron  and steel presents particle size emission
factors for the following:

          "Sinter plant windbox - uncontrolled, and controlled
             with cyclone, scrubber, electrostatic precipitator
             (ESP) arJ baghouse

          "Sinter breakers - controlled with baghouse

          "Blast furnace casthouse - uncontrolled

          "Basic oxygen furnace (BOF) charging and tapping -
             uncontrolled, and controlled with baghouse

          "Basic oxygen furnace (BOF) refining (02 blow) -
             controlled with scrubber

          "Open hearth - uncontrolled,  and controlled with ESP

          "Quelle-Basic Oxygen Process  (Q-BOP) - uncontrolled,
             and controlled refining cycle with scrubber

          "Electric arc furnace - uncontrolled, and controlled
             with baghouse

          "Hot metal desulfurization -  uncontrolled, and
             controlled with baghouse
METALLURGICAL COKE

     The draft report presents particle size  emission factors for the following:

          "Coal preheating - uncontrolled, and controlled with
             scrubber

          "Coal charging sequential

          "Coke pushing - uncontrolled, and controlled with
             scrubber

          'Push cars in both travel and push nodes - controlled
             with scrubber

          "Coke quenching - uncontrolled (with dirty and clean
             water), and controlled with baffles

          "Coke oven combustion stacks - uncontrolled
                                      145

-------
IRON FOUNDRIES

     The draft report presents particle size emission factors for the following:

          "Cupola - uncontrolled, and controlled with baghouse
             and scrubber

          "Metal pouring and cooling - uncontrolled

          "Shakeout process - uncontrolled
FERROALLOY
     The draft report presents particle size  emission factors  for  the following:

          "50 percent FeSi open furnace - uncontrolled, and
             controlled with baghouse

          "80 percent FeMn open furnace - uncontrolled, and
             controlled with baghouse

          °Si metal open furnace - uncontrolled, and
             controlled with baghouse

          °SlMn open furnace - uncontrolled,  and controlled
             with scrubber

          "FeCr open furnace - uncontrolled,  and controlled
             with ESP.
PRIMARY AND SECONDARY NONFERROUS METALS

     The draft  report  presents  particle size distribution  information for  the
following operations in the primary aluminum, copper,  lead,  and secondary lead
smelting industries.

          "Primary Aluminum

               Fugitive particulate emissions from a prebake
                 plant - uncontrolled

               Fugitive particulate emissions from a horizontal
                 Soderberg plant - uncontrolled

               Prebake reduction cells - uncontrolled

               Horizontal Soderberg reduction cells - uncontrolled
                                      146

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'Primary Copper

     Multihearth  roaster  and  reverberatory  smelter
       operations  -  uncontrolled

     Reverberatory smelter  operations - uncontrolled
       and  controlled with  ESP

     Converter operations - uncontrolled and  controlled
       with ESP

     Reverberatory furnace  matte  tapping operation
       fugitives - uncontrolled

     Reverberatory furnace  slag tapping operation
       fugitives - uncontrolled

     Converter slag  and copper blow operations  fugitives
       uncontrolled

'Primary Lead

     Blast  furnace - controlled with baghouse

     Blast  furnace fugitives  - uncontrolled

     Ore storage  fugitives  -  controlled

     Sinter machine  fugitives - uncontrolled

     Reverberatory furnace  fugitives - uncontrolled

     Dross  kettle  fugitives - controlled

'Secondary  Lead

     Blast  furnace - controlled with baghouse

     Blast  furnace - (ventilation system fugitives
       from charging hood,  metal  and slag tapping
       hoods) - uncontrolled

     Blast  furnace (ventilation system as above) -
       controlled  with baghouse
                           147

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CEMENT AND LIME

     External peer review of the Portland Cement Industry and the Lime Industry
Source Category reports have been  completed.   Reviewer comments are under con-
sideration by EPA  and ORD  contractors  to accommodate these  comments and make
revisions, where necessary.  Particle  size distribution and  related emissions
factors are presented as follows:

          "Portland Cement

               Wet kiln - uncontrolled,  and controlled with ESP

               Dry kiln - uncontrolled,  and controlled with
                 multiple cyclone and baghouse

               Clinker cooler - uncontrolled,  and controlled with
                 gravel bed filter


          "Lime

               Rotary kiln - uncontrolled

               Rotary kiln - controlled  with cyclone, multiple
                 cyclone, ESP and baghouse

               Product loading fugitives - limestone into open
                 trucks and enclosed trucks,  and lime into
                 enclosed trucks
ASPHALTIC CONCRETE

     External peer  review  of  the  source  category report  is  completed.   The
report is presently being  revised  to reflect  reviewers comments.   The  report
presents particle size emission factors  for the following:

          "Conventional asphalt plant

               Stack emissions - uncontrolled,  and controlled
                 with  cyclone collector,  multiple centifugal
                 scrubber,  gravity  apray  tower  and baghouse

     "Drum mix plants  - uncontrolled, and controlled with baghouse
                                      148

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KRAFT PULP MILLS

     External peer  review  of  the  source  category report  is  complete.   The
report presents particle size emission factors for the following:

          °Direct contact evaporator (DCE) recovery boiler -
             uncontrolled, and controlled with ESP

          "Nondirect contact evaporator recovery boiler -
             uncontrolled, and controlled with ESP

          "Lime Iciln - uncontrolled, and controlled with
             venturi scrubber or ESP

          "Smelt dissolve tank vent - uncontrolled, and
             controlled with packed tower or venturi scrubber
COMBUSTION

     The source category report is currently in external peer review.  Particle
size emission  factors  for  the following  were presented  in  the draft  source
category report.
BITUMINOUS COAL

     "Dry bottom boiler - uncontrolled, and controlled with
        multiple cyclone, scrubber, ESP or baghouse

     "Wet bottom boiler - uncontrolled, and controlled with
        multiple cyclone or electrostatic precipator

     "Cyclone furnace - uncontrolled, and controlled with
        scrubber or ESP

     "Spreader stoker 'overfeed and underfeed) - controlled,
        and controlled 
-------
     "Spreader  sto* . r with and without  flyash  reinjection -
        uncontroi:  i, and controlled with multiple  cyclone,
        ESP, or  bit; louse

     "Spreader  st.-.er (overfeed and underfeed) - uncontrolled,
        and controj.led with multiple cyclone
SUBBITUMINOUS (LIGNITE) COAL

     "Dry bottom boiler - controlled, and uncontrolled with
        multiple cyclone

     "Spreader stoker - controlled, and uncontrolled with
         multiple cyclone
ANTHRACITE COAL

     "Dry bottom boiler - uncontrolled, and controlled with
        multiple cyclone

     "Stoker - uncontrolled, and controlled with cyclone
RESIDUAL OIL

     "Utility boiler - uncontrolled, and controlled with
        ESP or scrubber

     "industrial boiler - uncontrolled, and controlled
        with multiple cyclone

     "Commercial boiler - uncontrolled
WQOE WASTE

     "Bark boilers - uncontrolled, and controlled

     "Wood and b.irk boilers - uncontrolled, and controlled
                                       150

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  TABLE III.  ADDITIONAL SOURCE CATEGORIES FOR WHICH SOME PARTICLE SIZE

                 DATA AND EMISSION FACTORS ARE AVAILABLE
                  Combustion  in boilers
                       Bark/Sawdust Boiler
                       Wood Bark/Sawdust Boiler
                       Bagasse Boiler
                       Municipal Garbage Boiler
                  Off-Highway Diesel Internal Combustion
                  Automobile Spray Booth

                  Carbon Black Oil Furnace of Gas Boiler
                  Soap  and Detergents Spray Dryer

                  Sodium Carbonate*

                        Calciner
                        Trona Dryer
                        Dryer
                        Rotary Predryer
                        Bleacher Dryer

                  Cotton Ginning
                        Lint Cleaner Air Exhaust
                        Bactery Condenser
                        Saw Gin - Gin Stand and Bale Press
                        Roller Gin - Gin Stand and Bale Press

                  Feed  and Grain Mills and Elevators
                        Grain Unloading
                        Grain Elevators
                        Agricultural Feed Production

                  Ammonium Sulfate Fertilizer Bed Dryer
                  Ca^ob Kibble Dryer
                  Cereal Dryer
                  Rice  Dryer
                  Bauxite Processing
                        Ship Unloading
                        Fine Ore Storage Bin

                  Secondary Aluminum
                        Reverberatory Furnace Exhaust
                        Chlorine Demagging

                  Steel Foundries
                        Open Hearth Exhaust
                        Shakeout Hood Duct Exhaust
*AP-A2 Sections being updated.
                                     151

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    TABLE III (CONTINUED).  ADDITIONAL SOURCE CATEGORIES  FOR WHICH SOME

           PARTICLE SIZE DATA AND EMISSION FACTORS  ARE AVAILABLE
                     Lead Battery Manufacture
                          Grid Casting and Small  Parts
                          Casting Pot
                          Paste Mixing
                          Lead Oxide Mill
                          Element Assembly Operations
                          Assembly and Ball Mill  Processes
                          Reclamation Furnace

                     Bricks and Related Clay Products*
                          Screening and Grinding
                          Tunnel Kiln Exhaust
                          Sawdust Firing Brick Kiln

                     Coal Cleaning
                          Air Table
                          Thermal Dryer

                     Glass Manufacturing*
                          Furnace Exhaust

                     Glass Fiber Manufacturing
                          Flame Attenuation Forming Line
                            Exhaust

                     Phosphate Rock Processing
                          Calcining
                          Grinding - Ballmill
                          Oil Fired Rotary Dryer
                          Oil Fired Rotary and Fluidized  Bed
                            Rock Dryer

                     Taconite Ore Processing*
                          Main Waste Gas Stream

                     Fluorospar Processing
                          Rotary Drum Dryer

                     Petroleum Refining
                          Gas fired Boiler
                          Gasoline Cracking - CO  Boiler Exhaust
                          Gas Fired Process Heater

                     Wood Products Industry
                          Sanding and Sawmills
                          Belt Sander Hood Exhaust
*AP-42 Sections being updated.


                                     152

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      FIELD MEASUREMENTS STUDIES FOR THE DEVELOPMENT
             OF POINT SOURCE EMISSION FACTORS

                        J.M. Ekmann
                    DOE PTPA No. 5-083

                   DOE Project Officer:

                      Edward Trexler
                       Fossil  Energy
                 U.S.  Department  of  Energy
                       Presented at:


Second Annual Acirf Deposition Emission Inventory Symposium

                      Charleston,  SC




                   November 12-1H. 1985
                             153

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               FIELD  MEASUREMENTS  STUDIES  FOR  THE  DEVELOPMENT
                       OF  POINT  SOURCE  EMISSION FACTORS

                                 INTRODUCTION

     The models ander development  for  prediction of  acid  deposition require
detailed emission data  on a number of chemical  species.   These compounds or
elements may  act as  direct acidic  emissions  to  the  atmosphere  or  may be
involved in reactions  that  produce or  eliminate acidic  species.  Many of the
species in question are non-criteria  pollutants, and limited  information is
available concerning  emission  factors  for them.   Furthermore,  emission data
have  been  requested   at   levels  of   temporal  and   spatial  resolution  not
generally available.   A  number of projects  have  been developed  to address
the need for such data,  including  literature  studies and  field  tests.   This
project  largely  focuses   on   a  series   of   actual   measurements  for  two
particular  categories:  sulfate  emissions  from residential  and  commercial
combustion  of  fuel   oil;  and  emission  of   chlorine  species  from  coal
combustion.
     Projects  aimed   at  developing emissions  data  from   literature sources
identified gaps  in  available test data  for several  categories.1'    In the
area of sulfate emissions,  data  on sulfates emitted  from  the  residential and
commercial combustion  of  fuel  oil  were either  absent or  based  on analytical
approaches that have  been superseded  by more  reliable  techniques.   Data on
chlorine emissions  from combustion of coal were judged unreliable.   It was
felt  that  new  measurements  should  be  made  employing  recent advances  in
analytical techniques.

                             TECHNICAL APPROACH

     As  the  emission  Inventory requirements  include  spatial   and  temporal
resolution and some measures of  addressing uncertainty  in  the data,  a multi-
task project was initiated.  These  tasks  include the  following:

o    Ttsts for  sulfate  emissions from two boilers at  the  Pittsburgh  Energy
     Technology Center (PETC)

o    Tests for sulfate  emissions at  sites external to  PETC  that are typical
     of residential  and commercial  combustion  of No. 6 oil

o    A literature search  and data-base development  leading to information on
     the state or  regional distribution of vanadium  and   nickel  in  residual
     fuel oils and  the possible  impact  of these on  sulfate emissions

o    Tests for chlorine and,  incidentally, for  fluorine  emissions from coal
     combustion based  on  the  use  of  a furnace  simulator at the  Pittsburgh
     Energy  Technology Center  (PETC)

o    A literature search  to develop information on  the chlorine  content of
     U.S.  coals, and  calculation of the equilibrium distribution of chlorine
     species in flue gas

     The sulfate tests  at PETC  were  conducted  in  two package boilers;  a 20-
hp  fire-tube  boiler  (700 Ib/hr of  steam)  and  a 7CO-hp watertube  boiler
                                      154

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(24,000  Ib/hr  of  steam).   These boilers are typical of  those package boilers
widely  used  for  raising  steam  in  commercial  and  residential  applications.
Tests  were  conducted  in  the 700-hp  facility  for high-sulfur No.  6 oils at
two excess air  levels.  Data  are reported  for  four tests in the 20-hp boiler
on both  No.  2 and No.  6  oil.  For the  No.  6  oil test, two different excess
air  levels  were studied.   All tests were  conducted  at full load.   Samples
were drawn using  a  controlled condensation sampling (CCS)  train;  analysis of
the  samples   was  performed  using  ion   chromatography,   with   occasional
duplicate analyses performed  via barium-thorin titration.
     Field tests  were  conducted, through a  subcontract  to  Roy  Weston,  Inc.,
at  three sites:  a  residential site with  a boiler rated  at  1^5 RBtu/hr;  a
commercial  site  with  a  unit  rated  at 98 RBtu/hr;  and a  light industrial
facility  with a  boiler  rated  at  63  RBtu/hr.   Triplicate  samples  using the
CCS  method  were   taken   at   all  locations,  and   supporting tests  using  a
modified EPA  reference method 8  were  performed at  the commercial site.
     Studies   nave   shown   that  the   trace  metal  content  of  fuel  oils,
particularly  vanadium,  can affect the  conversion  of  sulfur  species  to  SO3. 3
As  extensive  data   to  quantify  this  dependence  are  absent,  a  literatur'
search  was  made,  through a  contract  with  Radian,  to  develop  data on  the
current  and  past  emissions  of  vanadium and nickel  from combustion sources.
These  data  were  used  to project  sulfate  emissions  as a  function of  the
variations  in  vanadium   content  and   fuel  use;   for one   state,   these
projections were  compared,  to the  sulfate  emissions calculated  from the best
currently available  emission  factors.   It  was  hoped  that  this  information
would contribute  to  uncertainty  estimates in this area.
     Chlorine  emission  tests were  conducted in  a coal-fir 3d  furnace  simu-
lator  having  a firing  rate  of 500 Ib/hr  of coal.  These  tests  were piggy-
backed  into a  series of tests  examining spray dryer/E?P performance in this
unit.   A  sampling train  was  used that allowed  us to collect all chlorine and
fluorine species.   The  train consisted  of  a glass-lined probe  inserted into
the  stack,  a  quartz fiber particulate  filter, and  an  impinger  train.   The
solutions in  the  impinger  varied with the  test method  chosen;  both  the "LA"
method  and  a  method proposed by  GCA were  used. "* > 5    Samples  were analyzed
using  ion chromatography.   Additional  samples vere  obtained or  samples were
split where appropriate and analyzed  using  the Volhard technique.1*
     Finally,  data   in  the literature  indicate  that  although  the  chlorine
content  of United  States, coal  is  low,  the actual chlorine content can vary
substantially  within a given  seam.   For  commercially  significant  coals in
the United States data  regarding the  chlorine  content and  its variation were
collected  from a  number  of literature  sources.    In  addition,  multiphase
equilibrium calculations  have  been   performed to  provide  a basis  for com-
parison with the experimental data.

                                   RESULTS

     Table 1   presents  the amount of  total  sulfur converted  to  sulfates for
the tests at  PETC.   Levels of  conversion  are  typical  of  equilibrium levels
at high  temperature with  the  exceptions of test  PS-06.  This test was run
after 30 hours of operation on  No.  6  fuel  oil  without cleaning  the inside of
the boiler  except  for  the  fire tube  itself.   Operator comments   indicated
that the gas  passes did  have  ash  deposits  in them.   With  the  exception of
PS-06,   no evidence  of  conversion   due  to  catalysis  by   Vz^s  was   found;
                                      155

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however, boiler  surfaces  were generally clean  at the start  of each of these
tests.


                   TABLE 1.   Test Results from Sulfate Runs
Test

PS04
PS05A
PS05B
PS06
PS07
PS08
            Fuel/?02
          0.3?S,No.6F.O./2.2?
          0. 35?S, No. 6F.O./2.0?
          0.35?S,No.6F.O./3.1?
          0.35$S,No.6F.O./3.3?
          1.4556S, No. 6F.O./2.0?
          1.1*3, No. 6F.O./3.0*
   Sulfate
% Total Sulfur

      1.4
      2.1
      2-1
      8.4
      1.2
      1.8
                                                       V/Ni (ppm)a     Boiler
                                                      1.4/0.1
                                                      6.4/8.6
                                                      6.4/8.6
                                                      6.4/8.6
                                                      94/22.8
                                                        64/12
a  Vanadium and Nickel content of  fuel oil  (ppm)
                                                                        20 hp
                                                                        20 hp
                                                                        20 hp
                                                                        20 hp
                                                                       700 hp
                                                                       700 hp
     A  field  test  program  was  initiated  after  reviewing  these  results.
Objectives of  the activity  were  to test typical units,  preferably units  that
had some degree of  deposit  buildup inside the  furnace that might  be  charac-
teristic of  the normal  condition of  residential and  commercial units.   In
addition,  it  was  planned  to  conduct  tests  at  one  site  that  had been  pre-
viously studied and to  compare  the total measured sulfate  from the CCS train
to that found by a  modified Method  8  train.   Table 2  presents  data regarding
the facilities and operating conditions.
Site
( — )
              TABLE 2.  Site Information  for Field  Sulfate  Runs

                   Type        Rating    Capacity Factor  Excess Air  % S  in
                   (---)     (MM Btu/hr)  (% of Full  load)     (*)    No. 6 Oil
Starrett City   Residential    145.0


                                98.0


                                63.0
Philadelphia    Commercial
State Hospital

Wyeth           Light
Laboratories    Industrial
          50
          21
          75
                                                         40
                                                        170
                                                         25
                                                                        0.3
                                                                        0.5
                                                                        1.0
     The field tests were  conducted  in the spring and  summer,  accounting  for
the low  load  factors at the  residential  and commercial  sites  and accounting
for the high  excess  air  at the commercial  site.   The  residential  boiler  had
been cleaned  immediately before  to  the start  of  testing;  the boiler  at  the
commercial  site  had  fired fuel  oil  for  72 hours  before  the testing;  the
industrial boiler had  not  been cleaned in the  recent  past.   Table 3 provides
a summary of the results.
                                      156

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                   TABLE 3.  Test Results from Field Tests

     Site          Method       V/Nia       % S from Fuel as Primary Sulfate
Starrett City       CCS^      1U.9/16.1     1.5? (37? as acid)

Philadelphia
State Hospital      CCS       15.5/30.8     0.95? (46? as acid)

Philadelphia
State Hospital      IPAC      15.5/30.8     1.5?

