vvEPA
United States
Environmental Protection
Agency
Environmental Sciences Research EPA-600/4-78-028
Laboratory June 1978
Research Triangle Park NC 27711
Research and Development
Regional Air
Pollution Study
Point and Area Source
Organic Emission
Inventory
-------
RESEARCH REPORTING SERIES
Research reports of the Office of Research and Development, U.S Environmental
Protection Agency, have been grouped into nine series. These nine broad cate-
gories were established to facilitate further development and application of en-
vironmental technology. Elimination of traditional grouping was consciously
planned to foster technology transfer and a maximum interface in related fields.
The nine series are:
1. Environmental Health Effects Research
2. Environmental Protection Technology
3. Ecological Research
4. Environmental Monitoring
5. Socioeconomic Environmental Studies
6. Scientific and Technical Assessment Reports (STAR)
7. Interagency Energy-Environment Research and Development
8. "Special" Reports
9. Miscellaneous Reports
This report has been assigned to the ENVIRONMENTAL MONITORING series.
This series describes research conducted to develop new or improved methods
and instrumentation for the identification and quantification of environmental
pollutants at the lowest conceivably significant concentrations It also includes
studies to determine the ambient concentrations of pollutants in the environment
and/or the variance of pollutants as a function of time or meteorological factors.
This document is available to the public through the National Technical Informa-
tion Service, Springfield, Virginia 22161.
-------
EPA-600/4-78-028
June 1978
REGIONAL AIR POLLUTION STUDY
Point and Area Source Organic Emission Inventory
by
R. W. Griscorn
Rockwell International
Air Monitoring Center
11640 Administration Drive
Creve Coeur, MO 63141
Contract No. 68-02-2093
Task Order 1081
Project Officer
Charles C. Masser
Office of Air Quality Planning and Standards
Office of Air and Water Management
U.S. Environmental Proteclion Agency
Research Triangle Park, N.C. 27711
ENVIRONMENTAL SCIENCES RESEARCH LABORATORY
OFFICE OF RESEARCH AND DEVELOPMENT
U.S. ENVIRONMENTAL PROTECTION AGENCY
RESEARCH TRIANGLE PARK, N.C. 27711
-------
DISCLAIMER
This report has been reviewed by the Environmental Sciences Research
Laboratory, U.S. Environmental Protection Agency, and approved for pub-
lication. Approval does not signify that the contents necessarily re-
flect the views and policies of the U.S. Environmental Protection Agency,
nor does mention of trade names or commercial products constitute
endorsement or recommendation for use.
-------
ABSTRACT
An inventory of organic emissions from stationary and mobile sources
has been assembled for the St. Louis Air Quality Control Region. The inven-
tory covers point and area sources for process, combustion and evaporative
emissions.
A breakdown into five categories has been assigned to each source type.
The categories are (1) paraffins, (2) olefins, (3) aromatics, (4) aldehydes,
and (5) non-reactives. The breakdown was made part of the RAPS Emission
Inventory System, which is stored on the EPA's Univac computer at Research
Triangle Park, N.C.
-------
CONTENTS
Abstract iii
Tables vi
1.0 Introduction 1
2.0 Total Hydrocarbon Inventory 2
2.1 Point sources 3
2.2 Area sources 7
3.0 Hydrocarbon Classification ' 9
3.1 Point source inventory 10
3.1.1 Fuel combustion 10
3.1.2 Industrial processes 12
3.2 Area sources 16
4.0 Summary 22
References 24
Appendix
A. RAPS Hydrocarbon Classification for Types of Sources 26
-------
TABLES
Number Page
1 Total Hydrocarbon Emission Inventory 3
2 Sample of the National Emissions Data System (NEDS)
Source Classification Code (SCC) Report 5
3 Sample of Emission Factors 6
4 Hydrocarbon Breakdown—Point Sources 11
5 Coke Oven Gas Analysis 13
6 DuPont Gasoline Analysis 14
7 Average Composition of Gasolines 14
8 Hydrocarbon Breakdown—Area Sources 17
9 Airport Hydrocarbon Emissions 16
10 Composition of Surface Coating Solvents 19
11 Dry Cleaning Hydrocarbon Emissions 20
12 Summary of Total Organic Emissions Inventory by Class 23
VI
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1.0 INTRODUCTION
The Regional Air Pollution Study (RAPS) has as its first goal the
validation of atmospheric dispersion models. Emissions data, generally
supplied in the form of an emission inventory, are a major constituent of
a dispersion model. The RAPS Point and Area Source Hydrocarbon Inventory
was designed to provide emission data for the evaluations of photochemical
reaction models. Since orgam'cs participate in photochemical reactions
leading to "smog", the inventory includes all available organic emission
data. As the reactivity of organics varies widely, it is important to
determine not only the amount emitted, but also the composition.
Chemical kinetic mechanisms present in air quality simulation models
require some form of hydrocarbon classification in order to treat the reac-
tion processes and rates associated with their structural make-up. One such
classification scheme required in using a lumped chemical kinetic reaction
mechanism approach distributes hydrocarbons in the atmosphere structurally
into paraffin, olefin, aromatic, aldehyde, and non-reactive classes. This
report describes how this classification has been determined for hydrocarbon
emissions in the St. Louis AQCR and provides sufficient reference data to
derive alternative schemes as required.
-------
2.0 TOTAL HYDROCARBON INVENTORY
The basic RAPS Hydrocarbon Inventory is composed of several separate
inventories which have been described in various reports.
The hydrocarbon inventory for stationary point sources was developed by
Rockwell under Contract No. 68-02-2093, T0108F, and provides an up-to-date
listing of hydrocarbon emissions from stationary point sources in the
St. Louis AQCR, with a breakdown into methane and non-methane hydrocarbons.
The inventory includes all industrial hydrocarbon emission sources which emit
more than one ton per year of hydrocarbons. Point sources in the St. Louis
Air Quality Control Region (AQCR-70) emit approximately 47,600 tons per year,
or 22.6 percent of the hydrocarbon emissions in the AQCR. The report also
describes an analytical technique, based on gas chromatography, which is
suitable for analysis of hydrocarbons in the concentration range of 1 to 106
ppm and is linear with respect to both carbon number and hydrocarbon
concentration.
Area source evaporative hydrocarbon emissions from dry cleaning plants,
surface coating, and gasoline marketing are included in the "Residential
and Commercial Area Sources Emission Inventory" (EPA 450/2-75-078), which
provides information on hydrocarbon emissions on a grid square basis.
Spatial allocations were based on population and land use densities.
Temporal apportioning was based on an 8 AM to 5 PM workday or the diurnal
traffic cycle in St. Louis.
Hydrocarbon emissions from small industrial sources are included in the
report on "Stationary Industrial Area Sources" (EPA No. 68-02-2093, T0108D).
This category contributes only about 110 tons annually, or about 0.05 per-
cent of the total hydrocarbon emissions.
Emissions from mobile sources are the subject of several inventories:
The Highway Vehicle Emission Inventory described in EPA 450/3-76-035 and
-------
EPA 450/3-77-019 defines emissions from motor vehicles on a grid square or
line basis. Emissions from river vessels are described in "River Towboat
Air Pollution in St. Louis" (DOT-TSC-OST-75-42). The "Airport Emission
Inventory" (EPA 450/3-75-048) deals with emissions from aircraft. A report
on rail operations (EPA 450/3-77-025) describes the methodology and resultant
inventory. Emissions from off-highway sources are described in "Off-Highway
Mobile Source Emission Inventory" (EPA Contract No. 68-02-2093, T0108E).
A summary of hydrocarbon emissions is shown in Table 1.
TABLE 1. TOTAL HYDROCARBON EMISSION INVENTORY
SOURCE CATEGORY ANNUAL EMISSIONS. TONS
Point Sources
Fuel Combustion 2,717
Chemical Manufacturing 6,702
Primary Metals - Coke Ovens 2,339
Refinery Operations 7,161
Surface Coatings 21,072
Petroleum Storage and Marketing 7,457
Solid Waste Disposal 136
Miscellaneous 24
TOTAL 47,610
Area Sources
Industrial Area Sources
Residential and Commercial
Vehicles, Line Sources
Vehicles, Area Sources
Railroads
River Vessels
Airports
Off -Highway Mobile
Gasoline Marketing
Dry Cleaning
Surface Coating
TOTAL
TOTAL, ALL SOURCES
no
22,610
100,440
12,565
4,220
940
1,460
16,280
13,650
645
3,757
176,677
224,287
2.1 POINT SOURCES
Point sources are those individually identified industrial sources which
-------
release emissions through a stack, such as a boiler, or a vent, as in the
case of a petroleum storage tank. (Exceptions to this are leaks in refin-
eries from valves, seals, flanges, etc., which are included as point sources
under the appropriate SCC numbers.) Point sources in the St. Louis Air
Quality Control Region (AQCR) emit approximately 47,600 tons per year total
hydrocarbons, or 22.6 percent of the hydrocarbon emissions in the AQCR. The
lower cut-off used to define point sources is one ton per year hydrocarbons.
The point source inventory is comprised of data for individual sources
in the AQCR for which emissions have been obtained in the course of the RAPS
study. Each source is classified by its identification code, called the
Source Classification Code (SCC). The SCC is an identification system devel-
oped for the National Emissions Data System (NEDS), upon which the point
source hierarchy is structured. The SCC system is being used for the RAPS
point source data handling system. All data are stored and retrieved by use
of the SCC. A process which emits one or more of the criteria air pollu-
tants can be represented by one or several SCC numbers. Table 2 shows a
typical sample of SCC numbers. The SCC numbers consist of four groupings.