Wyeth
Laboratories        CCS       15.1/27.5     3.8? (82? as acid)
a    Vanadium and Nickel (ppm)
b    Controlled Condensation Sampling Train
G    Modified EPA Reference Method 8
These data  that the  conversion  to sulfate  was  2.0?  or  less for  the  lower
load tests  with boilers that had  been  cleaned recently.   Only  for the Wyeth
Laboratories  test  was  a  higher  sulfate  conversion  noted,  and  all of  this
increase  appeared   as  acid.   In  addition,  the  results  from   the  modified
Method  8  test  were  consistently higher  than  from the  tests using the  CCS
train.6
     Some results  from  the  vanadium data  base  are  shown in Figure 1.  Calcu-
lated emissions  are  shown by  state for the years  1950 and  1980.   Only Ohio,
Oregon, Pennsylvania,  and  Rhode  Island have shown a  decrease.   Otner  states
that now  have  reasonably large  emissions have shown  a  significant  increase
over the  1950  numbers.   Among these  are Alabama  (4-fold), Delaware (7-fold),
Florida  (6-fold),   Louisiana  (18-fold),   Mississippi   (88-fold),  and   North
Carolina  (9-fold).   Each  of these  six states emits over  100,000 kilograms of
vanadium  per  year   (1980) and each has  sho^n  more than  a  400?  increase  in
such emissions  since  1950.7
     Results  of the  chlorine and  fluorine tests have  been reduced  to  the
form of emission factors, and are  presented  in Table  4 as pounds per million
Btu per percent of the element  in the  fuel.   The  values calculated  from the
emission  tests  in   the  stack are in  reasonably good  agreement  with  the
quantities  of  each   element  that entered in  the  fuel.    Furthermore,  the
results indicate that essentially  all the  chlorine and  fluorine are present
as HC1 and HF.
     Equilibrium calculations were performed using a multiphase equilibrium
program available at  PETC.  These  calculations predict that HC1  would  be the
dominant gas  phase  species  (by over  two orders of magnitude) at the tempera-
tures of interest.   These calculations agree with earlier studies.8' >
                                      157

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                    TABLE 4.  Calculated Emission Factors

                                 Calculated Emission Factors
Element
(X) lb/(flBtu)a Ib/CflBtu x ?X)a


a
b
Cl 4.4 x 10-2 0.69
F 4.4 x 10-3 0.87
Calculated From Emission Tests
Calculated Fron Fuel Compositions and Feed Rate
lb/(flBtu x ?X)b
0.76
0.71

                                 CONCLUSIONS

     In general,  the  results  of all  the  sulfate tests  indicate low conver-
sions of sulfur to primary  sulfate.   However for two tests, where  the boiler
may  have  contained  significant  deposits,   higher   conversions  were  noted.
Data have  been developed  for  a rang?  of unit  sizes,  operating conditions,
and fuel properties.
     Chlorine  and  fluorine emissions   follow  the   concentration   of  these
elements in the fuel;  HC1 and  HF are the dominant gas-phase species.
                                     158

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                                 References

 1.   D.  Misenheimer,  R.  Sommer, H.R.  Glowers,  and A.S. Werner,  "Assessment
     of Ammonia, Hydrogen  Chloride,  Hydrogen Fluoride  Emission Factors  for
     the NAPAP Emission Inventory,"  CCA Corporation EPA Contract  No.  68-02-
     3168,  TASK No.  90,  Revised Draft Final  Report,  March  1985.

 2.   J.  Hornolya,  "Primary  Sulfate Emission  Factors  for the NAPAP  Emissions
     Inventory," Radian Corporation,  EPA  Contract  No.  68-02-399^,  Task  No.
     5,  Revised Draft Final Report,  July 1985.

 3-   Workshop  Proceedings   on  Primary Sulfate   Emissions   from   Combustion
     Source,   Volume  2,  U.S.  Environmental  Protection  Agency,  NTIS  PB-287
     1436,  August 1978.

 ^.   J.   Driscoll,   Flue   Gas  Monitoring  Techniques,   Ann  Arbor  Science
     Publishers, Inc., Ann  Arbor,  Mich.

 5.   D.A.  Stern, B.M. Myatt,  J.F. Lachowski, and K.T.  McGregor,  "Speciation
     of  Halogen  and  Hydrogen  Halide  Compounds  in  Gaseous   Emissions,"
     presented  at  the  Ninth  Annual   Research   Symposium,  Land   Disposal,
     Incineration,  and  Treatment  of  Hazardous  Waste,   Ft. Mitchell,  Ky. ,
     (May,  1983).

 6.   "Characterization of  Primary Sulfate Emission  from a Residential  and  a
     Commercial  Boiler  Firing  No.  6   Fuel  Oil,"  draft   final   report  by
     Ray F.  Weston  under  Subtask 7.9,  U.S.   DOE  Contract DE-AC-22-8^PC75571
     (August  1985).

 7.   S.  Kulkarni,  C.   Arnold, J. Homolya, and J. Dickermann,  "Vanadium  Nickel
     and Primary Sulfate  Emissions   From  the Combustion of  Fossil  Fuels  in
     the United States of  America,"  draft final report  by Radian  Corporation
     under  U.S.DOE  Contract No.  DE-AC-8HPC71505  (August  1985).

 °.   T.L.   Tapalucci, R.J. Demski,  and  D.  Bienstock,  "Chlorine  in Coal
     Combustion,"  U.S. Department  of  the Interior  RI7260 (May 1969).

 9.   M.J.  Hodges,  W.R. Ladner, and T.G. Martin, "Chlorine in Coal:   A  Review
     of Its  Origin   and Mode  of  Occurrence,"  Journal  of  the  Institute   of
     Energy,  pp. 158-169  (September  1983).

10.   W.D.  Halstead  and  E. Raask,   "The  Behavior  of   Sulphur  and  Chlorine
     Compounds in Pulverized-Coal-Fired  Boilers," Journal  of  the  Institute
     of  Fuel,  pp.  3^-3^9  (September  1969).
                                     159

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       Figure  1.  Computed Vanadium Distribution

                     For  1950 and  1980
            \ANADIfM EMIcsIGN DENSITi  LTi  .-TATt;
                                            V._-
  LEOENC
                       C!
                                   25'
           \ANADICM EMISSION DENSITY BY cflA
              •'—*£:-   --4  \  "r*" c
              ' '•-. J"1"     ^' I- <   . -*z^    i—
                ^^Lrf}   ^
LEGEND
                    o C;
                    10
0. I

25
                           160

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           VOC COMPOSITION OF AUTOMOTIVE EXHAUST
                 AND SOLVENT USE IN EUROPE
                         C. Veldt
                            TNO
           (Netherlands Organization for Applied
                   Scientific Research)
                       Presented at:


Second Annual Acid Deposition Emission Inventory Symposium
                Charleston, South Carolina
                   November 12-14, 1985
                             161

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                    VOC COMPOSITION OF AUTOMOTIVE EXHAUST
                          AND SOLVENT USE IN EUROPE
                              by:  C. Veldt
                                   TNO
                                   (Netherlands Organization for
                                   Applied Scientific Research)
                                  ABSTRACT

     Compositions of automotive exhaust hydrocarbons and aldehydes are
presented at a level of detail  relevant for input into photochemical air
pollution and acid deposition models.   Data were compiled from literature
for gasoline-, diesel- and LPG-powered vehicles without exhaust controls.
For gasoline-derived compositions, data were converted to separate profile?
for saturates, unsaturates and aromates.  Relations between gasoline
composition and exhaust composition were used to combine the average profile
compositions to one average overall composition.  A comparison with fuels
measurements was made.
     An attempt has also been made to estimate an average solvent
consumption resp. emission pattern for Western European countries.  Since
data appeared to be very scarce, all available material both inside Europe
and abroad was used for a first approximation.  An average mass rate per
capita and an average composition is proposed.  Spatial distribution
criteria are suggested.  The results should be used as default values
anticipating more reliable data.
                                       162

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                    VOC COMPOSITION OF AUTOMOTIVE EXHAUST
                          AND SOLVENT USE IN EUROPE

                                 INTRODUCTION

     The two largest contributors to total anthropogenic VOC emissions in
most European countries are non-catalyst automobiles and the evaporation of
solvents (ca. 50 percent and ca. 35 percent of total VOC emissions
respectively).  For the purpose  of modeling photochemical air pollution and
acid deposition, it is necessary to know the composition of these pollutants
as detailed as relevant.  Modeling large areas in Europe implies the
possibility that nationally different emission factors have to be used.
While differences in vehicle fleets as well  as driving habits can reasonably
be taken into account in estimating mass emissions,  their influences on
composition are not known.  When solvent emissions have to be assessed,
considerably larger problems must be faced as both mass emission rates and
compositions are sufficiently known for only a few countries.
     The need of widely applicable emission factors  being apparent, an
attempt has been made and is presented in this paper to quantify:
     a.   exhaust hydrocarbon composition from gasoline-powered vehicles
          with only fuel composition as a variable,
     b.   exhaust hydrocarbon compositions of diesel- and LPG-powered
          vehicles,
     c.   an average per capita mass emission factor fir solvent use,
     d.   an average composition of solvent emissions
and,  finally, to draw up spatial distribution criteria for solvent emissions.

                                 DISCUSSION

1.   Exhaust Emissions
     For gasoline-powered vehicles, the literature was searched for test
data satisfying the following demands:  a) test vehicle(s) without exhaust
control, b) VOC-analysis comprising at least main components, c) complete
                                      163

-------
(or nearly complete) mass balance.  Eleven investigations answered these
demands (Table 1).
     All data were converted to percent by weight to facilitate combination
with mass emission factors.  As could be expected, averaging absolute
fractions was not of much use.  Therefore, composition profiles were
calculated for saturates, unsaturates and aromates.  These resulted in
applicable averages (Tables 2a and 2b).
     Next the profiles had to be integrated to one average composition.
Only for aromates a useful correlation between fuel- and exhaust composition
appeared to exist (Figure 1).  It has been shown, however (12, 13), that
there is a relation between fuel aromates and exhaust olefines (Figure 2).
With this, exhaust composition can be estimated by the aromatic content of
the fuel (Figure 3).  Finally, a correction for oxygenates is needed.
Oxygenate content and composition, as well as diesel- and LPG-exhaust
composition were estimated from literature data satisfying the same
above-mentioned demands  (Tables 3-5).  In contrast with gasoline-exhaust
composition, useful material was scarce; for diesel fuel only six more or
less incomplete data sets were found, for LPG only two (20, 22).
     Since only one report about field measurements was found that could be
used as a comparison (21), an average road traffic exhaust composition was
calculated for that purpose (Netherlands, 1978; Table 6).  In this table, a
comparison based on a reactivity scheme has been added because this is what
ultimately is of interest.
2.   Solvent Emissions
     Assuming that a society's solvent consumption, with respect both to
quantity and substances used, depends on the level of industrialization and
material development, it can be expected that comparable emission patterns
exist in several European countries.  This was checked by collecting as much
data as possible about solvent emissions from different countries and taking
averages wherever it made sense (Tables 7 and 8).  Due to divergencies among
data and uncertainties about representativeness the results should be
characterized as default values only.  Another approach, in progress now, is
the assessment of mass balances to which solvent consumption factors are
applied.  It is not certain yet whether this will give more reliable
results.
                                     164

-------
     The geographic distribution of solvent emissions is complex because a
comprehensive source type-substance matrix is involved.   In view, however,
of the very large number of small sources and the relatively few large ones
it seems justifiable to distribute all emissions proportional  to population
density and make corrections for large area sources afterwards.   This
approach is valid only for meso- and macro-scale modeling.

                                 CONCLUSIONS

     An average composition of road traffic exhaust (dominated by gasoline
powered vehicles), based on a literature survey comprising old as well as
recent investigations, has a variation that is considered appropriate for
air pollution modeling.  Taking  into account the scarce data about the
influence of vehicle speed, vehicle age and ambient temperature on
composition, indicating that these influences cause no larger variations
than those presented in this study, it seems reasonable to assume that no
better input data can be expected to be available for modeling than these.
     The quality of emission factors for solvent use can not easily be
estimated since there is insufficient knowledge about the reliability of
individual national data.  Analysis of national mass balances may possibly
improve the factors.
                                     165

-------
                                 LITERATURE


 1.  J.D.  Caplan,  SAE Progr  Tech.  Ser.  12 (1967)  20-31.

 2.  M.W.  Jackson,  ibid,  241-67.

 3.  I.D.  Lytollis,  MIRA  Report Nr.  1971/1 (1970).

 4.  W.E.  Morris,  K.T.  Dishart, ASTM STP 487 (1971)  63-101.

 5.  K.  Schofield,  Env.  Sci.  and Tech.  8,  9 (1974)  826-3*.

 6.  L.J.  Papa,  'SAE  Progr.  Tech.  Ser.  H (1971)  43-65.

 7.  B.  Dimitriaderl  et  aJL, Bur.  of Mines  Rep.  of  Inv.  7700  (1972).

 8.  S.  Yanagihara,  Proc.  16th FISITA-Congress,  Tokyo 1976,  2-149-56.

 9.  P.M.  Black, I.E. High, EPA-600/2-80-085 (PB 203136),  JAPCA 30, 11
     (1980) 1216-21.

10.  P.P.  Nelson,  S.M.  Quigly, Atm.  Env. 18, 1  (1984) 79-87.

11.  R.  Steenlage,  R.C.  Rijkeboer,  MT-TNO Rep.  Nr.  G 1115 (1985).

12.  E.E.  Wigg,  et al..  SAE-Paper 720251 (1972).

1J.  K.  Hosaka,  et al..  SAE Tech. Paper Ser. 780625 (1?78).

14.  P.M.  Carey, EPA-AA-CTAB-PA-81-11  (PB 82-118159) (1981).  (a) 4 LDV's
     (1970); FTP;  DNPH.   (b)  10 LDV's  (1970-1973);  FTP; DNPH.  (c) AMC Pacer
     (1977); FTP;  DNPH (average value  of five types of malfunction).

15.  See 12.  1970 repr.  test vehicle;  FTP; MBTH (total), DNPH (ind.)

16.  P.E.  Oberdorfer, SAE Progr. Tech.  Ser. 14,  32-40 (1971).

17.  C.S.  Wodkowski,  et al..  West Coast APCA Mtg.,  San Francisco  1970 (cit.
     from Vapor-Phase Organic Pollutants,  EPA 600/1-75-005,  PB 249357);
     a = 30 mph, b = FTP).

18.  M.F.  Fracchia,  et iL, Env. Sci.  and Tech.  I,  11 (1967) 915-22.

19.  Nat'l Res.  Council,  EPA 600/6-82-002  (PB 82-180498); a = idle,  b =  FTP.

20.  R.  Steenlage,  R.C.  Rijkeboer,  MT-TNO Rep.  Nr.  G 1115 (1985)  (Dutch.
     Org.  for Appl.  Sci.  Res.); Opel Ascona 1.6 S (1983), EEC-cycle, MBTH;
     a = optimal,  b = rich.
                                     166

-------
21.  R. Guicherit, Th.R. Thijsse, IMG-TNO Rep. Nr. G 1198 (1982).

22.  K.E. Egeback, et al..  Nat'l Swedish Environ. Protect Board Rep.
     Nr. 1635 (1983).

23.  Umweltbundesamt Berlin.

24.  CITEPA, Paris.

25.  K.A. Brice, R.G. Derwent, Atm. Env. 12 (1978) 2045-54.

26.  Project Emission Registration, Min. of Housing, Physical Planning and
     Environment (Netherlands).

27.  Swedish Environ. Res.  Inst., Stockholm.

28.  EPA, Office of Air Quality Planning and Standards.

29.  Environ. Protect. Progr. Dir., Report EPA 3-EP-83-10 (1983).

30.  Photochemical Smog, OECD, Paris 1982.

31.  R. Schaaf, Wasser, Luft and Betrieb, 1984-3, 36-8.

32.  C. Morley, Shell Res.  Ltd., Thornton Res. Centre,  England; paper for
     submission to Atmospheric Environment (1981).

33.  P.F- Nelson, et al_,  Atm. Env. 17, 3 (1983) 439-49.
                                     167

-------
   60
                                               40 r
.c
X
HI
c  40
   20
               20        40        -60
           Wt.Z aromates in fuel
                   Fig. 1
.c
x
                                   r=0.53
                                 • (this work)
                                 v r=0.94
                                  (Wigg et al)
               20        40        60
           Wf.Z aromates in fuel
                   Fig.2
                        100
                        80
                        60
                      u 40
                        20
                                      saturates
                                     aromates
                                    20        40         60
                                  Wt.% aromates in fuel
                                         Fig.3
                                   168

-------
Table 1
Investigations of automotive exhaust;  gasoline powered vehicles; experi-
mental data.
Lit.
nr .
1
2


3


4

5

6



7






8






9
10




11




Test vehicle(s)
no data
0.63 1 single cyl .
motor; compression
ratio = 8.9/1
1 of A cyl . of 1 .3 1
motor; compression
ratio = 8.5/1
Automobile without
control system
No data; "represen-
tative composition"
"62 privately owned
and operated automo-
biles" Composition of
one of these is given.
1969 Valiant; 3.8 1






"pre-emission control-
led car with retrofit
device of retarding
ignition timing"



1963 Chevrolet 283 V8
67 automobiles repre-
sentative for Sydney
fleet. Ages: < ' 72 -
> '78. Weighed average
composition given.
Test
procedure











Calif, cycle



7-mode Calif.
cycle. Each
fuel : rich,
resp. lean;
with, resp.
without vacuum
spark advance
Hot 10-mode,
6 cycles





FTP
1975 FTP




Opel Ascona 1.6 S (1983) EEC-cycle,




rich and opti-
mal ;
90 km/h opt.
120 km/h opt.
Gasoline
composition (wt.%)
sat. unsat. arom.

55 10 35


46 16 38


59 10 31







a) t i.5 H.5 22
b) 5? 10 33
c) 48 2 50




a) 51 b 4j
b) 71 i: 17
0 C2 12 26
d) 59.5 0.6- 40
e) 41 19 40
f) 40 12 48
g) 33 11 5t>
69 5 Jb
63.5 6 30.5









Approx. ye
of invest!
1967
1967


1970


1968

1971

1970



1971






1975






197?
198(




198




                              169

-------
Table 2.
                          Investigations  of  automotive  exhaust;  gasoline  powered  vehitles.  Hydrocarbon  aualyses
Hydroca rbon


methane
propane
butanes
pentanes
hexanes
heptanes
octanes
C > 9 saturates
wt . X aba .
et Ly lene
acetylene
propy !ene
propad i cne
methyl acetylene
1 -butenes
I ,3-butadiene
\ -pentenes
2-pentenes
1 -hexenes
C > 7 unsaturates
wt. X abs
a roma 1 1 c
benzene
toluene
xy I enes
ethylbenzene
st y**ne
1 ,2,4-1 rime thy) benzene
1,3,'i-triinrthyl benzene
} , 2, 3-tri me thy! benzene
other Cg-« mmates
C > 10 aromales

wt. X abs

3 naphLa 1 cne
1 2 3


22.0 16 0 20. 1 1

4.7 5.1 12.0 1
13.3 14.9 19.8 1
94 12.4 17.4 1
7.5 9.4 13.5 1
40 3 35.9 10.5 .
2.2 2.0 ''
30.8 27.8 21.2 4
21.5 18.3 33.6 2
15 9 13.1 24.5 1
12.6 15.8 13.1 1
2-6 b &
1.8 1
Il2 5 )l6 0 >8 5 '
1 ' 1 I ' )
3.1 3.5 3.7
7.0 6.9 4.6 2
4.7 4.2 1.4
14.6 12.2 1.5
32.0 33.7 40 6 3

8.2 7.2 11.3 1
47.2 46.7 20.1 3
11.2 11.0 23.2 2;
3.0 3.5 5.4

	 7.8V 9.8 f
1.2 1.5 2.9 I
29.2J 8.6 12.0 I18
13.7 14.0 '

37.2 38.5 36.2 2(


456


2 8 23.7 19 1

D.3 11.0
f>.0 14.0
). 1 16.3
1.4 12 3
20 8
3 4.8
2.8 34 5 44.4
9." 22.4 25.5
96 25.8 35. 7
S. 5 175 11.8
2.3 0.5
1 0
3.6 12 g 5.7

3.6
.4 7 9
1 2
1 .5
).3 37.1 24.9

.0 12.5 8 1
.5 40 8 20.8
.5 14.0 21 4
.5 ' 4.0 4.3

.5 8.1
2 5
H5
22.2

.9 28 4 30 7


7
a b c

14 8 12 9 15.7

5.7 6.0 11.6
12.7 16.9 13.7
24.8 19.5 11.9
14.7 10.4 11 .6
10.7 9.3 21 .4
15 0 23.6 12.6
40 3 15.0 28.0
29.1 24 6 22.8
22.4 214 27.8
113 10 4 15.4
0.7 0.5 1.0
1.2 1.3 2.1
4.2 3.5 6.4
28 2.5 16
2.8 4.2 2.5
4.2 5.9 5 '1
3.6 2.9 4 2
12.2 15.7 6. 1
30.2 25.3 IB.O

5 7 2.6 2.9
14 5 10.0 14. 7
18 5 19 6 25 7
1.6 35 5.8
1.3 0.9 0.9
98 96 75
23 1.9 1.5
}ll 4 }|1.9 JI0.6
12.9 40.0 10.4

21 5 19 7 54 0


8
a h c d p f g

14.6 22.9 22 4 28.0 40.3 28.6 31 . 1
0.2 0.3 0.4 0.5 03 0.4 05
3.7 4.6 3.9 2.6 4.7 4.1 2.7
22 7 10.7 116 151 18.2 18.4 19.6
35.4 15.0 18.5 22 8 19.8 27.6 26.2
8.7103 62 74 68 9.5 10.0
10.2 34.1 10.3 20.8 51 6.4 6.3
4.5 2.1 4.7 2.8 48 5.0 36
41.7 58.8 56 8 53.4 50 6 42.1 17 4
33.2 30.7 32.9 39.1 31 9 36.2 J9.0
24 9 25.4 28.1 24,1 23 8 39.7 29 4
13.1 23 5 158 13.8 16.7 8.9 11.6


3.7 4.0 3.7 3.7 41 3.1 2.6

5.1 3.4 3.7 1.6 3.3 1.4 2.3
10.3 4.0 4.4 3.8 7.6 2.1 3.0
3.5 1.3 2.0 40 1.6 2.1 2.6
3.6 4.1 6.5 2.3 3.6 5.0
15.5 24.6 20.4 14.1 22.6 19.9 13.9

14.9 14.7 15.0 12.3 162 14.8 46.2
32.0 2C.3 27.3 32 3 31.1 16 2 21.5
23.7 23.5 24.0 22.2 24 4 24.3 15.8
5.4 6.3 5.8 6.1 65 71 4.1

5.4 5.6 4.5 4.4 24 3.6 2.7
2.2 2.5 1.3 18 10 0.7
3.9 15 2.0 10 1.1 1.5
6.4 86 6.8 7.0 51 6.7 1.8
6.1 11.0 146 144 111 5.2 1.7

42 >• 16 6 22 fl 32.5 26.6 38 0 48 ?