For example, in SCC 4-03-001-02:
Group I - a single digit (4) - designates "Point Source, Evaporative"
Group II - two digits (03) - designates "Petroleum Storage"
Group III - three digits (001) - designates "Fixed Roof"
Group IV - two digits (02) - designates "Breathing-Crude"
In addition, the base unit upon which the emission factors are based is
given; in this case, "100C gallons storage capacity".
The starting point of an emission inventory is data collection.
Inventory data such as process, consumption or storage data are gathered.
Modeling information is also collected in the form of location and stack
parameters. From the inventory data, the appropriate emission factors are
obtained and stored in the aata file. These factors are based upon the best
available information, generally gathered from source tests. The inventory
data gathered and emission factors are applied to generate emission figures
for total hydrocarbons, as well as other criteria pollutants. Table 3 shows
a typical sample of emission factors and the associated SCC numbers.
-------
TABLE 2. SAMPLE OF THE NATIONAL EMISSIONS DATA SYSTEM (NEDS)
SOURCE CLASSIFICATION CODE (SCC) REPORT
I
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
3
•
4
4
4
4
4
4
4
4
4
4
4
4
SCC
• *«
II
90
90
90
90
90
90
9V
90
9V
90
90
90
90
90
90
90
90
90
9U
90
90
90
on
TO
90
90
90
90
90
90
90
9V
90
90
90
90
90
99
01
01
01
01
01
04
02
04
04
02
02
03
OJ
10
III
001
002
002
002
002
002
00*
004
00*
004
00*
004
004
004
OOb
OOb
OOb
OOS
oos
oos
oos
oos
OOb
OOb
OOb
OOb
OOb
OOb
OOb
OOb
oor
000
oov
999
999
994
994
001
001
004
004
999
001
003
00*
009
OOb
999
001
0.01
SCC CATCGOHY NAMES
IV
99
01
Ob
07
OH
99
01
02
03
04
US
Ob
07
99
111
02
U3
0*
US
Ob
07
V9
0 1
02
03
04
OS
Ob
07
99
99
99
9V
97
90
99
4v
01
02
01
1
INDUSTRIAL
INDUSTRIAL
INDUSTRIAL
INDUSTRIAL
INdL'bTWlAL
INDUSTRIAL
INOUSTWI «L
INDUSTRIAL
iNflUSTPIAL
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INOUbTHl AL
INDUSTRIAL
INUUSTHIAL
INDUSTRIAL
iNOUSTilUL
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INC.U'., TRIAL
INtlUSlRI AL
IMiUblKl AL
iNUlibTRlAL
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INDUSTRIAL
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INDUSTRIAL
INUUSTOI AL
INDUSTRIAL
INDUSTRIAL
INDUSTRIAL
INDUSTRIAL
INOUSTRI AL
INDUSTRIAL
INDUSTRIAL
INDUSTRIAL
11
PROCESIINPWOCESS
pROCES 1 iNPHOCtSS
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(KAOLIN KILN llOOC OALLONj
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I6RICK KILN/OR* (1000 GALLONS
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(METAL MELTING 1000 GALLONS
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IMETAL MELTING MILLION CUBIC
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PHOCEbl iNPMOCtbS
HMOCESIOlHLM/MOT
POINT SC lVA-> (CLEANING
POINT SL EVAP (CLEANING
POINT SC t
ViP (CLEANING
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94 POINT SC EVAP ICLUNlMb
01
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'(((SPECIFY IN RlMAAKITCNb COATING
IBREAThl«tG-PMOUuCT 1 1000 GALLONS
IHMEATHINO CMUIJE 11000 GALLONS
CLEANCO
CLEANED
USED
LSEO
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S10HA6E
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CAPACITY
CAPACITY
-------
TABLE 3. SAMPLE OF EMISSION FACTORS
sc r»*i> -sum A« CQATUK, (CONTINUED)
»A»NISM/SHtllAC
4-02-001-01 GENCRAl
IACUM
4-02-OCK-OI 0(Nf"»L
1N«MCI
4-02-001-01 GENERAL
FOUNDS EHITTCO PER UNIT
PMT SOU HOI NC
I.POO.
CO UNITS
TONS COATING
TONS CM TINT,
0. TONS COMING
4-02-OOG-01 GENERAL
co OKtAlH-jiT fdIL
4-OJ-OJl-O'l UHlMH-HftUl'itNl
4-03-OUl-OI DPEATH-OISI K'CL
4-01-001-09 BnlAlK-erNiCNE
N-C1-OOI-9-* e»f ATM-OCLOxU
4-C1-001-10 6«^ATM-(.ir IU»INT
4-01-UOl-ll HaEATht-HETANl
4-01-001-12 aH^AIht-lll KA-iE
4-01-001-1) MEAlw-ISOl/CI ANE
4-01-001-14 UREAHt-ISIIPtMANE
4-03-001-14 iKtiTII-lllLUtNt
4-fll-OOl-lO KORKING-Jll fujl
4-61-OOl-SI HUH* iNG-HEHDStNC
4-01-CC1-52 MOHKINl-OIST IJtl
4-OJ-001-5) mJHMNC-llFNfENE
4-01-001-55 IORKINI.-CY'LCrtir
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4-01-001-1?