93) 10" 11


28. S U 8 217
0.2 0.3
10.7 7.7 6.1
9.0 211 25 2
14.8 22.0 2 0
9.7 117 97
16.7 10 1 272
5.2 9.6 3.5
37.3 38 8 270
34.4 31.2 28 2
24.6 27.5 42 4
14.8 13.6 11 9
0.8 1 3
1.9 1.2
6.4 6.2 12.2
4.3 1 1
6.0 1.5
2.0 3.4
1.4 ,
0.2 1
40.3 29.5 25. ,

17.6 14 0 10 1
22.7 29.2 23 
-------
Table 2b
          Investigations of automotive exhaust;  gasoline  powered  vehicles
                              Average values  (wt.  %)
Hydrocarbon
saturated
methane
ethane
propane
butanes
pentanes
hexanes
heptanes
octanes
C9 + saturates

C. + saturates
4

unsaturated
ethylene
acetylene
propylene
propadiene
methyl acetylene
1-butenes
1 ,3-butadiene
1-pentenes
2-pentenes
1-hexenes
2- and 3-b.exenes
C unsaturates

aromatic
benzene
toluene
xylenes
ethylbenzene
styrene
1 , 2, 4- 1 rime. -benzene
1 ,3,5-trime .-benzene
1 ,2 ,3-trime . -benzene
other C9 aroraates
C . aromates

average

21
3
0
6
16
18
10
18
6
101
76


29
26
14
1
1
5
2
3
5
2
2
6

100

12
28
23
5

6
2
1
7
14

102

6 ±
1 ±
3 ±
5 ±
4 ±
6 ±
2 ±
6 t
2 ±
5
7 ±


7 ±
1 ±
3 ±
2 ±
6 ±
3 ±
5 ±
2 ±
1 ±
7 ±
6 ±
4 ±

9

9 ±
9 ±
1 ±
8 ±

6 ±
0 ±
6 ±
6 ±
0 ±

6

7.3
1.3
0.1
3.2
4.2
7.5
2.4
11.4
5.9

7.3


5.9
7.2
3.3
0.8
0.5
2.8
1.2
1.2
2.3
1 .2
1.0
5.2


9.1
9.9
6.8
2.1

2.8
0.9
1.0
2.3
10.5


34
44
33
49
26
41
23
6!
95

9


20
28
23
67
31
52
47
39
45
46
41
81


71
34
29
37

42
44
61
30
75

average
(excl. 2o)
%o

20
3
0
6
15
18
10
18
5
99
77


29
25
13
1
1
4
2
3
4
2
2
6

100

11
28
22
5
1
6
1
1
7
12

98

5
1
3
5
9
6
2
6
5
2
6


7
2
S
2
6
9
5
0
8
7
6
4

9

1
9
5
3

6
8
3
6
1

3

+
+
+
+
+
+
+
+
+

+


+
+
+
+
+
+
+
+
+
+
+
+


+
+
+
±

+
+
+
+
+


5.9
1.3
0. 1
3.2
3.7
5.2
2.4
11.4
3.9

6.1


5.9
6.2
2.5
0.8
0.5
2. 1
1.2
1.0
1.9
1.2
1.0
5.2


4.5
9.9
6.1
1.6

2.8
0.7
0.4
2.3
7.9


29
44
33
49
23
28
23
61
70

8


20
25
18
67
31
43
47
34
40
46
41
81


40
34
27
30

42
36
32
30
65

a

18
12
9
18
17
16
18
18
15

17


19
18
18
8
7
14
5
15
15
15
15
14


18
19
19
19
4
15
14
7
11
15

adoptf
averaj

19
3
0.







77
100

29
25
14


6
2
j
I
\
\
I
10i


2
2






1

1
                               171

-------
Table 3
                     Oxygenates in automotive exhaust; gasoline-po;vered vehicles (wt. X)
Component
i
forma 1 defiyde
aceta 1 dehyde
acetone
propiona Idehyde
aero 1 e'l n
buty la] dehydea
hexana 1 dehyde
benzi Idehyde
tolualdehyde
other aldehydea
total oxygenates
14 IS 16 17 18 19 20
abc at atab
86 74.2 48.7 48 5 .16 9 42 0 53 0 53.9 49.3 50.0 46.0
13.5 19.6 9.3 7 3 12 9 67 91 92 13.4
5.2 ... , 0.5 8.2 0.8 3 0 9.0 23.0
|22 . 2
1 12.7 3.0 8 7
1 0.7 4.4 1.5 30 3.0 2.0
1.2
12.4 20.8 7.2 11.6 H.I 11.2 10.2
12.3 14.5 7.5
0.9 9.5 15.9 26.9 12.1 13.7 2.1
2.0 5.8 1.9 2.31.6
average
(exc 1 . 2o) %o
50.3 t ').fl 20
11.2*40 36
4.5(0.5-9)

8. 1(3-12.7)
2.4*1.3 54

12 1 » 4 2 35
11 .4(7.5-14.51

2.7*1.7 64
adopted
average
50
10
5




10
10
15
2
Se>  1 ist of  references  tor  experimental  data
                    Table  4



         Compos i t ion of  dlese 1  exhaust
                                                                               Compos iti on of I.PG-exhaus I
Component
methane
ethane
sat tirates C— -
'•I hy I rut-
ac ety 1 ene
propy lene
1 -butenea
penteneg
benzene
aronales Cr-r
formaldehyde
aliph. aldehydes C-
unsat. aldehydes C-
acetone
organic acids C =
a
3
0
SO
1 1
3
3
1
0
2
2
8
5
4
0
2
1
vera
.7 1
.5

.0 !
.2 i
.4 »
5 *
.7
6 1

.9 i

.5
(0.

"
1 .5


1.4
1.6
i .n
0 5

i i

2 5


6-3.6)

adopted
average
4
0.5
50
11
3 !
3.5
1 5
0.5
2
2.5
8
'6
4
0.5
2
1
Component
met hane
ethane
p ropane
ethyl em-
acet y 1 ene
propy lene
benzene
to 1 urne
aylenes
forma 1 dehyde
ac^Laldehyde
organic acids
average
8
2
34
15
21
7
0
0
1
3
0
1
.9
.7
.5
.6
,8
.6
(1.
• 0
* 6
* 4
* 5
1 2
. 15(0
.3
.5
.4
.6
.7
(0
(0.
* 1

1 1
3-16.4)
8
0
9
.7
. 1
03-0.4)
06-0.5)
OI.-3.5)
.5

.0
adopted
average
9
3
35
15
22
8


1
4
1
1








5


5

-------
Table 6
Road traffic exhaust composition (ut.  % and mole/kg   )


methane
ethane
propane
€,-€,„ saturates
ti 10
C saturates
etnylene
acetylene
propylene
propadiene
methyl acetylene
1 -butenes
1 ,3-butadiene
2-butenes
1-pentenes
2-pentenes
1-hexenes
2- and 3-hexenes
C.+ unsaturates
benzene
toluene
xylenes
ethylbenzene
styrene
1 , 2, 4- 1 rime . -benzene
1 ,2,5-trime . -benzene
1 , 2, 3- 1 rime . -benzene
other Cg-aromates
C,. aromates
10+
formaldehyde
other oxygenates
OLE
PAR
TOL
m
FORM
ALD
ETH
UHR
calculated

8.0
1.3
1.2
29.8
5.5
7.9
6.3
3.6
0.2
0.3
1.4
0.5
0.5
0.7
0.9
0.5
0.5
1.5
3.:
7.2
5.7
1.2
0.3
1.6
0.5
0.4
2.0
3.9

1.6
1.8
1.4
32.7
0.9
1.2
1.5
0.6
2.8
11.1
measured
(21)
7.2
0.6
0.6
32.3
2.2
6.6
4.8
2.6


1 .0

0.4
1.2
1.3
2. 4

0.7
3.9
9.9
6.4
2.3
0.8
2.3
1.3
0.6
2.8
3.7

1. 1
1.0
1.1
31.1
1.3
1.4
0.7
1.0
2.4
10.0
!7
2)
30% aromates in gasoline,  gasoline exhaust:  86%,  diesel  exhaust:
LPC exhaust 3% (Dutch 1978 average).

Chemical bond species (CBM-X,  SAI)
                                                                      11%,
                            173

-------
Table 7
                      VOC-emissions from solvent use
                              (kg/cap. year)




INDUSTRIAL
paiut application
degreasing
printing
chemical industry
storage & handling
metal products manuf.
glues, adhesives
other
total from industry
NON- INDUSTRIAL
paint application
chemical cleaning
consumer products
- a.w. aerosol cans
total non-industrial
total emissions
total paint appli-
cation
OECD-estimation 1975
1985
23 24
FRG France

1978-'80 1979

3.25
2.31} 1.65
1.15 0.65



0.8
0.3
7.8

2.6
0.25 0.55



13.7 13

5.85 3.7
13.2 12.2
18.8 17.5
25 26
27 28 29
UK Nether- Sweden USA Canada
lands
1975 1981

(2)2)
0.45
0.55
1.3
0. 15
0.7

2.4
5.1

2.6 2.7
0.66 0.25
3.5
1.25
6.45


1984 1982 1978

2.4
1.2
0.85
^

'0.35

'

6.8
1.6 2.25
1.3


•4.1


4.8 13.8

1.2
0.18
3.83)
•
5.2

2.85
0.95 0.7
3.5 0.9

7.3
5.5 11.6 10 21.1 5.6

4.7

3.6

9.65
5.55) 11.4 12.1 29.5 10.0
7.4 15.3
16.1 40.4 13.5

defa
valo


2
1,
1.







2
0
3

6
12

4


 'or 1.9
2);
3)
5)
included in industrial emissions
OECD-figure
Ref. 30
from ref. 25
                               174

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Table 8
              Compositions of VOC-eroissions from solvent use

                                   (wt. %)




sat. hydrocarbons C,
4+
toluene
xylenes
other aromates
total aromates
methylalcohol
ethylalcohol
isopropylalcohol
butanoles
cellosolves

other alcohols
total alcohols
acetone
me thy le thy Ike tone
methy lisobuty Ike tone
other ketones
total ketones
acetates
other esteres
total esteis
ethers
methylene chloride
trichloroethylene
perchloroethylene
other Cl-hydrocarbons
total Cl-hydrocarbons
Cl-F- hydrocarbons
other solvents
31 24 32 26 28 33
FRC France OECD Nether- USA Sydney
Eur°Pe2) lands
1982 1978 1981 1982
19.2 27 36.3 42.5 5.9.3 25.7
5.4 5.1 >6.6 18.4
3.9 4.0 >3.1 10.6
1.6 9.8 1.6 16.6
10.9 24 19.5 45.6
3.8 1 .. .i 5.0 — |
3.3 6.1 .0 5.3 13.7
1.4 (6) 6.7 2.6 ^
6.7 ) „ 1.5 , ,
r'-8 r-3
5.3 , xj.6.4 4. r
241)| J C.2 J
20.5 20.4 13.7 19.3 15.0
(6) 6.. ...3 3.2 1.6
3.2 4.1 2.9
2.1 ^.0 1.0 1.0
0.3
5.4 J 11.4 4.3 8.6 5.5
7.1 95.1 2.8 2.6
0.5
7.6 5.1 3.9 2.8 2.6
11.9 1.9
6.0 5.5 4.6 1.8
2.2 4.4 1.3 1.3 1.9
4.4 4.8 3.5 4.0 0.4
4.9 3.0 1.0 1.6 1.5

def ai
.•alue

32
6
4
5

2
6
5



5

i

2


6


2

2
4
2
1.75 16 17.7 10.4 6.9 5,6
3.8 3.6
3.2 0.2 1.5
3

1),
2)
incl. ethers

Non-reactive compounds not included.  Added for this study:  300 kt acetone,
60 kt methylalcohol, 270 kt methylene chloride, 150 kt trichloroethane.
                           175

-------
     SESSION 4:   DEVELOPMENT OF EMISSION  INVENTORIES  FOR  NATURAL SOURCES

Chairman:   Fred  Fehsenfeld
           National  Oceanic  and Atmospheric  Administration
           Aeronomy  Laboratory
           R/E/AL6 325 Broadway
           Boulder,  CO  80303
                                    176

-------
         MEASUREMENT OF BIOGENIC SULFUR FLUXES AT
         THREE SITES IN THE EASTERN UNITED STATES
                       P. D. Goldan
                       W. C. Kuster
                     F. C. Fehsenfeld
                      D. L. Albritton
                    Aeronomy Laboratory
      National Oceanic and Atmospheric Administration
                 Boulder, Colorado  80303
                       Presented at:


Second Annual Acid Deposition Emission Inventory Symposium
                Charleston, South Carolina
                   November 12-14, 1985
                            177

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                  MEASUREMENT OF BIOGENIC SULFUR FLUXES AT
                  THREE SITES IN THE EASTERN UNITED STATES

                                INTRODUCTION

     An assessment of the significance of natural  biogenic sulfur sources
compared to anthropogenic sources as potential  contributors to the
acidification of rainfall requires measurement  of fluxes at or below 10 ng
   ^
S/m  min over large geographic areas.  To date,  such an assessment has
rested almost entirely on one study completed in 1979,  by Adams, et al. (1).
In view of the importance attached to these measurements, the analytical
difficulties recognized by previous workers, and recent improvements and
advances in measurement technology for trace sulfur species, a reassessment
of the strengths of natural sulfur fluxes was deemed desirable.
Consequently, simultaneous measurements at three previously-measured sites
were undertaken jointly by NOAA, Washington State University Air Resources
Laboratory and University of Idaho Department of Chemistry in July and
August 1985.
     Measurements were based on the use of enclosures that were placed over
bare soil, various types of agricultural crops,  and naturally occurring
vegetative cover, and were flushed with controlled flows of synthetic air or
scrubbed ambient air.  Concentrations of H-S, OCS, S0?, CH,SH, DMS
(CH3-S-CH3), CS2, DES (C^-S-C^), MES (CH3-S-C2H5) and DMDS (CH3-S-S-CH3)
in the enclosures were measured gas chromatographically by the NOAA group
using a one-step cryogenic sample enrichment technique in a microbore Teflon
capillary sample loop.  Concentrations of OCS,  DMS, CS? and DMDS were
measured gas chromatographically by the Washington State group using a
two-step cryogenic sample enrichment technique  similar to that used by
Adams et al. (1).  In addition, H2$ was measured by the Washington State
group using an impregnated filter   fluorometric quenching technique (2),
and total  sulfur was measured by the University of Idaho group using a Metal
Foil  Collection - Flash Vaporization technique  (3).  Surface and biomass
fluxes were related to the concentration measurements by means of the known
                                     178

-------
flush gas flow rate (typically 1.5 Std L/Min), the biomass enclosed
(measured by weighing at the end of a suitable measurement period) and the
surface area covered.
     Although an intercomparison of the results of the various data sets is
an important goal of the measurement program, we will discuss here only the
details of the NOAA measurements.  Preliminary intercomparison has, however,
shown that no gross discrepancies exist in the sulfur fluxes measured using
the various techniques.

                                   RESULTS

     Measurements in the vicinity of Ames, Iowa and Celeryville,  Ohio, over
bare soil demonstrated a high degree of correlation between the observed
fluxes and the enclosure air temperatures.  Plots of log (flux) versus
temperature showed a linear relationship with correlation coefficients
ranging from 0.89 to 0.98.  Although in agreement with the results of
Adams et al. (1), the observed correlation coefficients were significantly
higher than those obtained in the earlier study.  The inclusion of various
types of actively growing vegetative cover dramatically altered the fluxes
of DMS and DCS, the former being significantly increased and the latter
decreased.  The other significant sulfur flux contributors, H~S and CS-,
were affected to a much lesser degree by the presence of vegetation.
Table 1 summarizes our findings of hLS, DCS, DMS and CS^ fluxes from bare
soils and soils with different vegetative cover for Ames, Iowa.  Similar
results were obtained in Celeryville, Ohio, over bare histosol soils and
several native "grassy" ground covers.  The fluxes measured in this study of
                       o
approximately 10 ng/S/m  min at both Ames, Iowa and Celeryville, Ohio are
                                          2                   2
much smaller than the values of 350 ng S/m  min and 130 ng S/m  min reported
by Adams et al. (1) for the same two sites, respectively.
     The results obtained over salt water marshes at Cedar Island, North
Carolina were much more temporally and spatially variable and, therefore
difficult to summarize.  Measurements taken over Spartina Alterniflora  in
the same location, as were many of the measurements of Adams et al.  (1),
show obvious tidal effects; a radical diminution of the H?S flux and  a
                                     179

-------
temporary diminution of the DMS flux when the enclosed surface was covered
by water.  Measurements made over tidal  mud flats covered by the species
Juncus Romerianus, which appears to comprise more than 95 percent of the
tidal marshes in the Cedar Island-Beaufort area, again showed the I^S flux
to have high temporal variability, sometimes changing by more than a factor
of 100 in a half-hour period, and frequently surpassing the DMS flux as the
dominant species.  Although it is difficult to generalize from a few
measurements in such a highly variable environment, it appears certain that
FLS and DMS are the dominant species, with DCS, CS,, and CHjSH playing a
lesser role and DMDS hardly even appearing in quantifiable amounts.  The
results of our measurements in saline marsh environments are summarized in
Table 2.  Extreme ranges observed and estimated mean fluxes are listed for
H2S, COS, CH3SH, DMS and C$2.  No other significant contributors to the
natural sulfur flux were observed chromatographically.  For comparison, the
fluxes measured by Adams et al. (1) and Aneja et al.  (4, 5) are also shown.

                                 CONCLUSIONS

     The strong correlation of sulfur gas flux with ambient air temperature
noted in earlier studies has been corroborated by the present GC
measurements at Ames, Iowa and Celeryville, Ohio.  Absolute flux values at
weighted mean daily temperatures are found, however,  to be about a factor of
10, lower than previoMsly reported.  Similar measurements carried out over
saline marshes at Cedar Island, North Carolina also show a mean flux
averaged over tidal cycles, about a factor of 10 lower than previously
reported measurements.  Concurrent measurements of H?S and total sulfur
fluxes by entirely independent techniques substantiate the lower fluxes
reported here.
                                    180

-------
                                 REFERENCES
1.   Adams, D.F., Farwell, S.O., Robinson, E., Pack, M.R., and
     Bamesberger, W.L., tJiogenic sulfur source strengths, Environ. Sci.
     Tech.. 15, 1493-1498, 1981.

2.   Natusch, D.F.S., Klonis, H.B., Axelrod, H.D., Teck, R.J., and
     Lodge, J.P., Sensitive method for measurement of atmospheric hydrogen
     sulfide, Anal. Chem.. 44, 2067-2070, 1972.

3.   Kagel, R.A., and Farwell, S.O., Evaluation of different metallic foils
     for the preconcentration of sulfur-containing gases witli subsequent
     flash desorption/flame photometric detection, Anal. Chem.. (submitted,
     1985).

4.   Aneja, V.P., Overton, J.H., Jr., Cupitt, L.T., Durham, J.L., and
     Wilson, W.E., Direct measurements of emission rates of some atmospheric
     biogenic compounds, Tell us. 3_1, 174-178, 1979.

5.   Aneja, V.P., Overton, J.H., Jr., Cupitt, L.T., Durham, J.L., and
     Wilson, W.E., Carbon disulphide and carbonyl sulphide from biogenic
     sources and their contributions to the global sulphur cycle, Nature,
     282.  493-496, 1979.
                                     181

-------
                       TABLE 1.  AMES, IOWA, JULY 1985
            Bare Soil Flux
      F(T) = AEBT (ng S/m2 min)
           A          B       F(25.5)
                          Vegetative Cover Flux at  ?5.5
                          Oat         Gramma        Soy
                         Grass        Grass       Plants
        0.124
0.0643
0.6
3.0+1.0
2.3+0.8     1.0+0.4
COS     0.301
0.0870
2.8
2.0+0.8
1.7+C.6     0.7+0.3
DMS     0.0461     0.115
             0.9
           6.2+3.4
              3.5+1.0     5 3+2.9
CS2     0.0711     0.0831

TOTALS
             0.6
           0.6+C 2
           5.0+1.3     11.8+4.4
              0.4+0.2     C.5+0.2
                         7.9+2.6     7.5+3.8
                                     182

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TABLF 2.  PREDOMINANT NATURAL SOURCES (ng S/m2 min)
          CEDAR ISLAND, NORTH CAROLINA   SALINE MARSHES





H2S
COS
CH3SH
DMS
cs2
TOTALS


Adams et al
10-77 5-78
33 38
4 19

13 76
17
55 150



7-78
300
38
0.6
3000
114
3450


Ane.ia et al
7-78
100
80

1500
400
2080
NOAA,
Juncus
Tidallv
Observed
Auqust
1985
and Spartina
Flooded
Range
3 ---> >10,000
4 ---
1 ---
60 ---
2 ---

> 15
> 80
> 9''0
> 12

Me, "Si es
Mec n
100
8
7
200
6
220
                       183

-------
 DETERMINATION OF NITROGEN EMISSIONS FROM NATURAL SOURCES
                     F. C. Fehsenfeld
                      E. J. Williams
                       D. D. Parrish
                    Aeronomy Laboratory
      National Oceanic and Atmospheric Administration
                 Boulder, Colorado  80303
                       Presented at:


Second Annual Acid Deposition Emission Inventory Symposium

                Charleston, South Carolina

                   November 12-14, 1985
                            184

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          DETERMINATION OF NITROGEN EMISSIONS FROM NATURAL SOURCES
                            by:  F. C. Fehsenfeld
                                 E. J. Williams
                                 D. D. Parrish
                                 Aeronomy Laboratory
                                 National Oceanic and
                                 Atmospheric Administration
                                 Boulder, Colorado
                                  ABSTRACT

     The estimated fluxes of NO   (NO + NO-) from the principal natural
                               A         L~
sources a^e presented.  According to our present understanding, the largest
natural sources of NO  on the North American continent are lightning and
biogenic activity in the soils.  However, because of the large uncertainties
associated with the estimation of soil emission, improvements  in these
estimates have been given a high priority.  Accordingly, two of the
techniques used to measure biogenic NO emissions from the soil have been
'ntercompared.  The agreement between the techniques was good.  One of tnese
techniques,  an enclosure method, has beer, subsequently used to measure the
NO fluxes from the soils at a grassland site in Colorado.  The measured NO
fluxes compare favorably with NO fluxes measured at a similar  site in
Australia.
                                     185

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          DETERMINATION OF NITROGEN EMISSIONS FROM NATURAL SOURCES

                                INTRODUCTION

     Natural sources of NOX (NO + N02) are important,  not only because they
represent the irreducible minimum for the precursors of the nitrate
component of acid precipitation,  but also because they dominate the NOX
budget in the upper troposphere,  as well  as remote regions of the lower
troposphere.  This budget is important because NO  controls the
                                                 A
photochemical production of ozone and influences the concentration of
tropospheric hydroxyl radicals (OH).
     Five natural sources of NO  have been identified:  lightning, biogenic
                               A
processes ir soil, oxidation of ammonia,  stratospheric injection, and
photolytic processes in the oceans.  Table 1 lirts the emission inventories
for the identified sources for global and North American continental
averages.  The NO  fluxes contained in Table 1 are based on the estimates of
Logan (1983), updated to account for recent developments in this field that
have been reported in the current literature.  With regards to North
America,  the emission estimates presented in Table 1 can be summarized as
follows:   natural NO  production is dominated by two sources, lightning and
soil emissions.  Presently, the greatest  uncertainty lies in the estimation
of soil  emissions by NO    An improved quantification  of NO  soil fluxes
                       A                                   A
demands the development of improved field methods, intercomparison of new
and existing field methods, and extensive field studies.  This is the
objactive of the present study.

       INTERCOMPARISON OF METHODS USED TO MEASURE NO FLUXES FROM SOILS

     Several techniques have been utilized to measure NO fluxes from the
soil, including principally enclosure, gradient, and eddy correlation
methods.   The enclosure technique measures the NO  flux from a small,
                                             o   X
enclosed area of soil surface (typically -1 m ), while the gradient and eddy
                                     186

-------
correlation techniques determine the average NO  fluxes from larger areas
              32                             x
(typically -10  m ).  The enclosure method is genially simpler a^ n^re
convenient than the other two techniques, but it is possible that the fluxes
that it  is intended to measure are modified due to the disturbance of the
soil environment by the presence of the enclosure.  Thus far, all the
published measurements of NO  soil (Galbally and Roy, 1978; Johansson and
Granat,  1984; Johansson, 1984; Slemr and Seiler, 1984) fluxes have relied on
the enclosure technique.
     In  the present study,  a gradient technique for measuring NO fluxes from
the soil during nighttime hours has been developed.  This technique relies
on the measured (NO) gradient with height above the ground to define the
vertical mixing and, thus,  does not require the simultaneous measurement of
micrometeorological parameters.  Intercomparison of results from the
gradient technique with those from enclosure measurements were made at a
site located  in Colorado during August and September 1985.  The NO fluxes
during this period of intercomparison ranged from 0.3 ng N m   s   to
         -2   -1
25 ng N  m   s   .  Results obtained during this intercomparison are shown in
Table 2.  The agreement appears to be good over a wide range of NO fluxes.

                  MEASUREMENTS OF N0x FLU/ES FROM THE SOIL

     Following the intercompar'son studies, a larger set of flux
measurements has been obtained using the enclosure technique.  These fluxes
were measured from unfertilized, ungrazed, grass-covered soils in a period
between  1 August 1985 and 28 October 1985.  NO  fluxes measured during this
                                                               -2-1
period using the enclosure  technique ranged between 0.03 ng N m   s   and
         -2  -1
40 ng N m   s  .  The average flux of NO determined in these studies is in
good agreement with the fluxes of NO from ungrazed pastures in Australia
measured by Gal bally and Roy (1978).  The NO flux was found to depend
strongly on soil temperature, increasing rapidly with increasing soil
temperature.   A compilation of these results for data obtained between
5 September 1985 and 28 October 1985 is shown in Table 3.  In addition, this
sampling period was marked  by an extended dry period during the August and
October measurement periods.  For similar soil temperatures, the NO flux was
                                      187

-------
lowest toward the end of the dry periods and increased sharply with the
onset of precipitation.  At the end of the extended dry periods, NC^ is
observed to be present in the effluent from the sampling enclosure.

                                 CONCLUSIONS

     Present estimates indicate that, pertaining to the North American
continent, lightning and biogenic activity in the soil are the largest
natural sources of NO .  However, the estimates of the soil  emissions are
very uncertain.  In the present study, two techniques used to measure
biogenic soil emissions, an enclosure technique and a gradient technique,
have been intercompared during the nighttime hours.  The agreement between
the techniques was good.  In addition, the enclosure technique has been used
to systematically measure the NO  fluxes at a grassland site and to study
the climatological  factors that control  the NO fluxes.  There are no other
results published reporting measurements of NO  fluxes on the North American
continent.  However,  the present results agree with NO fluxes measured at a
temperate grassland site in Australia (Galbally and Roy,  1978).
                                    188

-------
                                 REFERENCES
1.    Galbally,  J.E., and C.R. Roy, Loss of fixed nitrogen from soils by
     nitric oxide exhalation, Nature. 275. 734-735, 1978.
2.    Johansson, C., Field measurements of emission of nitric oxide *
     fertilized and unfertilized forest soils in Sweden, J. Atmos. Chem. .  1,
     429-442,  1984.

3.    Johansson, C., and L. Granat, Emissions of nitric oxide from arable
     land,  Tellus. 36B, 26-37, 1984.

4.    Logan,  J.A., Nitrogen oxides in the troposphere:  global and regional
     budgets,  J. Geophvs. Res.. 38, 10785-10807, 1983.

5.    Slemr,  F., and W. Seiler, Field measurements of NO and NCL emissions
     from fertilized and unfertilized soils, J. Atmos. Chem.. 2, 1-24, 1984.
                                     189

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               TABLE 1.  ESTIMATED OF NATURAL SOURCES OF
                                       Global                   North America
Lighting                                  4                         0.3

                                       (2 - 8)                  (0.09 - 0.6)

Soil Emission                             8           ~             0.6

                                      (1   16)                  (0.08 - 1.5)

Ammonia Oxidation                     (0   10)                   (0   0.15)

Stratospheric Injection                 0.55                       <0.04

                                    (0.37 - 0.67)

Oceans                                   0.2                        —

                                      (0.1 - 1)
aUnits of flux are Tg N yr" .   Estimated range of uncertainty .isted in
 parentheses.
                                      190

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                TABLE 2.   INTERCOMPARISON OF BOX  AND  GRADIFNT
                          MEASUREMENTS OF NO FLUX3

Date
8/24
8/25
8/26
8/27
8/30
8/31
9/01
Box
0.35
0.28
0.83
0.83
0.37
0.37
20.0
Gradient
0.88
0.20
0.81
1.49
0.21
0.16
17.0
aThe result gives the value (or average value)  of the NO flux determined
 during the nighttime hours of each of these dates.   Units of flux are
 Ng N m   s  .
                                     191

-------
      TABLE 3.  THE AVERAGE FLUX OE NO MEASURED AS A FUNCTION OF SOIL
                TEMPERATURE OVER 5U INCREMENTS OF SOIL TEMPERATURE"
 Soil Temperature                                             Average Flux
      Range                                                        NO,   ,
      (°C)                                                   (n?  N m"" s~l)
     0 - 5                                                        0.075

                                                             (0.028 -  0.16)

     5   iO                                                       0.34

                                                              (0.075   1.4)

    10 - 15                                                       0.94

                                                              (0.20 -  3.9)

    15-20                                                        2.5

                                                               (0.72   10)

    20 - 25                                                        4.5

                                                               (2.4   7.3)

    25-30                                                        3.9

                                                               (2.9   8.1)

The range of measured fluxes  for each  temperature  increment  is  listed  in
parentheses.
                                   192

-------
               ALKALINE AEROSOLS EMISSIONS
                     Dale A. GUlette

        Geophysical Monitoring for Climatic Change
                 Air Resources Laboratory
     National Oceanic and Atmospheric Administration
                 Boulder, Colorado 80303
                      Presented at:

Second Annual Acid Deposition Emission Inventory Symposium

                      Charleston, SC




                   November 12-14,  1985
                            193

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                                   ABSTRACT







    Alkaline compounds contained In aerosols emitted  from open  (non-combus-




tion) sources may have the potential to neutralize acid precipitation.   This




potential depends on the quantity of aerosol mass emitted,  Its  transport,




fraction of alkaline compounds In the total aerosol mass, solubility  of the




alkaline compounds, and neutralization potential.  It  Is the mission  of the




Alkaline Aerosols Project to estimate the total neutralizing alkaline aerosol




fluxes by evaluating the above factors.







    Provisional estimates of alkaline aerosol fluxes  showed the  following:







(1) That the two most important sources (unpaved road  dust  and  wind erosion)




    dominate all other sources.







(2) That methods to estimate total alkaline aerosol emissions give total




    fluxes that are larger than observed deposition rates.  This  and  other




    inconsistencies of the estimates show that strong  efforts are needed to




    develop new methods to estimate emissions of alkaline aerosol.







(3) Knowledge Is lacking o.i the fraction of suspended  emitted aerosols,




    Knowledge is also lacking on solubility and neutralization  potential of




    the aerosol.







    Research efforts have been planned to estimate dust emissions from wind




erosion, dust devils, and unpaved roads.  Solubility  and neutralization poten-




tial of aerosols produced by these sources will be determined for several




experiments.
                                       194

-------
                      OPEN SOURCES OF ALKALINE  AEROSOLS










                                  INTRODUCTION







    Alkaline compounds carried In aerosols  emitted  from  open  sources  may  have




the potential to neutralize acid  rain.  To  determine  the importance of  open




sources of aerosols for neutralizing precipitation, a  systematic  appr_*ch was




laid out to estimate the flux of  alkaline aerosol  having sufficient residence




time i i the atmosphere to Interact with precipitation  systems.  After a




general framework of the estimation was laid out,  existing  data and models




were used to give a provisional estimate of alkaline  aerosol  em.  sions.




Additional work was undertaken to determine solubility and  neutralization




potential of the aerosols.  The estimate for quantity  of emitted  soluble  alka-




line aerosols was examined to find shortcomings  and to plan a more  thorough




estimation method.










                                  DISCUSSION







    Emission fluxes of alkaline aerosols (F) that  have potential  to neutralize




acid rain are expressed as follows:




                            E A'  Cf SX N
                                 A




         E  » Emission factor  [mass/(area  yr)]




         A' - Area of emission




         C  - Elemental abundance of  parent  material  (fraction of mass)




         f  • Fractionatlon of aerosol  composition  to parent  material




              composition
                                                                           (1)
                                       195

-------
         S  » Fraction of aerosol mass suspended




         X  - Solubility of suspended aerosol




         N  » Neutralization factor (fraction)




         A  » Total area in question.






    An initial evaluation of eq. (1) was made state-by-state.   The  values for




EA1 were those reported by Evans and Cooper (1980).  Relative  abundance  of the




alkaline compounds was assumed to be the same in the aerosols  as  in the  parent




material (fractionatlon of unity).  Solubility for alkaline elements  was taken




to be that derived from two soluble/insoluble data sets; daily  bulk data from




St. Louis and I year of weekly sampling data for wet side precipitation  from




Glen Ellyn, Illinois (Gatz, et al., 1984).  The composition of  the  parent




material was taken to be the median value of the state soil chemical  survey




data (Boerngen and Shacklette, 1981) for soil erosion and soil  tilling and to




be a combination of median state soil chemical composition and  chemical  com-




position of other road surface materials (see Barnard, et al.,  1985)  for




unpaved roads.  The fraction of aerosol mass suspended was 0.4  based  on  the




fraction of mass smaller than 10 pm and published aerosol sl^e  distributions.




Neutralization potential (N) was set to one even though  this can  only be an




upper limit.







    Results of the provisional evaluation of eq. (1) are shown  for  the 31




eastern states in Table 1 (after Gatz, et al., 1985).  The results  show  the




dominance of the two most important open sources (unpaved roads and wind ero-




sion) over conventional sources for all the alkaline elements  but sodium,




which has little neutralizing potential.
                                       196

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    Table I.  (after Gatz, et aL., 1985).  Total mass and estimated cation
              omissions from major open and conventional sources in the 31
              "eastern" states.  Emission estimates  for open sources are
              Limited to soluble materials <  10 |jm;  these limitations do
              not apply to the estimates of emissions from conventional
              sources.
Source category
OPEN**
Wind erosion
Tilling
Unpaved roads
Sum
CONVENTIONAL***

Total
mass

37,500
7.420
117,000
162,000
8,410
Thousands
Na

107
18.9
172
297
109
of tonnes/y
Mg

47.4
8.28
531
587
119
r (1980)*
K

123
23.7
231
378
71.6
k
Ca

109
18.7
4,110
4,240
274
*   Rounded to three significant  figures.

*"  Total mass emissions are from Evans and Cooper  (1980);  element
    emissions are based on the work of Stensland et  al.  (1985).

*** Sum of separate emissions estimated for the  following  categories:
    Fuel combustion, industrial processes, solid wai_e disposal,
    transportation, and miscellaneous  (less unpaved  roads).   Total  mass
    emissions are from U.S. EPA (1982); element  abundances  used  to
    calculate emissions are from  Gatz  et  al.  (1985).
    Comparisons on a state-by-state  basis  gave  total mass  fluxes  that  are  much

larger than downward fluxes calculated  from  NADP/NTN data.   This  poor

agreement pointed to overestimation  by  the provisional  evaluation cf  eq.  (1)

and pointed to needed research especially  emission  factors  (E),  fractionatlon

factors (f), solubility (X), chemical abundance  of  roads  (c),  and neutraliza-

tion potential (N).
                                       197

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    To correct for this overestimation and to Improve our knowledge of  alka-




line aerosols our plans for research Include:







I). Development of new wind erosion emission equation.  The equation will  be




    physically based and will reiy on results of past research and new




    research.







2). Development of dust devil emission estimations.  These estimates will  be




    based on aircraft baaed dust devil sampling and meteorological classifi-




    cation/generalization to the American Southwest.







3). Development of a new emission equation for unpaved roads.  This will  be




    based on new experimentation ano theory of dust emissions by  vehicles  on




    unpaved roads.







4). Experimentally determined fractionation factors.  These factors will  be




    developed by examining ratios of relative composition of emitted aerosols




    to parent material for both unpaved road emissions and wind erosion.







5). Experimentally determined solubility  factors.  This effort will be  for




    alkaline aerosols material collected  in experiments on road emissions  and




    wind erosion.







6). Chemical survey of unpaved roads in the U.S.   This chemical survey  will




    fill a gap In knowledge on the parent materials of U.S. unpaved  roads.







7). Experimentally determined neutralization potentials.  This work  is




    necessary because alkaline cations are not always associated  with  anions




    such that H Ions are readily replaced.  Composition of the alkaline aero-




    sols must be carefully studied.
                                       198

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                                 CONCLUSIONS







    The present state-of-the-art In  estimating  alkaline  aerosol  emissions




having potential to neutralize  acid  rain  gives  numbers which  are larger  than




NADP/NTN observed deposition  by  roughly a factor  2-3.  The  research  needed  to




improve the estimates will  Include development  of  emission  equations  for wind




erosion and unpaved roads.  Research into solubility,  neutralization  potential




and fractionation factors will  be  incorporated  into  the  new estimations.




Chemical surveys of the  national unpaved  roads  will  also be executed.









                                   REFERENCES







Barnard, W, R., G. J. Stensland, and D. F.  Gatz,  1985:   Alkaline materials




    flux from  unpaved roads:  Source  strength, chemistry  and potential  for acid




    rain neturalization.  Submitted  to Water, Air, and Soil Pollution.







Boerngen, J. G., and Shacklette, H.  T. , 1981:   Chemical  analysis of  soil and




    other surficial materials of the conterminous  United States.  Open  File




    Report 81-197, U.S.  Geological Survey,  U.S.  Dept.  of Interior,  Denver,




    Colo.







Evans, J. S.,  and Cooper, D.  W., 1980:  An  Inventory of  participate  emissions




    from open  sources.   J.  Air  Pollut. Control  Assoc., 30,  1298.







Gatz, D. F., W. R. Barnard, and G. J.  Stensland,  1985:   The role of  alkaline




    materials  In precipitation  chemistry:   A  review  of  the  issues.   Submitted




    to Water,  Air and Soil  Pollution.