4-03-UU-SS
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4-C3-OOI-60 MONK INo->*EM ANF.
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4-01-007-04
4-01-002-00
4-01-002-01.
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4-03-00/-10
4-01-002-11
4-01-002-12
4-O-002-14
4-01-O02-1S
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4-01-O01-02
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4-01-OCI-05
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4-01-003-10
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1000 oALl CMS
1000 C.»Li (INS
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1000 GALICNS
1000 r.«LLO«s
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100P (.ALA cm
1010 GAUONS
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1 J09 r,AI LONS
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1000 uALlONS
loui '.ALLUNS
IfOO GAILI'-IS
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11)0 ".AllONS
loon I/ALLPNS
1UOO GALLONS
1040 GAUONS
IOOU GALLONS
1100 GALLUNS
1000 GALICNS
UJO G'LLONS
ICOO r.ALLOMS
lOOJ CAILO'K.
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1 OOC C* LL PN S
10 >C GAIL DNS
1009 GALLCNS
1000 r.Aunss
IOOU GALLONS
1^00 GALLl'NS
IPCd G'lLJNS
1090 GALLONS
1003 GALLONS
inGO GALLONS
1000 GALLONS
1900 GALLTNS
IflPO GAI IONS
1000 GAlin-iS
1000 G'LI'NS
1'JOO GALLONS
1000 Ciltl.'iS
1000 CT
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-------
Hydrocarbon emissions from fuel combustion sources are part of the
RAPS hourly emission inventory. Data for evaporative emissions, which
account for approximately 40 percent of the point source hydrocarbon
emission, are only gathered as part of inventory or production control and
are presented as annual data.
Base data, such as storage capacity, throughput, production, consumption,
etc., for the St. Louis Air Quality Control Region (AQCR-70) were obtained
from 64 companies with emissions in excess of one ton per year. This repre-
sents about 450 points. Thirty-seven of the companies emit in excess of
100 tons per year, ten in excess of 10 tons per year, and seventeen in
excess of one ton per year. Gas stations and dry cleaning establishments
may emit greater than one ton per year hydrocarbons. However, they are
included in the area sources inventory. Locations of the stacks, accurate
to ten meters, were obtained from visiting plant sites and pinpointing the
location of sources on U.S. Geological Survey maps. In addition, stack
parameters and operating patterns were obtained from individual companies.
Emission patterns for hydrocarbon sources vary widely due to the
variety of types of hydrocarbon sources. As mentioned before, emissions
from combustion sources were received continuously as part of the RAPS
Point Source Inventory, generally on an hourly basis. Hydrocarbon data
from sources which produce or use coatings and solvents are accompanied with
hourly use patterns based on working hours during a year. Evaporative
emissions from petroleum storage are assumed to be generated on a continuous
basis and are, therefore, spread equally throughout the year.
All of this information has been stored in the RAPS emission inventory
data bank at EPA/RTP.
2.2 AREA SOURCES
Area sources of hydrocarbons include industrial area sources, residen-
tial and commercial sources, highway vehicles both as line and area sources,
railroads and river vessels, airports, and off-highway mobile sources. All
of the emissions from these sources have been spatially distributed into
1989 grids in accordance with the RAPS grid network (1).
-------
Industrial area sources which are too small to be considered as point
sources were determined by contacting individual companies and obtaining fuel
consumption or throughput data. From these data, emissions were calculated
using emission factors. These emissions were then assigned to the grid square
in which the company was located. This category includes 53 companies.
Stationary residential and commercial sources include fuel combustion for
heating, evaporative emissions from dry cleaning plants, surface coating
operations and gasoline marketing, structural fires, and solid waste disposal.
These emissions have been determined and distributed to each grid square
according to residential and commercial land use.
Highway vehicle line source emissions have been determined and distri-
buted over the AQCR according to the location of the line sources within the
RAPS gridding system. Highway vehicle area sources have been determined as
an off-shoot of the highway line sources arid the emissions have been assigned
to the appropriate grid square.
Airport emissions have been determined and distributed to those grids
containing airports and in which flight operations take place, such as take-
off and approach.
Off-highway mobile sources include motorcycles, lawn, garden and farm
equipment, construction equipment, industrial equipment and outboard motors.
The emissions from these sources have been distributed based on registrations;
residential, farm and commercial land use; and navigable waters, respectively.
River vessel emissions were based on towboat traffic and determined
primarily from records taken by the Corps of Engineers at Lock 27 near
St. Louis and on emission factors derived for similar engines of the Coast
Guard fleet and railroad locomotives.
Railroad fuel use and emissions were determined for two types of opera-
tions: line-haul operations and switch-yard activities. The former are
described as line sources consisting of a series of links within the study
area. Switch-yard operations utilize an area source concept.
For details of methodologies, the reader is referred to the reports
listed in Section 2.0. The area source inventory also has been stored in the
RAPS emission inventory data bank at EPA/RTP.