Gatr., 0. F. , Stensland,  G.  J. Miller,  M.  V.,  and  Chu,  L.-C.,  1984:   Alkaline




    aerosols:  An Initial Investigation of their  role In  determining preclplta-
                                       199

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tlon acidity.  Final Rept. NSF Grant ATM 77-24294.  Illinois State Water




Survey Contract Report No. 343.
                                  200

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 METHODOLOGY FOR ESTIMATING NATURAL HYDROCARBON EMISSIONS
                            By
                     James A.
         Atmospheric Sciences
           U.S. Environmental
       Research Triangle Park,
Reagan
Research Laboratory
Protection Agency
 North Carolina 27711
                      Presented at:


Second Annual  Acid Deposition Emission  Inventory Symposium

                      Charleston, SC


                   November 12-14, 1985
                            201

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                                 ABSTRACT






     An emission  inventory  system for  biogenic  sources of  hydrocarbons



has been developed. It is based on modifications of the  classic  formula:



               Emissions = £ Biomass  * Area * Emission Factor



It accomodates multiple sources with  emission factors dependent on season,



temperature and  sol<_r intensity.   It  provides emissions  on a  latitude



longitude based grid  system aggregated  by  plant specie,  hydrocarbon  com-



pound, study area (county, state, etc.),  or  time  interval.   The  emission




calculations from this  inventory  have  better  spatial,  source,  temporal



and hydrocarbon compound resolution  than prior  work  has provided.








                               INTRODUCTION





     Part of  the  evaluation  of   the  Regional  Acid  Deposition  Modeling



effort will  include  natural  source  contributions  and effects.  The  new



chemistry model has been extended  to  incorporate biogenic hydrocarbons in



the simulation.  The  use  of  kinetic  reactions employing natural  sources



of hydrocarbons in air and water  requires  definition  of their emissions.



Such an emission inventory should  recognize production of biogenic  hydro-



carbons from:




          - the foliage of trees,  shrubs, and crops



          - decaying leaf 1itter



          - grasses in urban  areas,  pastures, and  grasslands




          - decaying  vegetation  in  rivers,  lakes,  marshes,   and  oceans.



Methane, monoterpenes, and isoprene are the dominant hydrocarbon compounds



produced by biogenic sources.
                                   202

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     A syste atic methodology  was  needed for the estimation  of biogenic

hydrocarbon emissions.  Such an inventory should have the following capa-

bilities:

     - Generate hourly gridded emissions

         (a) for a variable number of hydrocarbon species;

         (b) from  a  variable number  of  plant  species,  leaf  litter,  and
            surface waters;

         (c) for any latitude/longitude-based grid system.

     - Apply temporal  variations to  emission  factors  on  a diurnal  and/or
         seasonal basis.

     - Adjust  emission  factors for  variations  in temperature  and  solar
       radiation.

     - Allow  for  future  modification of  emission factors  to  incorporate
         submodel calculations, including leaf  temperature, fol  iar density,
         soil types, moisture availability, and disease prevalence.

     - Provide  summary  reports of  emissions  by grid cell, county,  U.S.
         Forest Service (USFS) region, and state.

Such a system  has  been  developed  for the Northeastern United  States  and

offers the potential  for meeting one of the requirements of the Regional

Acid Deposition Model.



                                DISCUSSION


     Biogenic hydrocarbon emissions  are a function  of emission  rate  and

biomass within a given area.   An emission inventory  for  them  includes of

building files of  descriptive data  on land use,  emitter density, and emis-

sion factors.   It  also  includes   algorithms  implementing  the  relations

between the data elements of these descriptive  files.


     Area categorization  has  been   primarily  derived  from  the  USGS Land

Use and Land Cover map series supplemented as needed from other satellite
                                   203

-------
and aerial  sources.  Coverage areas for the  following  land use  classifi-

cations were estimated to the  nearest  five  percent  for each grid  cell:

     -urban                      -water

     -agricultural                -barren  land

     -rangeland                  -nonforested wetland

     -deciduous forest           -mixed agricultural  and rangeland

     -coniferous forest          -rocky open  areas  occupied by  low
                                  growing  shrubs  and  lichen (not
     -mixed forest  (including     including  tundra)
      forested wetland)


     Mixed forest was  split  between the coniferous and  deciduous classi-

fications, with data  from the  U. S.  Forest  Service inventories used  to

allocate area to individual  species.   The canopy area  is  a  function  of

the diameter at  breast height (dbh), which  is divided  into ten  intervals

or classes.  The area  for one tree in a dbh  class multiplied by the  num-

ber of trees in the class and summed across  classes  gives  the  total  area

for a  specie.   A mix  ratio   of the  specie  area  to  the  total  area  summed

across all  species  of  the same forest type,  deciduous  or coniferous,  was

used to allocate the proportion of the corresponding forest  type area  to

that specie.  Agricultural  land was apportioned among crops  based  on  the

1978 Census of  Agriculture as aggregated  to  the county level by the  Oak

Ridge National   Laboratory.   Several  state atlases  were used to resolve

the split between  fresh and  salt  water, especially  in  estuaries.   A  file

of the overlap  between grid  cells and  study  unit  (county,  forest region,

etc.) was  used  to  partition  classification  areas  among the  grid  cells.

It is  used  in   reverse to  summarize emissions  at  the   study unit  level.


     Most of the hydrocarbons emitted  by  vegetation are released  by  the

foliage.   The branches, twigs,  bole, and  root emissions are negligible in


                                    204

-------
comparison.  Foliage weight can be estimated from algorithms which  relate

foliage weight to tree diameters.  Tree diameter inventories are compiled

by the U. S. Forest Service for each state.  Emission factors for surface

waters, leaf litter, and some crops are area dependent and  do not require

a foliar weight estimate.


     The emission factor is expressed as moles or micrograms of  hydrocar-

bon emitted  over  a time  interval  per  unit  of  land  area  or dry  foliar

weight.  The identity  of the  hydrocarbons emitted is reported as  isoprene,

monoterpene, and/or unspecified  nonmethane  hydrocarbon.   When  emission

factors were  unavailable  for a  particular  vegetative type,  an  emission

factor from a biologically similar vegetation type was used.  These emis-

sion factors have several possible sources  of error:

     - Measurement error due to the experimental  method employed disturb-
       ing the natural emission process.

     - Inappropriate substitution of  emission  factors due  to unavailable
       data.

     - Emission factors may  vary with environmental  parameters  including
       geographic location, soil  conditions, and elevation.


     Because emission  factors are  known to vary with  light  and tempera-

ture, the  system  accounts for  seasonal changes  in  solar  radiation  and

surface temperature.   It  is  assumed  that  the leaves  of  all plants  are

exposed to full sun and the  same surface temperature.  Because  there may

be large variations in  solar  radiation and  surface  temperature,  hourly

estimates are made  of  these  variables.  Solar radiation is  derived  from

formulas that  give  the  solar  zenith  angle  as  a  function  of  latitude,

longitude,  date,  and time of day.  The  system  does  not currently account

for attenuation due to  clouds  and  aerosols, but provision  has  been  made

for this variable in  future  versions  of the system.   Thus, the emissions


                                    205

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generated by the system are maximum  rates with  respect  to the effects of




Sunlight.  Surface  temperatures  from  the  National  Weather  Service  are




transformed to  average  grid  cell  temperatures   by an  objective  mapping




technique for mesoscale processes  based  on  numerical filtering.   All  of




the emission factors have been standardized  to 30°C.  It has been  assumed




that all monoterpene emitters  and  nonmethane  hydrocarbon  emitters (other




than isoprene)  respond to temperature  in a manner  similar to monoterpene




emissions from  slash  pine.   Likewise all  isoprene  emitters have  been




assumed to respond  to changes  in  light And  temperature as  does  isoprene




from 1ive oak.








                               CONCLUSIONS






     An emission inventory system has been developed to  meet the require-




ments of the ne.; kinetic reactions  employing  natural sources of hydrocar-




bons in  air  and water.    It  provi  ies much better  resolution  than  prior




inventories especially  in terms of  spatial and temporal  variation.  It is




open ended allowing inclusion  of different areas,  sources,  emission  fac-




tors and temporial  variations.  It  will provide  insight  into the relative




contribution of a  few species  to the  total emissions in an area.  A syste-




matic,  detailed inventory increases the confidence  in the emissions since




variances can be reasonably calculated.  Future  research on emission fac-




tor development, module extensions,  etc.  can  be guided by  the knowledge



gained  from the system.
                                    ?06

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       SESSION 5:  RELATED EMISSION INVENTORY DEVELOPMENT ACTIVITIES

Chairman:  J. David Mobley
          Air and Energy Engineering Research Laboratory (Mp-61)
          U. S. Environmental Protection Agency
          Research Triangle Park, NC  2771_
                                     207

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      SUMMARY OF A 1982 NATIONAL EMISSIONS INVENTORY

              FOR REGIONAL MODEL DEVELOPMENT
                     Steven L.  Heisler
        Environmental Research  and Technology,  Inc.
                975 Business Center Circle
              Newbury Park, Jalifornia  91320
                       Presented at:

Second Annual Acid Deposition Emission Inventory Symposium

                Charleston,  South Caroline

                   November  13-14,  1985
                         208

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             SUMMARY OF A  1982 NATIONAL EMISSIONS INVENTORY
                     FOR REGIONAL MODEL DEVELOPMENT
               By:  S.L. Heisler
                    Environmental Research and Technology, Inc,
                    975 Business Center Circle
                    Newbury Park, California  91320
                                ABSTRACT

     None of the regional and national emissions inventories available in
1982 were suitable for regional deposition or air quality modeling.
Therefore, procedures were developed and applied to produce a suitable
1982 inventory for the United States and southeastern Canada.  The
inventory includes total emitted particulate matter (TEP),  alkaline TEP,
SO., primary SO,, NO, N0_, NH_, and hydrocarbons in nine photochemical
reactivity classes.  Point source geographic locations are  resolved to
±100 meters, and stack data are available for calculating emission
injection height.  Area source emissions are available by county or
within 1/4° longitude by 1/6° latitude elements of a grid system.  The
inventory contains annual, seasonal, weekday, weekend, and  3-hourly
average emission rates.  United States emissions of TEP, S02, NO  and HC
in the inventory are 1,698, 26.5, 23.8, and 20.8 million tons per year,
respectively.   The point source data are from various years; about
one-half of the S09 and NO  emissions pertain to 1982.  Older data for
                  £.       A
some states are currently being updated.  This inventory is currently
being compared with the 1980 National Acid Precipitation Assessment
Program (NAPAP) inventory by source category and state to identify and
evaluate differences.  Procedures used to develop them are also being
compared to evaluate consistency between the inventories and improve
inventory development procedures in general.
                                209

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             SUMMARY OF A 1982 NATIONAL EMISSIONS INVENTORY
                     FOR REGIONAL MODEL DEVELOPMENT

                              INTRODUCTION

     None of the regional and national emissions inventories that were
available in 1982 '  '  ' '  were suitable for regional modeling
applications throughout the United States and eastern Canada.   They were
limited with respect to geographic coverage, data concurrency, chemical
substances, or spatial resolution, or specification of uncertainties.
To improve upon the  situation, the Electric Power Research Institute
(EPRI) sponsored the development and application of procedures to compile
a 1982 emissions inventory for the contiguous United States and south-
eastern Canada ' .
     The inventory includes total emitted particulate matter (TEP),
alkaline TEP,  SO   primary 30^, NO,  NO , NH   and hydrocarbons (HC)  in
nine photochemical reactivity classes.  Point sources geographic
locations are  nominally resolved to ±100 meters.   Stack heights,
diameters, flow rates, and exit temperatures are included for  calculating
emission injection height.  Area source emission rates are available by
county.  Factors to  allocate these county-wide data to elements of a
1/4° longitude by 1/6° latitude grid system are also available.  The
inventory contains annual, seasonal, weekday, weekend, and diurnal
(3-hour resolution)  average emission rates.

                               DISCUSSION

     Annual emissions from point and area sources are in Table 1.  Almost
all TEP emissions are from wind erosion and agricultural tilling area
sources.  Point sources emit over 90% of the SO  in the country.  Point
and area sources contribute equally to NO  emissions, and area sources
account for 70% of HC emissions.
                                  210

-------
     Although the nominal  time period of the inventory is 1982, it
contains point source data  from several years.  The national distribution
of annual point source emissions by year-of-record is in Table 2.   About
one-half of the SO  and NO  emissions and 30% and 27% of the TEP and HC
                  ^        X
emissions are for 1982.  Less than half of the point source emissions for
any material pertain to years before 1981.
     Most point source SO   and NO  emissions are from a relatively small
                         ^       X
number of large sources.  Almost 80% of point source SO  emissions are
from 406 facilities that each emit more than 10,000 tons per year, and
about 70% of point source NO  emissions are from 440 facilities that each
emit more than 5,000 tons per year.  The 1,289 largest emitters account
for about 73% of point source TEP emissions, and the 784 largest emitters
account for about 75% of point source HC emissions.
     Annual emissions by source category are shown in Table 3.  Almost
all of the TEP is emitted by fugitive area sources, particularly wind
erosion and agricultural tilling.  Emissions from unpaved roads are also
substantial.  Industrial processes are the largest point source
contributors to national TEP emissions, and residential fuel use is the
largest combustion source.  TEP emissions from mining, which could be
important in some parts of the country, are not in the inventory.
     Fossil-fueled electric utility boilers account for 66% of SO,
emissions.  Industrial boilers and industrial processes each contribute
14%.  The remaining 6% is from-other fuel combustion.
     Electric utility and industrial boilers account for 53% of national
NO  emissions, and motor vehicles contribute 30%.  Industrial processes,
  X
which include refinery and chemical plant process heaters, contribute 9%.
     Industrial processes, motor vehicles, miscellaneous solvent uses,
and residential fuel combustion are the largest HC emitters.  Most
industrial process emissions are from storage tanks and solvent use.
Wood combustion accounts for most HC emissions from residential fuel use.
     Annual NH_ and alkaline TEP emissions are listed by source category
in Table 4.   Emissions from bacterial action in the ground and from
livestock account for most of the NH» in the inventory.  However,
emissions from fertilizer use are not included.  This category may be
significant.  Wind erosion and agricultural tilling emit most of the
alkaline TEP.
                                   211

-------
     Tables 5 and 6 show comparisons of total United States SO- and NO
emissions with Version 3.0 of the 1980 National Acid Precipitation
                                    Q
Assessment Program (NAPAP) inventory .   Although these national totals
agree within 5%, some of the procedures and data sources used to develop
the inventories were different.   In particular, electric utility data in
NAPAP were derived from forms filed by utilities with the Department of
Energy, while data in the EPRI inventory came from the National Emissions
Data System , state inventories,  and some plant operators.   These and
other differences may have produced significant differences in emission
rates from some source categories in some regions of the country.  It is
important tha* such differences  be identified and evaluated, since they
could affect results of regional  modeling applications.
     Procedures used to c.   ulate primary SO,,  NO, N07,  and EC reactivity
class emissions also differed between the inventories, as did procedures
used to calculate seasonal,  day-of-week,  and diurnal average emission
rates.   The effects of these differences  must also be evaluated.
                                  212

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                               CONCLUSIONS

     The data in  the inventory indicate that area sources, particularly
wind erosion and  agricultural tilling, dominate annual United States TEP
and alkaline TEP  emissions.  Point sources, principally electric utility
boilers, emit most of the S02 in the United States.  Point and area
sources emit nearly equal amounts of NO    Motor vehicles, industrial
processes, miscellaneous solvent uses, and residential combustion are the
major sources of  EC.  Animals and bacterial action in the ground are the
major sources of  NH_.
     The inventory does not currently include fugitive TEP emissions frora
surface mining, which could be significant in some parts of the country.
NH_ emissions from fertilizer use also are not included.  These sources
will be added to  ""he inventory in the future.
     A major fraction of national point source emissions in the inventory
pertain to time periods before 1982.  Work is under way to update some of
the older values  to improve data concurrency
     Although total S0» and N'O  emission rates for the United States are
almost the same in the EPRI and 1980 NAPAP inventories, some data sources
and procedures used to develop these inventories were different.  These
differences may have caused emissions from some sources to differ signif-
icantly in some parts of the country.  Therefore, these inventories
are currently being compared by source category and state to identify and
evaluate differences.  Procedures used to develop the two inventories are
also being compared to evaluate the consistency between the inventories
and, hopefully, improve inventory development procedures in general.
     Acknowledgement.  This work was supported under Electric Power
Research Institute Contract RP1630-23.
                               REFERENCES
1.   AEROS Manual Series; Volume II: AEROS User's Manual, USEPA Research
     Triangle Park, NC, EPA-450/2-76-029, December  1976.
                                   213

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2.   H. A. Klemm and R.  J.  Brennan,  Emissions Inventory for the SURE
     Region, GCA/Technology Division for the Electric Power Research
     Institute (EPRI),  EA-1913,  April 1981.

3.   C. M. Benkovitz, "Compilation of an Inventory of Anthropogenic
     Emissions in the United States  and Canada."  Atmos.  Environ.  16 (6):
     1551 (1982).

4.   F. M. Sellars, et al., Northeast Corridor Regional Modeling Project
     Annual Emission Inventory Compilation and Formatting,  Volumes I
     through XVIII, EPA-450/4-82-013a-r, August 1982-July 1983.

5.   Emissions,  Costs,  and  Engineering Assessments,  Work Group 3B,
     U.S./Canada Memorandum of Intent on Transboundary Air  Pollution,
     Junr 1982.

6.   S. L. Heisler, "Emission Inventory Requirements for Deposition and
     Regional Air Quality Model  Development:  A Summary."  In:
     Proceedings: First  Annual Aicd  Deposition Emissions Inventory
     Symposium,  Research Triangle Park, NC,  EPA-600/9-85-015,  May  1985.

7.   S. L. Heisler, et  al., "The EPRI 1982 Air Pollutant Emission
     Inventory."  Presented at the 78th Annual Meeting of the  Air
     Pollution Control Association,  Paper 85-4.3,  Detroit,  MI,
     June 16-21, 1985.

8.   D. A. Toothman, et  al., Status  Report on the  Development  of the
     NAPAP Emission Inventory for the 1980 Base Year and Summary of
     Preliminary Data, Research  Triangle Park, NC,  EPA-600/7r84-091,
     December 1984.
                               214

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3.    C.  M. Benkovitz, "Compilation of an Inventory of Anthropogenic
     Emissions in the United States and Canada."  Atmos.  Environ.  16 (6)
     1551 (1982)

4.    F.  M. Sellars, et al., Northeast Corridor Regional Modeling Project
     Annual Emission Inventory Compilation and Formatting, Volumes I
     through XVIII, EPA-450/4-82-013a-r, August 1982-July 1983.

5.    Emissions, Costs, and Engineering Assessments, Work Group 3B,
     U.S./Canada Memorandum of Intent on Transboundary Air Pollution,
     Junr 1982.

6.    S.  L. Heisler, "Emission Inventory Requirements for Deposition and
     Regional Air Quality Model Development: A /ummary."  In:
     Proceedings: First Annual Aicd Deposition Enissions Inventory
     Symposium, Research Triangle Park, NC, EPA-6CfV9-85-015 , May 1985.

7.    S.  L. Heisler, et al., "The EPRI 1982 Air Pollutant Emission
     Inventory "  Presented at the 78th Annual Meeting of the Air
     Pollution Control Association, Paper  85-4.3, Detroit, MI,
     June 16-21, 1985.

8.    D.  A. Toothman, et al., Status Report on the Development of the
     NAPAP Emission  Inventory for the 1980 Base Year and Summary of
     Preliminary Data, Research Triangle Park, NC, EPA-600/7-84-091,
     December  1984.
                                    215

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Table 1.   ANNUAL UNITED STATES POINT AND AREA SOURCE EMISSIONS
   Point Sources

   Area Sources

   Total
                                    Emissions
                                (million tons/year)
TEP

5.1
1693
1698
—2
24.4
2.1
26.5
NO
X
11.9
11.9
23.8
HC

5.9
15.9
20.8
      Table 2.   DISTRIBUTION OF INVENTORIED UNITED STATES
                POINT SOURCE SMISSIONS BY YEAR-OF-RECORD
                 Emissions (percent of total)
                      (million tons/year)
  Before 1980
1980
1981
1982
After 1982
TSP
so2
NO
X
HC
1.4
1.8
1.3
2.2
(27%)
(7%)
(11%)
(37%)
0.7
2.5
1.3
0.9
(14%)
(10%)
(11%)
(15%)
0.9
5.5
2.8
0.6
(17%)
(23%)
(24%)
(10%)
1
13
5
1
.5
.0
.8
.6
(30%)
(53%)
(48%)
(27%)
0.6
1.5
0.8
0.6
(12%)
(6%)
(6%)
(10%)
                              216

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Table 3.  ANNUAL UNITED STATES EMISSIONS BY SOURCE CATEGORY
                                        Emissions
                                   (thousand tons/year)
Source Category
Stationary Source Fuel
Combustion
Electric Utilities
Industrial Boilers
Commercial/ Institutional
Residential
Subtotal
Industrial Processes
Non-Ferrous Smelters
Other Processes
Subtotal
Solid Waste Disposal
Transportation
TEP


800
588
115
1,011
2,514

184
3,457
3,641
418

Motor Vehicles 129,519*
Airplanes
Vessels
Railroads
Other Off-Highway
Subtotal
Miscellaneous
Wind Erosion
Agricultural Tilling
Construction
Cattle Feedlots
Forest Fires
Other Burning
Gasoline Marketing
Miscellaneous Solvents
Subtotal 1,
Total 1,
^Includes entrained particulate
Includes entrained particulate
82
26
49
59
129,735

956,300
595,000
9,432
440
288
560
0
0
562,020
698,328
matter
matter
SO,
i

17,380
3,699
610
177
21,866

1,092
2,690
3,782
44

365
12
172
112
114
775

0
0
0
0
3
3
0
0
6
26,473
NO


7,920
4,138
354
404
12,816

47
1^994
2,041
176

6,869
109
141
725
827
8,671

0
0
0
0
68
102
0
0
170
23,874




1

2
3


5
5


6




7








3
4
21
HC


59
,039
15
,089
,202

16
,529
,545
677

,195
161
427
176
517
.476

0
0
0
0
325
417
960
,157
,859
,759
from road surfaces.
from unpaved air strips.
                           217

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      Table 4.  ANNUAL UNITED STATES NH3 AN^ ALKALINE TEP EMISSIONS
                                              Emissions
                                        (thousand tons/year)
      Fuel Combustion

      Industrial Processes

      Unpaved Roads

      Paved Roads

      Construction

      Wind Erosion

      Agricultural Tilling

      Cattle Feedlots

      Other Livestock

      Land Surfaces

      Human Beings and Pets

      Total








1
4
5

NH
774
23
0
0
0
0
0
,189
,900
,103
266
Alkaline TEP
0
0
3,972
111
300
46,960
18,880
168
0
0
0
12,255
70,39 1
Expressed as equivalent calcium carbonate.

-------
             Table 5.   COMPARISON OF ANNUAL SO  EMISSIONS  WITH
                      THE 1980 NAPAP INVENTORY
                                              Emissions
                                         (million tons/year)

                                         NAPAP3         EPRI

          Electric Utilities              17.3          17.4

          Non-Utility Combustion           4.6           4.5

          Non-Ferrous Smelters             1.2           1.1

          Transportation                   0.9           0.8

          Other Sources                    3.1           2.7

          Total                           27 1          26.5
               Table 6.  COMPARISON OF ANNUAL NO  EMISSIONS
                        WITH THE 19SO NAPAP INVENTORY
                                              Emi ss i ons
                                         (mi1 lion to n s/yea r_)

                                         NAPAPa         EPRI

          Electric Utilities                8.1          7.9

          Non-Utility Combustion            5.2          •* 9

          Non-Ferrous Smelters              0            0

          Transportation                    9.1          8.7

          Other Sources                    1 • 3           1 -3

          Total                           23.7          22.8
3National Acid precipitation Assessment Program  I960  inventory
 Version 3.0s.
                                  219

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            GENERATION OF TEMPORALLY-RESOLVED
             EMISSIONS INVENTORIES FOR CANADA
                      Trevor Scholtz
          MEP Company, Markham, Ontario,  Canada
                        Frank Vena
         Environment Canada,  Hull, Quebec,  Canada
                      Presented at:
Second Annual Acid Deposition Emission Inventory Synposium
                Charleston,  South Carolina
                   November  12-14,  1985

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          ABSTRACT

          Processing of North American anthropogenic and natural source
emissions for the Canadian long-range transport model (ADOM) Involves
the generation of an hourly speciated emissions file on the 127 km
Eulerian grid.  Some anthropogenic and most natural emissions are
strongly dependent on local climate and hourly meteorology.  The use of
generally derived or average temporal factors for these sources can
lead to inconsistencies between between prevailing meteorology and the
estimated emission rates used in evaluating the ADOM model.  This paper
describes a system for preprocessing of anthropogenic and natural
source emissions using the ADOM database of hourly gridded
meteorological data and other temporally variable parameters to provide
an hourly emissions file which avoids some of the inconsistencies
inherent in the use of average temporal factors.
                                      221

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 i.        INTRODUCTION

          A Eulerian long-range transport model Is presently being
 developed by the Ontario Ministry of the Environment, with Environment
 Canada and the Federal Republic of Germany as co-sponsors.  This model,
 known as the ADOM model, includes a model of the atmospheric chemistry
 which requires a detailed knowledge of the reactant mix in each 127 x
 127 km grid cell.  This mix is partly dependent on the spatial and
 temporal distribution of speciated emissions.  While presently
 available emissions Inventories provide reasonably good spatial
 resolution of the annual average emissions, temporal factors are
 generally based on typical seasonal and diurnal variations rather than
 year specific or hourly meteorological data.  The use of typical
 temporal profiles for climatologically and meteorologically dependent
 sources such as open anthropogenic and natural sources can lead to
 Inconsistencies between the prevailing hourly meteorology and the
 estimated emission rate.  Since under some circumstances, open sources
 and other meteorologically dependent emissions can overwhelm their
 better defined process-related counterparts, it is important for
 purposes of model evaluation to provide a more realistic temporal
 resolution of these emissions.  Part of the database for the ADOM model
 comprises hourly meteorological data as well as soil moisture and
 temperature, gridded to the 127 km Eulerian grid for the subject
 period.  The availablity of this database, facilitates the more
 realistic estimation of meteorologically forced emissions.

          This paper describes an emissions preprocessor for
anthropogenic and natural sources which provides a first level of
 refinement In preparing an hourly resolved emissions file and which
avoids many of the Inconsistencies inherent in using typical temporal
 factor profiles.  This preprocessor will have as Its first application,
the preparation of an emissions file for the 1980 PEPE/NEROS
experimental period.  Details of the methodology used to derive
seasonal, day-of-week and diurnal temporal factors for anthropogenic
area sources and natural sources are given In References (1) and (2).
                                    222

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2.        DISCUSSION

2.1       Emissions Processing  System  for  the ADOM

          Figure  1 shows  the general steps  taken in processing the
(1980) Canadian and U.S.  point  and area  source  emissions.  The Canadian
emissions file contains annual  average 1980 anthropogenic emissions for
area and minor point sources together  with  temporal factors for the
PEPE/NEROS period for a selection of major  point sources.  The area
source emissions  are provided on a 127 x 127 'urn gridded basis.  The
U.S. anthropogenic emissions inventory is  on a  county basis and
includes some temporal factor information  as part of the file.  The
system provides a facility  to allocate the  U.S. emissions to the ADOM
grid, reformat and merge  them with the Canadian data to provide a
single emissions  file.  This merged file is then processed through the
emissions preprocessor which applies the temporal factors to
process-oriented  emissions  and  which uses  appropriate climatological
arid meteorological data to  generate temporally  and spatially resolved
open anthropogenic and natural  source  emissions.  The output from the
system is a file  of gridded hourly emission rates for a specified
period.   While the system is intended  to process both Canadian and U.S.
sources , the climatological data and other  emission parameter data for
open and natural sources as well as other meteorologically dependent
sources  have so far only been prepared for  Canada for the year 1980.

2.2       Temporal Emissions Preprocessor

          Figure 2 shows the subsystem for  generation of temporally
resolved emissions.   For purposes of this  preprocessor, emissions are
divided  into the following  three classes:
                                       223

-------
          (1)  Production., Consumption and
               Process Related Emissions
          For sources in this class, the preprocessor function is
simply to apply prescribed seasonal, day-of-week and diurnal temporal
factors to the annual average emission rates.  Some sectors in this
class do have a climatic component (for example, gasoline and diesel
marketing, motor vehicle and residential heating emissions).  The
gridded annual average emissions in A are processed by G using
seasonal, day-of-week and diurnal factors contained in file B.
Seasonal factors are based on 1980 quarterly and monthly production,
consumption or other statistics available from Statistics Canada.
These statistics give an estimate of the province-wide monthly or
quarterly relative activity variations.  The annual average emissions
are available for Canada on the 127 km grid and the seasonal activity
profile and therefore the seasonal temporal factors are assumed to be
uniform throughout the province.  Where climate dependence is
significant (Table 1) the normalized seasonal profiles of the relevant
climate variable/s have been estimated for some thirty-five climate
zones of approximately 4  in latitude width as shown in Figure (3) from
Reference (2).  These zonal factors which reflect the intra-province
variation of climate extremes are used to weight the activity related
temporal factors to resolve the spatial variation of seasonal temporal
factors in each province.  These spatially resolved seasonal factors
are contained in file B.  Where possible, 1980 climate data have been
used; heating degree day distribution for example.  Figures 4 and 5
from Reference (1) are examples of the computed latitude variation of
seasonal temporal factors for diesel and gasoline marketing and
gasoline powered motor vehicles.

          Specific data on day-of-week or diurnal activity profiles
were not available and these temporal factors are extracted from other
studies as well as from a limited survey of industry practice.
                                    224

-------
          (ii)  Open Anthropogenic  Sources

          Sources  in this class  (Table  1) are mainly contributors to
suspended particulate bearing alkali and alkaline earth metals as well
as iron and manganese.  The alkaline material is important for pH
dependent wet chemical reactions while  the Fe and Mn ions catalyse wet
SOn oxidation.  Open source particulate emissions are strongly
dependent on prevailing meteorology, vegetative and snow cover, as well
as silt and moisture content.  Emissions in  this class are computed in
module E using the hourly gridded meteorological data in C.  In some
cases an emissions algorithm is  used to estimate the grid average rate,
for others only a  likelihood weighting  factor for certain activities
can be assessed on the basis of  meteorology  (for example spraying
activities, slash  burning).  Some emissions  which are primarily
determined by non-meteorological factors such as road dust are
suppressed during  and subsequent to precipitation events.  Again,
climate related parameters in the emission algorithm have been
estimated on a 4   latitude basis while  parameters such as soil type and
area of agricultural land have been gridded  to the  127 km resolution.

          (iii)  Natural Sources

          Apart from time-stationary factors such as vegetation and
soil type, natural source emissions are entirely determined by climatic
and meteorological factors.  While some annual average emission
estimates are available for natural sources, these  are used where only
seasonal variation is resolved,  for all other natural sources, the
hourly emission rates are determined using an emission algorithm
together with zonal climate data and hourly  gridded meteorological data
(Table 2).
                                     225

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3.        CONCLUSIONS

          In order to resolve natural and oorae anthropogenic emission
rates to the spatial and temporal scales required by the ADOM Eulerian
long-range transport model, it is necessary to consider the impact of
spatial climate variability as well as hourly meteorology on the
temporal variation of emission rates.  Using the hourly gridded
meteorological fields and other data from the ADOM database it is
possible to prepare an hourly emissions record which refines the
emissions estimates by including these effects.
          REFERENCES
I.   MEP Company and Ontario Research Foundation,  "Temporal Factors for
          1980 National Anthropogenic Area Source  Emissions", Report
          prepared for Environment  Canada, July 1985.
2.   Environmental Applications Group Ltd., "Gridded Natural Emissions
          Inventory and Temporal Algorithms",  Report prepared for
          Environment Canada,  May 1985.
                                      226

-------
                           Table 1
            Climatologically and Meteorologically
             Dependent Anthropogenic Area Sources
      Source

Gasoline Powered Motor Vehicles

Gasoline and Diesel Marketing

Residential Heating

Paved and LFnpaved Roads

Pesticide Application

Slash Burning

Tailings Piles

Landfill Sites

Tilling
    Parameters

Seasonal mean e_ (T)

Monthly mean e  (T)

Seasonal degree days

Precipitation

Wind, Precipitation

Wind, Precipitation

Wind, Seasonal PE

Growing degree days

Precipitation
                                 227

-------
                                 Table  2
                              Natural  Sources
    Source
Seasonal   Diurnal
Species
Parameters
 Marine  Salt
                      Ca,  Mg,  K,  SO
                      Fe,  Mn
                                                          wind, ice cover
 Soils
                      NH-,  VOC,  NOX,
                      S(B2S)
                soil temperature,
                air temperature,
                snow cover
Vegetation
                      VOC
                                          vegetative  state,
                                          air  temperature
Soil Erosion
                                      K, Mg, Ca, Fe,
                                      Mn, particulate
                                         wind,  snow  cover,
                                         vegetative  state,
                                         soil moisture
Lightning


Animal Wastes
                     NOX
                                         ,  VOC
                climatological
                                         climatological
Forest Fires
                                      SO-, CO, NOX,
                                      VOC, Ca, Mg, K,
                                      SO   particulate
                                         climatological
Marines Waters
                                      VOC, CO
                                         ice cover
                                         228

-------
Canadian 1980
Point and Area
Source Emissions
U.S. 1980 Point
and Area Source
Emissions
                            Merge and
                            Grid to
                            ADOM Grid
Cl imatological and
Meteorological Data

	 fc

Temporal
Emissions
Preprocessor
•fej

Hourly
tmissions
File
Figure 1:  Emissions Processing for the ADOM Model

-------
 1980 Annual
 Averaged
 gridded
 emissions
 inventory
Zonal temporal
factors for
emissions
                                      Emissions

                                     Preprocessor
 Hourly
 resolved
 1980 emissions
 file
 Hourly gridded
 meteorological
 data
 Zonal temporal
 factors for
 emission
 parameters
                                      Emission

                                     Algorithms
Other data
and parameter
files from
Eulerian
model input
  Figure  2:   Computation of  temporally  resolved emissions for the ADOM Model.

-------
                                                                  CLIMATE    ZONES
Figure 3

-------
                  29  DIESEL  S, GRSOLINE MflRKETING

                       SIC:  60802  GflSOLINE MflRKETING
        RLL  POLL
ZONEi  02

1.12 -
0.90 .
0.03 .
0.09 .
118

77









                         1.39
        FILL POLL
ZONEi  OIL

1.10 .
0.90 .
0.77 .

0.30 .
127


68












        flLL POLL
RLL  ZONES
 HI  SP SU  FA
 HI  SP  SU  FA
1.17 -
1.09 .
0.00 .
0.17 .
42



165



 HI  SP  SU  FA
                   35 ONTRRIO
                                 60 YUKON
    Figure 4:  Seasonal temporal factors adjusted for Climate, Diesel and Gasoline Marketing.

-------
                                                  nui ufiuaI LC5
   1.07
        12100  TOf.  PflRT.
        RLL  ZONES
1.03 .


1.00 -


O. SO -
   Ci.93
                 105
          95
                                 112603  N1TRO. OXIDE
                                 ZONEi  02
          UI  SP  SU  FM

1.02 .
1.00 .
0.87 .
0.93 -
103 103








96





                                                            i.to
     (12101   CHRB.MONOXI
     ZONEi  02
1.11 .


1.00


0.00 .


0.72
                                                                 120
                                                                         80
                                   UI  SP  SU  FA
                                                                  UI   SP  SU  FR
     U3101   VOTflLlIC
     ZONEi Oc'.
i.ao


1.14


1.00 .


0.00 .


0.72
                                                                                             120
                                                                                              HI  SP SU  FA
ro
U)
OJ
         12100   TOT.
         flLL ZONES

1.03 -
1.02 .
0.90 .
0.94 .






107












                                                   35  ONTARIO
                                  142603   NITFlO. OXIDE        U2101   CRRB.MONOXI        U3101   TOTflL HC
                                  ZONEi 05                   ZONEi 05                   ZONEi  05
                                                         1.21 .,	„        I.21
          UI  SP  SU  Ffi
1.01 .
1.00 .
0.99 .
0.97 .




98

102

                                                            1.09 .
                                                         0.97
                                                         0.03
                                   UI  8P  SU  FP
                                                         0.73
                                                                  114
                                                                         8n
                                                                                    1.09 .
                                                                                        0.97 .
                                                                                        0.03 .
                                                                                        0.73
                                                                                          114
                                                                                                 80
       UI  SP  SU FA
       UI  SP  SU  FA
                                                  60 YUKON
          Fl'gure 5:  Seasonal  temporal  factors adjusted for Climate; Gas Powered Motor Vehicles.

-------
          HISTORICAL ANALYSIS OF SULPHUR  DIOXIDE
          AMD NITROGEN OXIDES EMISSIONS IN  CANADA
                      Tom Furmanczyk
                    Environment  Canada
                  Ottawa, Ontario,  Canada
                       Presented At:
Second Annual  Acid Deposition  Emission  Inventory  Symposiun
                Charleston,  South  Carolina
                   November  12-14,  1985
                             234

-------
ABSTRACT

          Anthropogenic sulphur  dioxide and  nitrogen oxides emissions  in Canada
were calculated  biennially from  1970  to  1980.   For the  most  part,  emissions
were based  on national  statistics covering  the  production,  distribution  and
consumption  of  goods  and services  and on  estimates  of  appropriate  emission
factors.

          The trend in the emisisons of sulphur  dioxide has been  steadily  down-
ward in the  last  decade.   Traditionally the  largest source  of  sulphur dioxide
has been the  non-ferrous  smelting sector where  emissions  have  decreased   by 44
percent.  Other  major sources are  the  generation of thermal  power from  which
emissions  have  been  rising  and  the  combustion  of  fuels  in   industrial,
residential  and commercial applications where  a  downward trend  in emissions  was
observed.   The emissions of nitrogen oxides  come  predominantly  from  transporta-
tion and  the combustion  of   fuels,  including thermal  power  generation,   which
account for  dhout 60  and 35  percent  respectively  of  total  emissions.   This
ratio has remained relatively constant during  the  study period.
                                        ?35

-------
1.   INTRODUCTION

          The  current  concern  with the long  range  transport of air pollutants
(LRTAP)  is  with  sulphur  dioxide  ($02)  and  nitrogen  oxides (NOX)  which  give
rise  to what  has become  known as  "acid  rain"  or,  more  appropriately,  acid
deposition.  This  phenomenon occurs  because prolonged atmospheric transport  of
sulphur  and nitrogen  oxides  provides sufficient  time  for  these  compounds  to
undergo  chemical  and physical  transformations into  acidic  compounds, which are
subsequently deposited either  in wet  or  dry form  at locations distant from the
originating sources of pollution.  This  acidic deposition  causes acidification
of  sensitive  freshwater lakes  and soils,  as has  become  evident in  parts  of
Eastern North America, adversely affecting  various ecosystems.

          This  paper  summarizes  the results of  a  retrosoective  emissions
inventory  for  Canada  of  SOj  and  NOX from 1970 to  1980.   The  inventory  of
acid rain precursor pollutants  is  presented nationally  and regionally by major
source  sectors and categories.   This  information  is important in understanding
the  relationships  between  releases  of   pollutants  to  the  atmosphere  and
potential environmental effects and in the  assessment of control options.

          The  source  categories  included   in  the  analysis  are  industrial
processes,  fuel  combustion  from  stationary   sources,  transportation and  all
other  important  anthropogenic  sources.     The emissions  are  calculated  from
statistics  covering fuel consumption  and  industrial  output by using consistent
methodologies within each sector.

2.   DISCUSSION
     2.1  Methodology

          The  emission trends  inventory  was compiled  on  a  sector  level  by
province.   The  emission  estimates  were  then aggregated  to  give  provincial
                                       236

-------
(regional) and  national  emissions.   The  calculation  procedure by  sector can
generally be expressed as:
                Emission = Activity Level  x  Emission Factor
In order to  provide  a  common basis for comparison  for  the  period 1970-1980 it
was necessary that each  sector  be  treated  consistently  in terms of the statis-
tical  data on production,  fuel  consumption,  etc  and using  the most up-to-date
uncontrolled emission  factors  as well as  the  abatement technology utilized by
industry for each year of  the analysis.

          Most  of the  industrial   production  and  fuel  consumption  data were
derived from  national  statistics compiled and  maintained by  Statistics  Canada
(SC) and the Department  of Energy.  Mines and Resources  (EMR).   Emission factors
were obtained primarily  from the latest U.S. EPA  AP-42  publication and emission
control information was  gleaned  from  the literature  and determined from surveys
carried out  by  the Department  of the Environment (DOE).   Average sulphur  (and
ash) contents of  coal were derived  from  EMR  surveys and for liquid fuels,  from
information supplied to  DOE by  fuel producers  as  a  regulatory  requirement.  For
the  non-ferrous  smelting  sector,  historical   S02   emission  data  provided by
individual companies was judged the most  representative  and  was used for  this
analysis.