8
-------
3.0 HYDROCARBON CLASSIFICATION
In order to make a breakdown of hydrocarbon emissions according to
chemical structure, an appropriate compositional analysis must be applied
to each category of emissions within the available total hydrocarbon inven-
tory. Such an analysis has been applied by J. C. Trijonis and R. W.
Arledge (2) to organic emissions in Los Angeles.
The work described in that study appears to be applicable to St. Louis
with three major exceptions:
(1) Trijonis1 "reactivity classes" do not coincide completely with
the breakdown required for this report.
(2) Compositions of petroleum products and solvent usage may be
appreciably different between St. Louis and Los Angeles.
(3) There are sources in St. Louis which are not considered in the
Los Angeles study, such as coal combustion and coke ovens.
To make the information contained in the report applicable to the
present study, the following modifications were made:
1. The Trijonis report is organized according to reactivity classes
with 5-class reactivity categorization for organics. Each category contains
groups of compounds by name, e.g. C,-C3 paraffins in Class I, mono and
tertiary alkyl benzenes in Class II, C,+ paraffins in Class III, primary
and secondary alkyl benzenes in Class IV, and aliphatic olefins in Class IV.
All of the various organic emission sources in the Los Angeles area
are discussed and analyzed to determine what chemical compounds are emitted.
Each source is then tabulated to determine the extent of emissions in each
reactivity class. The results are expressed in mole percent. In addition,
the average molecular weights for each type of organic were determined and
included in the report.
-------
Since most of the source types exist both in Los Angeles and St. Louis,
the report has been useful in classifying RAPS data. The tabulations have
been reorganized by rearranging the chemical compounds into the broader
classes of paraffins, olefins, aromatics, aldehydes and non-reactives. The
non-reactives group includes all of the compounds in Class I of the Trijonis
classification. The paraffins group includes C,+ paraffins and alcohols,
ketones, acetates and cellosolves. The aromatics group is composed of all
aromatics with the exception of benzene, which is included with the non-
reactives. The hydrocarbon classification tables developed for each type of
source in the RAPS study area are included in the Appendix to this report.
The RAPS inventory presents emissions on a weight per unit time basis.
For this reason, the classification of hydrocarbons was reported on a weight
percent basis. This was accomplished by utilizing the molar percent tabula-
tions and the average molecular weights presented in the Los Angeles study.
The resulting tables are shown in Appendix A.
2. The composition of petroleum products in the St. Louis area was
ascertained and adjustments were made in the tabulation of emissions arising
from refinery operations, evaporative losses and automotive exhaust. These
changes are discussed in detail in the text of the report.
3. Emissions from coal combustion and coke ovens were investigated and
the results incorporated in this report.
3.1 POINT SOURCE INVENTORY
Once total hydrocarbon emissions were determined for each source, the
hydrocarbon classification was applied to determine the non-reactives,
paraffins, olefins, aromatics and aldehydes. The classification of hydro-
carbon emissions from point sources is shown in Table 4.
3.1.1 Fuel Combustion
The nature of fuel combustion for power generation or steam production
is similar at Los Angeles and at St. Louis; therefore, the same breakdown
has been used here for oil and gas consumption. The hydrocarbon classifi-
cation is shown in Table 1 of the Appendix.
10
-------
TABLE 4. HYDROCARBON BREAKDOWN—POINT SOURCES
Weight %
sec
1-XX-XXX-XX
2-XX-XXX-XX
3-01-018-99
3-01-026-99
3-01-999-99
3-03-003-01
3-03-003-02
3-03-003-03
3-06-001-02
to
3-06-001-09
3-06-002-01
3-06-004-01
to
3-06-008-05
3-90-XXX-XX
4-01-002-02
4-01-002-05
4-02-001-01
4-02-003-01
4-02-004-01
4-02-005-01
4-02-006-01
4-02-008-01
4-02-009-01
4-02-999-99
4-03-001-01
4-03-001-03
4-03-001-07
4-03-001-56
4-03-002-01
4-03-002-03
4-03-002-07
4-03-999-99
4-06-001-26
4-06-001-30
4-06-002-01
4-06-002-05
5-01-001-01
Non-Reactive
66
66
0
0
0
83
83
83
66
5
5
66
100
0
6
0
0
6
6
8
9
9
8
8
8
0
8
5
8
8
8
8
8
8
42
Paraffins
10
10
0
0
0
1
1
1
10
95
74
10
0
0
78
100
89
78
81
24
70
70
68
68
68
100
68
74
68
68
68
68
68
68
16
Olefins
9
9
0
0
0
13
13
13
9
0
15
9
0
100
0
0
0
0
0
1
0
0
24
24
24
0
24
15
24
24
24
24
24
24
31
Aromatics
5
5
100
100
100
3
3
3
5
0
6
5
0
0
16
0
11
16
13
67
21
21
0
0
0
0
0
6
0
0
0
0
0
0
4
Aldehydes
10
10
0
0
0
0
0
0
10
0
0
10
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
7
11
-------
Hydrocarbon emissions from coal combustion were not studied by Trijonis,
and the only literature data found on this subject referred only to total
hydrocarbons and polynuclear hydrocarbons. Because of this lack of informa-
tion, the classification reported for oil combustion was also used for
emissions from coal combustion. This should be reasonably satisfactory con-
sidering the similarity of conditions of high temperature and residence time
in a boiler, as well as the small amounts emitted. Two percent of the total
hydrocarbons in the AQCR originates from boiler operations; moreover, most
of it is methane.