          Transportation  emissions of  $03 and NOX were determined  in  three
ways:   vehicle  registration,  fuel  consumption  and use  statistics  such as take-
off and landing cycles  or calls  at port.   Vehicle  registrations were used to
calculate emissions  from automobiles and  trucks  (road  vehicles); the  emission
factors were developed using software based on ERA'S Mobile 2.

          Fuel  consumption  data were  used  to  calculate  the  emissions  from
railroads as  well as  off-road  diesel and gasoline powered  vehicles.    Motive
fuels  used  in  railroads were:    coal,   heavy   and  light  fuel  oil  and  diesel.
                                      237

-------
Average emission rates by  engine  type  were  used  to calculate the emissions  for
aircraft (landing and take-off cycle)  and marine  (calls  at port) sectors.   The
numbers of  calls  at port and LTD  (landing  and take-off)  cycles were obtained
from Statistics Canada.

          2.1.1  Sulphur Dioxide

          Sulphur dioxide  emissions  come primarily from  two  main source cate-
gories,  industrial  processes and  stationary  fuel  combustion.    The  trend  has
been steadily  downward,  total national  emissions  going from 6.7 million  tonnes
in  1970  to  4.6 million  tonnes  in 1980  (Figure 1).    Since  1970 S02 emissions
from non-ferrous smelters,  the largest emitting  sector,  have decreased by 44%,
this  includes  the   emissions  from  primary  copper,   nickel,  lead,   zinc   and
aluminum.   As  shown in  Figure  2  the  industrial  contribution to  total   S02
emissions  decreased from 76% in  1970  to  67% in 1980.    The  stationary fuel
combustion  contribution  to total  S02  emissions  rose   from  23%  in 1970  to  30%
in  1980, however  in absolute terms  emissions  decreased   by  11%.  Residential,
commercial    and   industrial  (non-utility)   fuel   combustion   S02   emissions
decreased 40% while utility S02  emissions increased 52%.

          The decrease in  the non-ferrous smelting  sector can be attributed  to
process improvements, increased  pyrrhotite rejection at some  operations and  the
expansion or  addition  of  acid  plants  at others.   The  decreases in  the non-
utility fuel combustion emissions  can be attributed to reduction  of the sulphur
content of fuels,  the decline in the use of coal  for industrial   and residential
use as well as a shift to cleaner fuels like natural gas and  light oil.

          The power utilities used additional  low sulphur coal,  introduced coal
blending and  coal  washing  and shifted to  alternate  electric power generation
technologies.  These measures served to limit the  increase of   sulphur dioxide
emissions to 52%,  the  total power generation  from  coal-fired plants  increased
by 83% during this time.
                                       238

-------
          2.1.2  Nitrogen Oxides

          Nitrogen  oxides   predominantly  come from  the transportation  sectors
and  stationary  fuel  combustion categories.  The 30% increase  in  national  emis-
sions  during  the period  1970-1980  (Figure 3)  generally  reflects  the  increase  in
energy  demand or fuel  consumed throughout the decade.   The  relative  amounts,  as
seen  from  Figure   4,  contributed  by  each  category   to  total   emissions  has
remained  essentially  the same.   Mitrogen  oxides  from stationary  fuel  combustion
were  largely  uncontrolled.

          In  transportation,  there  was   an   increase  in  NOx  emissions  from
light-duty  vehicles from 1970  to  1980.   The enactment  of light-duty  vehicle
regulations  in  the early seventies  had  a  moderating  effect  on  this  increase.
As  the older uncontrolled  vehicles  are removed  from the  total  fleet  the  ''per
vehicle"  emissions  decreased substantially however this trend is offset  by  the
increasing  vehicle  population.  The increase in  transportation emissions was
36%  with  the  largest percentage increases  occurring in uncontrolled  heavy  duty
vehicles  such  as   trucks,  off-road  diesel  engines,  aircraft   ar.d   marine
equipment.

          The 20%  increase  in nitrogen  oxide emissions  from  stationary  fuel
combustion was  incurred  mainly because of  a 60% increase in utility  emissions.
Despite  a  growing  population,  non-utility   fuel   combustion  emissions  were
unchanged from  1970  to 1980; this  reflects the  change  in fuel use  patterns  to
natural  gas  and  electricity  and  energy  conservation  practices.   During  the
seventies Canadian  utilities  heavily  promoted  electricity  for  industrial  and
home use while  government  grant programs  were instrumental in the rapid  expan-
sion  and  improvement  of the  gas  pipeline distribution  systems especially  in
central and eastern Canada.
                                        239

-------
3.   CONCLUSION

          National emission trends of  sulphur  dioxide  and nitrogen oxides have
been presented for the period  1970 to  1980.   The  emissions  of sulphur dioxide
have steadily  declined with  the  major decrease  occurring  in  the non-ferrous
smelting  sector.     Nitrogen   oxides   have  increased  reflecting  the  general
increase in energy demand, the contribution  from  transportation and stationary
fuel combustion having increased at an equivalent rate.

          Due to  the  limitations  inherent in a retrospective  emissions inven-
tory exercise it should be stressed that  the data  are  more suited to the study
of emission trends.   If comparisons tc other studies are  made,  a prudent basis
for comparison would be on the degree of change in the  emissions.
                                        240

-------
  National  Sulphur Dioxide Emission Trends
7000





6000





5000





4000 \





3000
    ,000 tonnes
2000H
   r




1000h

   L



  OL
      1970

                          S02
                                    j
1972
1974     1976



   Year


   Figure 1
1978
1980

-------
              DISTRIBUTION
OF S02
1970
EMISSIONS
  NON-FERROUS 54-. 9%
             3665
      FERROUS 5..&r.,
              385 \.
  FOSSIL FUEL 13.2
             885
OTHER I NDUSTR t  1 . 6X
              110
                                                     TRANSPORTATION 1.3X
                                                     85
                  NON-UTILITY 15.7%
                  1050
                                        UTILITIES 7.5X
                                        500
                              Ki I otonnes

              DISTRIBUTION  OF S02  EMISSIONS
                                1980
                                      NON-FERROUS 4-4.9%
                                      2070
       FERROUS 5.4%
               250
     FOSSIL FUEL 13.9X
                 640
        OTHER INDUSTRI 2
                                                     TRANSPORTATION 3.OX
                                                     140
                                                 NON-UTILITY 1 3.5X
                                                 625
                      130
                                   UTILITIES 16.5X
                                   760
                               f i gure 2

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National   Nitrogen  Oxides  Emission  Trends
                        N02
    ,000
1800r	
   i-
1600JJ-
1400L
1200
1000
 800
 600^-
 400 £-
    i-
 2001-
  oL
       tonnes
    1970
              1972
1974     1976
   Year
   Figure 3
1978
1980
                                                 1
                                                 H
                                                 •n
                                                 1
                                                 H
                                                 i

-------
           DISTRIBUTION  OF  NOX  EMISSIONS
                              1970
              NON-UTILITY 25.7%
LIGHT DUTY 21.1%
VEHICLES     280
                                                 UTILITIES 12.1X
                                                 160
                                                    OTHER INDUSTRY 2.
                                                    30
                                                 9.15S AIR/RAIL/MARINE
                                                 120
                                  29.8X OTHER TRANSPORTATION
                                  395
                            K1 lotonnes
                              1980
             NON-UTILITY 19.5X
                          335
LIGHT DUTY 20.7X
VEHICLES     356
                                                UTILITIES 15.1X
                                                260
OTHER  INDUSTRY 2.9!
50
                                                 10.5X AIR/RAIL/MARINE
                                                 180
                            540
                                OTHER TRANSPORTATION
                            FIGURE 4

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            UNITED KINGDOM  EMISSION  INVENTORIES
                      H. S.  Eggleston
                         G.  Mclnnes
                 Warren Spring Laboratory
                     Stevenage, Herts.
                      United Kingdom
                       Presented at:


Second Annual Acid Deposition Emission  Inventory Symposium
                Charleston, South Carolina
                   November 12-14,  1985

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                     UNITED KINGDOM EMISSION INVENTORIES
                            by:  H. S. Eggleston
                                    G. Mclnnes
                                 Warren Spring Laboratory
                                 Stevenage, Herts.
                                 United Kingdom
                                  ABSTRACT

     Warren Spring Laboratory (WSL) is an environmental/industrial research
e tablishment of the United Kingdom Department of Trade and Industry.  WSL's
Air Pollution division is a major center for research on the physical and
chemical aspects of air pollution in the United Kingdom and covers emission,
dispersion and ambient air quality.  National emission estimates for S0_,
NO , CO and VOC have been made for several years.  A new project is now  in
progress to produce spatially disaggregated emission inventories for the
United Kingdom.  Estimates of SO- have been made and work is proceeding  to
cover other pollutants, initially NO  and VOC.  The disaggregated
inventories will be based on a relational data base which, in addition to air
quality information, will contain emission information on large plants and
estimates of area emissions mainly on a 20 x 20 km grid basis using emission
information and surrogate statistics to cover smaller emission sources.
Emissions from fuel combustion as well as from industrial processes and
evaporative emissions are included using, where available, emissions factors
based on emission measurements made under United Kingdom conditions by WSL
and others.  The emissions data base will be used by WSL primarily in
numerical  dispersion modeling of urban and longer range transport, chemical
reactions and depositions, as well as assisting in the assessment and
interpretation of the data from the national United Kingdom monitoring
networks for acid deposition, smoke, S02, N0x, and ozone, coordinated by
WSL.

-------
                      UNITED  KINGDOM  EMISSION  INVENTORIES

                                 INTRODUCTION

     Warren  Spring  Laboratory  (WSL)  is  a  research establishment of the
United Kingdom  Department  of Trade and  Industry whose  interests cover
environmental and  industrial fields.  The Air Pollution division  is a major
center for research  on  the physical  and chemical aspects of air pollution in
the United Kingdom  and  covers  emission, dispersion  and ambient air quality.
Current  research topics include  the  measurement of  combustion and process
emissions from  mobile and  stationary sources, modeling of air pollution, and
the operation and coordination of monitoring  networks measuring smoke and
SO-, acid deposition, NO  , ozone, hydrocarbons and  suspended particulates
including lead.  New projects  are the construction  of  a national  automated
network  of NO   and  ozone measurement sites, the development of spatially
disaggregated emission  inventories and  the creation of a new computer system
based on a relational data base.  The data base will include information
held by  WSL  on  emissions and related statistics, measurements of  air quality
and deposition, meteorological data  and other relevant information.
     Tha different  monitoring  networks  are designed for a variety of
purposes.  The  smoke and sulphur dioxide  monitoring networks were created in
1961.  They  provide  daily  measurements  and are voluntarily operated sites
coordinated  by  WSL.   The aim was to  provide baseline information  about the
distribution and trends of smoke and S02  in the United Kingdom.   This was
reorganized  in  1982  into a number of networks with  separate aims.
Continuous monitoring of NO, N02> CO, 03  and  S02 also  is undertaken by WSL.
Sites representative of urban  and rural situations  have been monitored for
up to 10 years.  The results of  these surveys are published and summaries
are given in the DOE  Digest  of Environmental  Protection and Water
Statistics.   The continuous  monitoring network is being extended  with the
construction of a network  of fully automatic  N0x/0j monitoring stations.
There is also a national network of  sites measuring pollution concentration
                                     247

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in rain.  A network of remote rural sites collects samples of precipitation
and these are analyzed for a variety of ions.  These results plus sulphur
measurements form the United Kingdom input to the United Nations Economic
Commission for Europe's European Monitoring and Evaluation Program
investigating the long-range transport of air pollutants.

                            EMISSION INVENTORIES

National Aggregates
     For several years WSL has estimated national emissions of S0?,  NO ,  CO
                                                                 w    A
and hydrocarbons in the United Kingdom.  These estimates are mainly based on
emissions from fuel combustion, but they do include estimates of emissions
from other sources.  Originally, the emission factors used relied heavily on
American data but now most are based in measurements made under United
Kingdom conditions by WSL and others.  These estimates were published in  the
Department of the Environment Digest of Environmental Protection and Water
Statistics (Reference 1).
     Emissions of SO- since 1960 are shown in Figure 1.  The emissions were
about 6 million tonnes during the 1960s, but have not fallen by about
40 percent to 3.54 million tonnes in 1983.  This has been due to the large
reduction in low and medium level sources and has resulted in a reduction in
average urban levels of S0? of over 70 percent.  This reduction is still
continuing and the total emissions have fallen by nearly 25 percent since
1980.
     The estimates of emissions for 1983 are shown in Table 1.  These
figures show clearly the most significant sources of each pollutant.  Over
70 percent of SO. is emitted from power stations and most of the remainder
from industrial sources.  The largest sources of NO  are power stations and
road transport both emitting about 40 percent of the total.  Road vehicles
also account for nearly 84 percent of the CO and are a significant source of
non-methane hydrocarbons emitting a similar quantity to solvent evaporation
and industrial processes.
     Recent measurements, made on 72 commercial and industrial boilers in
Scotland (Walker et al., Reference 2),  with sizes between 430 and 14,200 kW,
have resulted in the adoption of new emission factors for NO , CO and VOC.
                                     248

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Comparison of the factors with  the  previously used factors is complicated
because the study used different  size  ranges for the boilers.  However, the
factors used to calculate the national emissions have been altered as shown
in Tdble 2.
     Many of the factors are only altered  slightly, but for some there are
more substantial differences.   As a result of these changes, the estimate of
emissions from commercial and industrial fuel consumption has changed.  A
comparison is shown  in Table 3  for  the year 1982.
     Until 1983, vehicle emissions  were estimated on the same basis as
emissions from stationary sources by applying an emission factor to the
total fuel consumed.  However,  as emissions from vehicles are related to the
speed of the vehicle and the manner in which it is driven as well as the
amount of fuel consumed, this method took  no account of varying patterns of
road use.  Measurements on the  road, rather than on a dynamometer, were made
by WSL of emissions  from motor  vehicles at a range of speeds so that the
variation of emission with speed  could be  determined (Potter and Savage,
Reference 3).  Emission factors for pollutant emission per kilometer driven
at each speed could  then be estimated.  The sample of cars tested was chosen
to reflect the makeup of the United Kingdom car fleet.  Road traffic
statistics give the  number of vehicle-kilometers driven on different types
of roads and the average speeds of  different categories of vehicles.
Measurements of vehicle speeds  in the United Kingdom indicate that the
distribution of vehicle speed about the mean is approximately gaussian with
a standard deviation of one-sixth of the mean.  This enables a speed
distribution for a particular type  of  road to be calculated and then using
the measured speed-related emission factors, the emissions can be estimated
(Reference 4).  Emissions estimated using  this method have the advantage
that they reflect the types of  roads and driving patterns and are sensitive
to any changes in them.  A comparison of the results obtained using the
single emission factor method and the new  speed-related method is given in
Table 4.
Data Base
     WSL has recently installed a new GEC  63/30 computer running the AT&T
UNIX System 5 operating system.   It has 8  M bytes of random access memory,
over 1 G byte of backing store  and  is accessed through an open-system  local
                                     249

-------
area network which is also connected to other computers and services.  A
relational data base management system, MISTRESS, has also been purchased
and will be usod to store the national air pollution data base.
     The data base will be central to the work of the air pollution division
of WSL.  It will store all the information relating to air pollution:
ambient air monitoring, acid deposition measurements and meteorological data,
was well as emission inventories.  The system is illustrated in Figure 2,
Data will be processed into the data base and will  be available for
comparison with other data or with model results.  The emissions data will
be collected in separate data base files along with surrogate statistics.
Only completed and validated inventories will be stored in the main data base
and be available for general interrogation and input to modeling programs.
The data base will be linked to statistical and graphical  packages as well
as report writing facilities.  The system, which should be fully operational
in the first half of 1986, will provide an integrated and comprehensive
package of retrieval, presentational and analytical  routines.
Spatially Disaggregated Inventories
     The estimation of spatially disaggregated inventories for the United
Kingdom is a new project started this year.  The inventories are to be
prepared on a 20 x 20 km grid for the whole United  Kingdom but smaller grids
will be used for some areas.
     A few local authorities have compiled local, spatially disaggregated
inventories and these are being collected by WSL.  They are mainly compiled
from questionnaires to local firms and estimates of local  fuel consumption
in various sectors.  These can be used as direct input to the national
inventories but will  also be used to help validate  the disaggregation
procedures adopted to provide information for the United Kingdom as a whole.
     The Greater London Council has compiled an inventory for London  in 1976
and is in the process of updating this.  Sheffield  and Coventry have
inventories for S02 in 1983, compiled from fuel use information.
     There is no comprehensive national program for the routine measurement
of emissions in the United Kingdom, so that there are very few actual
emission measurements available for inclusion in an emission inventory.
Emissions, therefore, must be estimated from other  information available
                                  250

-------
about individual  sources  or  by  using  surrogate statistics.  Uhere
appropriate,  emission  sources will  be stored  as point sources within the
data base, otherwise emissions  will be  aggregated on an area basis.  The
following approaches have been  adopted  by WSL for the production of the
spatially-disaggregated  inventories for the United Kingdom.
     Power Stations:   most of these are publicly owned and information is
available on  type,  age,  power output  and efficiency of individual stations.
Pollutant emission  factors can,  therefore, be applied to the appropriate
statistic, fuel  consumption  or  power  output,  in order to estimate emissions
from each station.  To date, it has been assumed that 10 percent of the
sulphur  in coal  is  retained  in  the  ash  at each station; recent evidence
suggests that this  may be a  high estimate of  retention and investigations
are under way to determine a more realistic figure.
     Other industrial  sources:   directly relevant information on these are
not so readily available.  Contact  is being established with the relevant
industry associations  with a view to  obtaining more information on
individual large plant on a  voluntary basis and questionnaires are being
used to obtain such information in  a  consistent and readily usable form.  To
date, emissions  from large emission source categories, where available, have
been estimated from emission factors  and national throughput disaggregated
in proportion  to plant capacity to  provide estimates of point source
emissions.
     Emissions fron other stationary  sources  including smaller industrial
source categories, commerce, and housing will be treated as area sources.
These emissions  will be estimated from  spatially disaggregated statistics on
fuel deliveries  or from nationally  aggregated statistics, for example
production, output or  national  fuel consumption and then disaggregated using
an appropriate surrogate  statistic  (e.g., population or employment).
     A statistical data base, called  PINGAR,  is available for petroleum
deliveries into  10 km  squares for the whole United Kingdom with densely
populated areas  covered at a 1  km resolution.  These statistics cover
different fuels  and users  and provide a basis for estimation of emissions
from all  stationary petroleum consumption.  While this will not directly
provide data on  individual point sourcas, it will locate accurately
                                    251

-------
consumption within the corract grid square.  Other surrogate statistics are
not usually available on a grid basis; an exception is census data for
Scotland.  Other statistics which can be used are population and household
density from census returns, land use, employment and agriculture.  These
are provided for various areas (e.g., counties) and have to be transposed to
a grid before they can be used.  Spatially disaggregated domestic emissions
will be estimated from regional coal consumption and population.
     Motor vehicles contribute over 40 percent of the NO  and VOC emissions
                                                        /\
so considerable effort is necessary to account adequately for these sources.
In London, vehicle counts have been made so that total vehicle kilometers
are available for each borough for motorways and other roads and for peak
and off-peak hours together with average speeds, so it is possible to use
the speed-related emission factors to estimate emissions in each borough.
Outside London, there is less information available on traffic on a
spatially resolved basis, but the Department of Transportation does produce
statistics on vehicle kilometers for each county in the United Kingdom.
Another source of information is the 1981 Census which provides statistics
on the distribution of cars in the country.  This will be used to
disaggregate the county estimates.
     The emission inventory data base will contain details of individual
point sources   source category, location, height, number and size of
stacks, thermal input, abatement details (if present), fuel consumption and
type, period covered by the information, etc., as well as emission
estimates.  It will, therefore, be possible to interrogate the data base
using a number of search criteria.  For example, emission estimates could be
computer-mapped to show the spatial distribution or used as input to a
predictive model.  It will  also be possible to use the system to convert the
emission estimates from one spatial-grid system to another.
Sulphur Dioxide
     Using the above mentioned approaches, an emission inventory for SO, on
a 20 x 20 km grid, based on the United Kingdom's Ordinance Survey grid, has
been produced for 1983 and is shown in a graphical form in Figure 3.
                                    252

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Nitrogen Oxides
     The production of a disaggregated inventory for NO  involved a similar
approach to that for S02 with the major difference being that more effort
was required to account for emissions from vehicle sources as motor vehicles
contribute dbout 40 percent of the emissions.  The accuracy of the
disaggregated  inventory will be dependent on the method used to distribute
these emissions across the grid cells.  Using the method described aoove, a
first estimate has been made and this could be further refined with the use
of more appropriate traffic statistics.
Other Inventories
     The most  important of these will be the hydrocarbon inventory.  The two
main sources are vehicles, which are dealt with as above, and evaporative
and process emissions.  The latter will be difficult to quantify accurately
in a spatially disaggregated inventory due to both the lack of individual
plant or area  production/consumption data and reliable emission factors for
individual hydrocarbons.  For the foreseeable future, surrogate statistics
(e.g., industrial floorspace or employment in particular industrial sectors)
and bulk hydrocarbon emission factors will continue to be used.
     Active consideration is being given to other pollutants such as NH,.
This will require further study to determine the major sources and the best
statistics that are available to describe them.
     Another long-term aim is to provide temporal disaggregation of
emissions.  Relevant information is being collected, but such refinements
will take second priority to the annual inventories.