3.1.2 Industrial Processes
Industrial sources of hydrocarbon emissions in AQCR 70 include some
chemical manufacturing, coke production, refinery operations (which include
fuel combustion covered previously), and evaporative emissions from
degreasing operations, petroleum product storage and bulk marketing.
Emissions from chemical manufacturing in the St. Louis area occur
primarily from manufacture of products used for plastic and rubber formula-
tions. In all processes examined, the products are derivatives of benzene or
phenol. The emissions are, therefore, entirely aromatics. This classifica-
tion is shown in Table 2 of the Appendix.
Coke oven emissions result from several points in a coking plant
including charging holes, pushing doors and many leaks. The best available
sources (3-5) indicate that the composition of the emissions is similar to
the coke oven gas which is produced in a coking plant. The composition of a
typical coke oven gas is given in Table 5. This analysis has been reorgan-
ized and the hydrocarbon classification is included as Table 3 in the
Appendix.
12
-------
TABLE 5. COKE OVEN GAS ANALYSIS
Hydrogen Sulfide
Carbon Dioxide
Nitrogen
Hydrogen
Carbon Monoxide
Methane
Ethane
0.7% by vol.
1.7% by vol.
0.9% by vol.
56.7% by vol.
5.7% by vol.
29.6% by vol.
1.28% by vol.
Ethyl ene
Propylene
Propane
Butyl ene
Butane
Acetylene
Light Oil
2.45% by vol.
0.34% by vol.
0.08% by vol.
0.16% by vol.
0.02% by vol.
0.05% by vol.
0.65% by vol.
Refinery emissions arise from a variety of sources. Emissions from
power house boilers and process heaters are included in the previous section
on fuel combustion. Other emissions are from leaks or vents connected with
transfers, drains, blow-downs, vacuum jets, compressors, valves, seals, and
flanges. The Los Angeles study was very complete for refinery emissions.
The operation of refineries is very similar at St. Louis and at Los Angeles.
The basic difference is that crude oil in St. Louis is obtained from mid-
continent and Arabian sources whereas the crude processed in Los Angeles is
primarily from West Coast and Indonesian sources. Crude oil processed in
California is generally of a much higher aromatic content, typically 20 to
35 percent versus 10 to 15 percent in the Midwest (6).
The Petroleum Chemicals Division of DuPont reports biannually on the
characteristics of gasolines sampled across the country (7). Gasoline from
St. Louis is not included in the survey, but Kansas City is, and the compo-
sition of gasoline in St. Louis is much like that in Kansas City (8). The
average hydrocarbon analyses of gasolines from Los Angeles and Kansas City
are given in Table 6. It can be seen that the aromatics are considerably
higher in Los Angeles.
13
-------
TABLE 6. DUPONT GASOLINE ANALYSIS
Research Octane Aromatics Olefins Saturates
Percent
Winter
1975-1976
Los Angeles — leaded regular
Kansas
Summer
unleaded regular
premium
City—leaded regular
1976
unleaded regular
premium
Los Angeles--leaded regular
Kansas
unleaded regular
premium
City—leaded regular
unleaded regular
premium
93.
93.
98.
92.
91.
98.
93.
93.
98.
93.
91.
98.
2
2
6
9
7
8
3
5
7
7
5
6
27.
30.
26.
14.
13.
14.
29.
35.
29.
22.
21.
14.
0
0
0
5
5
0
0
0
0
0
0
5
7.
7.
4.
13.
15.
7.
6.
7.
5.
7.
12.
6.
0
0
0
0
0
5
0
0
0
5
0
5
65.
63.
70.
72.
71.
78.
65.
58.
66.
70.
67.
79.
0
0
0
5
5
5
0
0
0
5
0
0
Combining the values for summer and winter as well as leaded and
unleaded regular gasolines gives the values shown in Table 7. Since in
1975-1976 about 55 percent of the gasoline sold was regular, 45 percent
premium, the averages were weighted by this proportion, which gave the values
shown in columns 3 and 6 of Table 7. The percentage difference between Los
Angeles and Kansas City is shown in the next column. These values were used
to adjust gasoline related emissions and are reflected in Tables 4, 20 and
21 in Appendix A.
TABLE 7. AVERAGE COMPOSITION OF GASOLINES
Aromatics
Olefins
Saturates
Los Angeles
1 2 3
Weighted
Regular Premium Average
c/ °/ °/
h h /o
30.25 27.50 29.00
6.75 4.50 5.75
63.00 68.00 65.25
Kansas City
456 7
Weighted Percentage
Regular Premium Average Difference
°/ °i °i
h h h
17.75 14.25 16.17 0.557
11.88 7.00 9.68 1.686
70.37 78.75 74.15 1.136
14
-------
The classification of hydrocarbons emitted from catalytic crackers was
determined by source test results and is included as Table 5 in the Appendix.
Degreasing operations are very straightforward. The solvents used are
either trichloroethane or trichloroethylene. Trichloroethane is a partially
halogenated paraffin, whereas trichloroethylene is a partially halogenated
olefin. These sources are shown in the hydrocarbon classification scheme
in Tables 6 and 7 in the Appendix.
Surface coating emissions occur from coating operations which include
automobile and truck body and parts coating, applicances coating, and can
manufacturing. A few of the companies have purely air-dried operations,
but most of the coating operations involve a heat curing step. Each
company involved in surface coating was evaluated to determine what percent-
age of the emitted hydrocarbons are evolved in the spray booths versus the
curing ovens. This involved estimating the percentage of overspray and the
time allowed for "flash-off" of a portion of the solvents used in formulation
before the piece entered the curing oven. The values reported by Trijom's
for heat treated coatings were applied to the hydrocarbons emitted in the
curing ovens. The SCC codes differentiate between the types of surface
coatings applied; i.e., lacquers, enamels, varnish, etc. Each type of
coating was studied to determine the approximate hydrocarbon composition used
in formulation (9, 10) and these compositions were used to classify the
hydrocarbons emitted during the air drying part of the surface coating
operation - the spray booths. The hydrocarbon classification for each type
of surface coating included in the inventory is shown in Tables 8 through
12 in the Appendix.
Petroleum product storage and bulk marketing facilities have emissions
which are typical of the vapors which exist over the liquids stored. All
volatile petroleum products such as gasoline and crude oil are stored in
floating-roof storage tanks. Emissions from these are solely due to leakage
around the seals within the tanks. The other source of emissions is the
filling of tank trucks and barges as vapors are displaced as the tank fills.
The composition of the vapors accumulated over the gasoline approaches the
equilibrium composition of gasoline vapor. The hydrocarbon classifications
for emissions from gasoline storage tanks are shown in Table 13 of the
15
-------
Appendix.
3.2 AREA SOURCES
The classification of hydrocarbon emissions from area sources is shown
in Table 8.
River vessels and railroads are assumed to have diesel engines which
produce all of the hydrocarbon emissions. Emissions from diesel engines
were studied extensively by Battelle Labs (11). The results should be
applicable to St. Louis. The classification of hydrocarbons used here is
the same as for diesel engines presented in Table 22 in the Appendix.
Airport emissions include aircraft operations, exhaust emissions from
service vehicles and evaporative emissions from fuel handling. Hydrocarbon
emissions are distributed 79 percent, 13 percent and 8 percent, respectively,
to these sources (12). Lambert International and Scott Air Force Base con-
tributed 96.2 percent of the total hydrocarbons. Since, within the bounds
of this study, it was not possible to classify the hydrocarbons from all
airports individually, the hydrocarbon classification was based on the
operations at Lambert International and Scott Air Force Base.
Table 9 shows the classification of emissions for each of the hydro-
carbon sources and the weighted average for the airport. The complete
classification of these emissions is presented in Table 14 of the Appendix.
The aircraft emissions are based on the assumption of originating entirely
from jet engines; 98 percent of the aircraft emissions occur during the taxi
and idle modes of operation. The service vehicle emissions are assumed to
be the same as automotive exhaust emissions. Fuel handling emissions are
the same as the evaporative emissions from storing jet fuel.
TABLE 9. AIRPORT HYDROCARBON EMISSIONS
TYPE % OF TOTAL NON-REACTIVE PARAFFINS OLE FINS AROMATICS ALDEHYDES
Aircraft 79 11 44 27 15 3
Service Vehicle 13 12 47 15 26 0
Fuel Handling 8 0 70 5 25 0
Weighted Average 10 47 24 17 2
16
-------
TABLE 8. HYDROCARBON BREAKDOWN—AREA SOURCES
River Vessels
Railroads
Residential and Commercial
Fuel Combustion
Evaporative
Surface Coating
Missouri
Illinois
Gasoline Marketing
Dry Cleaning
Structural Fires
Solid Waste Disposal
Stationary Industrial
Airports
Highway
Light Duty Vehicle
Exhaust
Evaporative
Heavy Duty - Gas
Exhaust
Evaporative
Heavy Duty - Diesel
Exhaust
Off-Highway Sources
Motorcycles
Lawn & Garden
Farm Equipment
Construction Equip.
Industrial Equip.