                                 CONCLUSIONS

     Spatially disaggregated emission inventories are being produced for a
variety of atmospheric pollutants.  In the United Kingdom, surrogate
statistics have to be used to overcome the scarcity of emission
measurements.   Future work will involve the establishment of inventories of
other pollutants and the estimation of temporally disaggregated inventories,
as well  as the refinement of existing inventories.
                                      253

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     This work will be integrated via the new data base system with
monitoring and modeling of air pollution in the United Kingdom and Europe to
improve our understanding of the dispersion and deposition of atmospheric
pollutants.
                                     254

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                                 REFERENCES
1.   Digest of Environmental Protection and Water Statistics No. 7 (1984),
     HMSO, London, United Kingdom.

2.   Walker, D.S., Galbraith, R., and Galbraith, J.M., Warren Spring
     Laboratory, Report LR 524  (1985), Survey of Nitrogen Oxides, Carbon
     Monoxide and Hydrocarbon Emissions from Industrial and Commercial
     Boilers in Scotland.

3.   Potter, C.J., Savage C.A., Warren Spring Laboratory, Report LR 470
     (1983). A Survey of Gaseous Pollutant Emissions from Tuned In-Service
     Gasoline Engined Cars over a Range of Road Operating Conditions:
     Executive Summary.

4.   Rodgers, F.S.M., Warren Spring Laboratory, Report LR 508 (1984), A
     Revised Calculation of Gaseous Emissions from United Kingdom Motor
     Vehicles.
                                        255

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    TABLE 1.  NATIONAL EMISSIONS OF AIR POLLUTANTS 1983 (MILLION TONNES)
SO,,
Mt %
By Fuel:
Coal
Solid Smokeless
Motor Spirit
DERV
Burning Oil
Gas Oil
Fuel Oil
Refinery Fuel
All Gas
Bv Consumer:
Domestic
Commercial/Public Service
Power Stations
Refineries
Agriculture
Other Industry
Rail Transport
Road Transport
Incineration
Process and Evaporation
TOTAL

2.
0.
0.
0.
-
0.
0.
0.
-

0.
0.
2.
0.
-
0.
-
0.
-
-
3.

81
10
02
03
-
05
53
16
-

19
14
53
16
-
52
-
04
-
-
72

76
3
--
1
--
2
14
4
--

5
4
68
4
--
17
--
1
--
--


0
0
0
0

0
NO
Kt

.80
.04
.52
.19
--
.06
0.09
0
0

0
0
0
0

0
0
0
0

1
.03
.08

.05
.04
.76
.03
--
.18
.04
.70
.01
--
.85
A
%

43
2
28
10
--
3
5
2
4

3
2
41
2
--
10
2
38
1
--



0
0
3
0

0
0

0

0
0
0


0
0
4
0

5
CO
Mt %

.37 7
.20 4
.99 79
.25 5
.-
.02 --
.01 --
.-
.01 --

.46 9
.01
.05 1
--
-.
.07 1
.01
.23 83
.22 4
--
.08
VOC
Mt

0.08
--
0.49
0.04
--
0.01
--
--
--

0.07
--
0.01
--
--
--
0.01
0.53
0.04
0.60
1.27
%

6
--
39
3
--
1
--
--
--

6
--
1
--

--
1
42
3
47

Note:  The figures are mainly based on fuel  related emission factors and will
underestimate the emissions from industrial  processes of all but VOCs.  This
will only be a few percent of the total  emissions.  The total for hydrocarbons
excludes leakage from the distribution system.  This is mainly methane and
amounted to about 2.2 million tonnes in  1983.
                                     256

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             TABLE 2.  COMPARISON OF "OLD" AND "NEW" COMMERCIAL
                       AND INDUSTRIAL EMISSION FACTORS
                                                       Emission Factor
                                                  (g/kg or Gas kq/Mtherm)

N0v
X


CO



voc



Fuel
Coal
Solid Smokeless
Gas Oilc
Fuel Oil
Natural Gas
Coal
Solid Smokeless
Gas Oilc
Fuel Oil
Natural Gas
Coal
Sol id Smokeless
Gas Oil
Fuel Oil
Natural Gas
"Old"a
7.79
7.79
2.6
7.5
5280
6.64
6.64
0.24
0.5
247.5
0.115
0.115
0.07
0.06
165.0
"New"5
4.8
4.8
2.6
7.4
5340
4.1
4.1
0.24
0.50
250.0
0.07
0.07
0.07
0.06
153.0
aThe "old" factors are based on U.S. ERA factors, but they have been updated
 to take into account previous measurements in the United Kingdom.
bThe "new" factors result from a series of measurements made on United
 Kingdom boilers (Reference 2).
GThe factor for Gas Oil has not been updated as too few measurements were
 made to provide an accurate figure, however, the measurements agreed with
 the "old" value rather than with the U.S. EPA factor.

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  TABLE 3.   EMISSIONS FROM COMMERCIAL AND INDUSTRIAL FUEL CONSUMPTION 1983
                                                 Emission (k tonnes)
                                       01da                          Newb
NOV                                 221 (13%)c                   187 (11%)
  A
CO                                   82 (1.6%)                    54 (1.1%)
VOC (non-methane)                     4 (0.3%)                     3.2 (0.2%)

a01d refers to the U.S.  EPA based (but modified by United Kingdom measure-
 ments) factor.
 New refers to the factor based on measurements made in the United Kingdom.
GThe numbers in brackets are percentages of the national total  emission.
                 TABLE 4.   EMISSIONS FROM MOTOR CARS (1983)

N0x
CO
VOC
Single
Emission Factor
508
8107
538
Speed
Related Factors
725
4502
538
a(k tonnes).
                                     258

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                                     level emmert
                                Medum level emmei
                                Low l«v«l emitters
Power stations

R« Trie net

Otfief nduslry

Oiher non domestic

Domesoc
                                                                                               CONCENTRATION
                                                                                                    WOEX
                                                                                           1981/82-100
                                                                                                   r- 320
                                                                                                    -120
                                                           1974
                                                                   1976
                                                                          1978    1980    1982
                                                                                                1984
    Emmioni from fuel combuitton  only.  E*dud«  emunoni Ifom   Source.  Wtmn Spring Ltttorttory, D*p*rrm»or of Tr#Jt *nd Industry
    chemicel «r»t»b(f throughouT th* 196Oi ind eerly  I970l »t  about 6   I oni hgv* fallen by over 70 p«r cent irnc« 1962. m line wrth the reduc-
million tonne*  • y*»'  After 1973  however, ennuel emunoni fell to   tion in emmioni from low-level wurcet (tee T§b»* 2 4 end Addmonel
•bout S mrllion tonnet in 1976. 1977 »nd  1978, to 4 0 milhon tonnri   Tablet A1 and A3).
   Figure  1.   Sulphur  dioxide  emissions  froiji  fuel  combustion  and
                    average  urban  concentrations.

-------
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•i 1 : ; ; '
i : i i :" ;;
: : i i n :? i
1 ' ' J J 1 'j 1 1


i 7 16 i ) i : J i i
:o 7 jj ;? >!;r«). j : .' : n ;<)

< 1 .' < 5 5 i 12 11 76 11 5 1 1 1 1 I
: i t ; • 6 i, ;i :2 27 u 10 > t ; j<
J o 7 7 7 6 » ; || [| II 10 9 9 I
19 II M 5 J fJJ] J 5 90167 »J 6? :/ 0
ii i' :: i t ' /: :i n <;in::;:?o:=< : t
; -• ;; t > / • i: 15 n i i i « j
) J ( J J 5 ' 7 M 10 ? 7 , j J
r "" * i1'!}'111? 3 '^J1 7 ? '
i : : : :: > i :
i

                                                 Figure 2.



                                                 UK Emissions of SC^



                                                 20 x 20 km grid



                                                 Scale: 1=346.5 tonnes
     •i i

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APPENDIX




ATTENDEES

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                  SECOND ANNUAL ACID DEPOSITION SYMPOSIUM

                             LIST OF ATTENDEES
1.   Linda Allison
    ORNL/AODNET
    Oak Ridge National Laboratory
    Post Office Box X, Building 1505
    Oak Ridge,  TN  37831
    (615) 576-5454

2.   Wil1iam Bain
    Tennessee Valley Authority
    445 Chestnut Street, Tower 2
    Chattanooga, TN  37401
    (615) 751-0011

3.   David Beecy
    U.S. OOE/Office of Fossil Energy, FE-13
    Washington, DC  20545
    (301) 353-2617

4.   Carmen Benkovitz
    Brookhaven National Laboratory
    Building 51
    Upton, NY  11973
    (516) 282-4135

5.   Chris Bergesen
    Utility Data Institute
    2011 I Street, S.W., #700
    Washington, DC  20006
    (202) 466-3660

6.   John Bosch
    Office of Air Quality Planning and Standards
    U.S. EPA (MD-14)
    Research Triangle Park, NC  27711
    (919) 541-5582

7.   Art Braswell
    South Carolina Department of Health
     and Environmental Control
    2600 Bull  Street
    Columbia,  SC  29201
    (803) 758-5406

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 8.  Lyle Chinkin
     Systems Applications, Inc.
     101 Lucas Valley Road
     San Rafael,  CA  94903
     (415) 472-4011

 9.  Christian Cleutinx
     Commission of the European Communities
     2100 M Street, N.W.
     Washington,  DC  20037
     (202) 862-9570

10.  David Davies
     Environment  Canada
     West Isle Office Towers
     2121 Trans Canada Highway
     Dorval, Quebec,  Canada  H9P 1J3
     (514) 636-3026

11.  Jim Democker
     Office of Air and Radiation
     U.S. EPA
     401 M Street, S.W.
     Washington,  DC  20460
     (202) 382-5580

12.  Alan Dresser
     Colorado Air Pollution Control  Division
     4210 East llth Aven'ie
     Denver, CO  80220
     (303) 331-8524

13.  Simon Eggleston
     Warren Spring Laboratory
     Department Trade and Energy   U.K.
     Gunnels Wood Road
     Stevenage, Hertsfordshire  SG123Y
     Phone:  Stevenage 71887

14.  J.M. Ekmann
     U.S. DOE/Pittsburgh Energy Technology Center
     Post Office  Box 10940
     Pittsburgh,  PA  15236

15.  Todd Ellsworth
     State of Maryland
     Air Management Administration
     201 West Preston Street
     Baltimore, MO  21201
     (301) 383-3245
                                   263

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16.  Fred Fehsenfeld
     NOAA/ERL Aeronomy Laboratory
     Mail Code R/E/AL6
     325 Broadway
     Boulder, CO  80303
     (303) 497-5819

17.  Elizabeth Field
     Florida Department of
      Environmental Regulation
     2600 Blairstone Road
     Tallahassee, FL  32301
     (904) 487-1855

18.  Bob Friedman
     Office of Technology Assessment
     U.S. Congress
     Washington, DC  20510
     (202) 224-8713

19.  Douglas Fulle
     EBASCO Services, Inc.
     145 Technology Park
     Norcross, GA  30092
     (404) 449-5800

20.  William Gill
     Texas Air Control Board
     6330 Highway 290E
     Austin, TX  28723
     (512) 451-5711

21.  Dale Gillette
     NOAA R/E/AR4
     325 Broadway
     Boulder, CO  80303
     (303) 494-3842

22.  Paul Goldan
     NOAA/ERL
     325 South Broadway
     Boulder, CO  80303
     (303) 497-3814

23.  Gerhardt Gschwandtner
     Pacific Environmental Services
     1905 Chapel Hill Road
     Durham, NC  27707
     (919) 493-3536
                                    264

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24.  Steven Heisler
     ERT
     975 Business Center Circle
     Newbury  Park, CA  91320
     (805) 499-1922

25.  Merrill  Heit
     U.S. DOE
     Environmental Measurements Laboratory
     376 Hudson  Street
     New York, NY  10014
     (212) 620-3625

26.  George Hendrey
     Brookhaven  National Laboratory
     Terrestrial and Aquatic Ecology Division
     Building 318
     Upton, NY   11973
     (516) 282-3262

27.  Edward Hi!Isman
     Oak Ridge National Laboratory
     Post Office Box X, Building 4500N
     Oak Ridge,  TN  37831
     (615) 574-5938

28.  Andy Hoffer
     Ontario Hydro
     700 University Avenue (H10D 2)
     Toronto, Ontario, Canada  M5G 1X6
     (416) 423-7508

29.  James Homolya
     Radian Corporation
     Post Office Box 13000
     Research Triangle Park, NC  27709
     (919) 481-0212

30.  Allen Hughes
     The Mitre Corporation
     1820 Dolley Madison Blvd.
     McLean,  VA  22102
     (703) 883-6064

31.  Quang-Tuyen Huynh
     J.W. Environmental Data, Inc.
     60 Cowan Avenue, Suite 1505
     Toronto, Ontario, Canada  M4K 3X9
     (416) 248-3245

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32.  Marty Irwin
     Hoosiers for Economic Development
     11 South Meridian, Suite 1005
     Indianapolis, IN  46204
     (317) 632-3952

33.  Kurt Jakobson
     Office of Research and Development
     U.S. EPA
     Washington, DC  20460
     (202) 382-2583

34.  David Johnson
     Office of Air Quality Planning and Standards
     U.S. EPA (MD-15)
     Research Triangle Park, NC  27711
     (919) 541-5516

35.  Terry Juchnowski
     New Jersey Department of
      Environmental Protection
     CN 027
     Trenton, NJ  08625
     (609) 292-6704

36.  James Kelley
     U.S. DOE
     Office of Environmental Analysis
     Forrestal Building,  Room 4G-036
     1000 Independence Avenue, S.W.
     Washington, DC  20585
     (202) 252-8420

37.  Ismail A. Khatri
     Indiana State Board of Health
     1330 West Michigan Street
     Indianapolis, IN  46206
     (317) 633-8591

38.  Stephen Kiel
     State of Maryland
     Air Management Administration
     201 West Preston Street
     Baltimore, MD  21201
     (301) 383-3245

39.  Duane Knudson
     Argonne National Laboratory
     9700 South Cass Avenue
     Argonne, IL  60439
     (312) 972-5102
                                     266

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40.  Harry Lins
     U.S. Geological Survey
     410 National Center
     Reston, VA  22092
     (703) 860-6927

41.  Robert Lott
     Tennessee Valley Authority
     417 Multipurpose Building
     Muscle Shoals, AL  35660
     (205) 386-2033

42.  Gerald Lowry
     SAIC
     1710 Goodridge Drive
     McLean, VA  22102
     (703) 821-4555

43.  Thomas Lukow
     U.S. DOE
     Morgantown Energy Technology Center
     Post Office Box 880
     Collins Ferry Road
     Morgantown, WV  26507
     (304) 291-4622

44.  Terry McGuire
     California Air Resources Board
     Post Office Box 2815
     Sacramento, CA  95821
     (916) 322-2990

45.  Charles 0. Mann
     Office of Air Quality Planning and Standards
     U.S. EPA (MD-14)
     Research Triangle Park, NC  27711
     (919) 541-5694

46.  Mike Maxwell
     Air and Energy Engineering Research Laborator
     U.S. EPA (MD-61)
     Research Triangle Park, NC  27711
     (919) 541-3091

47.  Deborah Metrin
     Florida Department of
      Environmental Regulation
     2600 Blairstone Road
     Tallahassee, FL  32301
     (904) 488-0870

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48.  David Mobley
     Air and Energy Engineering Research Laboratory
     U.S. EPA (MD-61)
     Research Triangle Park, NC  27711
     (919) 541-2612

49.  Frank Noonan
     Office of Air Quality Planning and Standards
     U.S. EPA (MD-14)
     Research Triangle Park, NC  27711
     (919) 541-5585

50.  Joan Novak
     Atmospheric Sciences Research Laboratory
     U.S. EPA (MD-80)
     Research Triangle Park, NC  27711
     (91S) 541-4545

51.  William Oliver
     Radian Corporation
     10395 Old Placerville Road
     Sacramento, CA  95827
     (916) 362-5332

52.  Dale Pan!
     Air and Energv Engineering Research Laboratory
     U.S. EPA (MD-"l)
     Research Triangle Park, NC  27711
     (919) 541-5578

53.  Diana Parker
     Kentucky Department of
      Environmental Protection
     18 Reilly Road
     Fort Boone Plaza
     Frankfort, KY  40601
     (502) 564-3382

54.  Stephen Pearl
     Public Service Indiana
     1000 East Main Street
     Plainfield, IN  46168
     (317) 838-1758

55.  Edward Pechan
     E.H. Pechan and Associates
     5537 Hempstead Way
     Springfield, VA  22151
     (703) 642-1120
                                    268

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56.  David Powell
     Battelle Pacific Northwest Laboratory
     2400 Stephens
     Richland, WA  99352
     (509) 375-3888

57.  Brian Price
     The Mitre Corporation
     1820 Dolley Madison Blvd.
     McLean, VA  22102
     (703) 883-6064

58.  James Reagan
     Atmospheric Sciences Research Laboratory
     U.S. EPA (MD-20)
     Research Triangle Park, NC  27711
     (919) 541-4480

59.  David Roberts
     Washington Department of Ecology
     PV-11
     Olympia, WA  98504
     (206) 459-6000

60.  Trevor  Scholtz
     MEP Company
     7050 Woodbine Avenue, Suite 100
     Markham, Ontario, Canada  L3R 4G8
     (416) 477-0870

61.  Paul Schengels
     Office  of Air and Radiation
     U.S. EPA (AR-445)
     Washington, DC  20460
     (202) 475-8468

62.  Frederick M. Sellars
     GCA/Technology Division
     213 Burlington Road
     Bedford, MA  01730
     (617) 275-5444

63.  Butch Smith
     Midwest Research Institute
     5405 Creedmoor Road
     Raleigh, NC  27612
     (919) 781-5750

64.  Lowell  Smith
     Office of Research and Development
     U.S. EPA (RD-676)
     Washington,  DC  20460
     (202) 382-5717
                                    269

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65.  Douglas Toothman
     Engineering Science
     10521 Rosehaven Street
     Fairfax, VA  22030
     (703) 591-7575

66.  E.C. Trexler
     Office of Fossil Energy
     U.S. DOE (FE-13)
     Washington, DC  20545
     (301) 353-2683

67.  C. Veldt
     Division of Technology, Society TNO
     Post Office Box 342
     7300 AH Apeldoorn
     The Netherlands
     055-773344

68.  Frank Vena
     Environment Canada
     14 Floor, Place Vincent Massey
     Ottowa, Ontario, Canada  K1A 1C8
     (819) 994-3127

69.  Ron Whitfield
     Argonne National Laboratory
     9700 South Cass Avenue
     Argonne, IL  60439
     (312) 972-8430

70.  Joan Willey
     University of North Carolina at Wilmington
     Chemistry Department
     601 South College Road
     Wilmington, NC  28403
     (919) 395-3459

71.  Simon Wong
     Ontario Ministry of Environment
     Air Resources Branch
     125 Resources Road, East Wing
     Rexdale, Ontario, Canada  T6B 2X3
     (416) 248-3245

72.  Daniel Woo
     Environment Canada
     4999 98th Avenue
     Edmonton, Alberta, Canada  T6B 2X3
     (403) 468-8031

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