Outboard Motors
Non-Reactive
3
3
66
6
9
8
76
42
42
26
10
11
4
11
4
3
12
12
8
7
10
12
Weight
Paraffins
53
53
10
57
70
68
23
16
16
52
47
48
60
48
60
53
47
47
49
50
49
47
%
Olefins
12
12
9
0
0
24
0
31
31
3
24
21
20
21
20
12
15
15
14
13
14
15
Aromatics
12
12
5
37
21
0
1
4
4
16
17
20
16
20
16
12
26
26
21
18
23
26
Aldehydes
20
20
10
0
0
0
0
7
7
3
2
0
0
0
0
20
0
0
8
11
4
0
17
-------
Stationary residential and commercial fuel combustion sources include
combustion of coal, oil, natural gas, and liquified petroleum gas. For
these emissions the same classification used with point source fuel combus-
tion was applied (Table 1, Appendix).
Evaporative hydrocarbons from surface coating include emissions due to
the solvent content of retail paints. Illinois has a state regulation
restricting photochemically reactive solvents which is very similar to Los
Angeles APCD Rule 66 (13). Trijonis1 report includes a table of the
national average solvent composition which is given in Table 10. According
to Mr. Raymond Connor of the National Paint and Coating Association (14),
this table of values is still the best available information. The State of
Missouri does not have a hydrocarbon regulation similar to Illinois; there-
fore, the data in Table 10, column 3, were used for the Missouri portion of
the hydrocarbons from surface coating. The composition in the last column
of Table 10 was used for the Illinois portion of the hydrocarbons. The
individual classifications of hydrocarbons in each state are presented in
Tables 15 and 16 in the Appendix.
Evaporative hydrocarbons from service stations are generated from
filling the underground storage tanks at service stations and from filling
automobile tanks. The volume of these emissions is considered as being
split equally from the filling of the underground tanks and automobile tanks
(15). The DuPont analyses of gasoline in Kansas City and Los Angeles have
been used to modify the emissions classification.
Evaporative hydrocarbons from dry cleaning operations are the result of
using cleaning solvents which are either perchloroethylene or petroleum
based solvents. Based on a 1974 study in St. Louis city, the usage if 76
weight percent perchloroethylene and 23 weight percent petroleum based
solvents. Table 11 gives the hydrocarbon compositions from each of these
solvent types and the weighted average which is used for classifying the
cumulative emissions in the AQCR. This classification is presented in
further detail in Table 17 in the Appendix.
18
-------
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19
-------
TABLE 11. DRY CLEANING HYDROCARBON EMISSIONS
SOLVENT NON-REACTIVE PARAFFINS OLEFINS AROMATICS ALDEHYDES
Perch! oroethylene
Petroleum Based
Weighted Average
100
0
76
0
94
23
0
0
0
0
6
1
0
0
0
Hydrocarbon emissions from structural fires and solid waste disposal
are the last type of residential and commercial sources. The only data
available for this source are reported by Trijonis and are reflected in
Table 8. The detailed classification of hydrocarbons from waste incinera-
tion is shown in Table 18 in the Appendix.
Emissions from stationary industrial sources include a variety of types
of activities. The best approximation of these sources indicates that 70
percent consists of air dried surface coating and 30 percent of combustion
(16). The classification in Table 8 reflects these percentages. A detailed
classification of hydrocarbons from this combination of sources is shown in
Table 19 in the Appendix.
As stated earlier, gasoline in Los Angeles has a much higher aromatic
content than gasoline in St. Louis. The effect of higher aromatic content
in gasoline on exhaust emissions has been heavily studied. A numerical
relationship has been expressed by Wigg, et al (17), which states that there
is a linear relationship between aromatic hydrocarbon emissions and fuel
aromatic content and an inverse relationship between olefin emissions and
fuel aromatic content. This relationship is reported to be in relatively
good agreement with other studies on the same subject (18, 19). The
equations which were developed in this study are:
Exhaust (aromatic - benzene), % = 0.49 fuel aromatic, %
and
Exhaust olefin % = 39-(0.30 fuel aromatic), %
These equations and the DuPont analyses have been used to modify the
composition of hydrocarbons in automotive exhaust. The exhaust composition
thus derived is also in agreement with results reported by Kopczynski, et al,
20
-------
in a planning study in preparation for the RAPS project (20).
Evaporative hydrocarbon emissions from automobiles are comprised of
emissions from fuel tank breathing and the evaporation of gasoline from the
carburetor fuel bowl. These emissions have been determined by modifying the
values reported by Trijonis by decreasing the aromatic content by 44 percent
and increasing the olefin content.
The composition of hydrocarbons from automobile exhaust and evaporative
emissions are given in Table 8. The composition of the exhaust and evapora-
tive emissions of heavy duty gasoline powered trucks have been assumed to be
identical to those for light duty vehicles since there is no fundamental
difference between the engines and fuels used. The composition of the
exhaust emissions for heavy duty diesel powered trucks are classified in
Table 8. These are the same as those used for railroads which use diesel
engines. Evaporative emissions from diesel engines are considered negli-
gible. The classifications of exhaust and evaporative hydrocarbon emissions
are presented in Tables 20, 21 and 22 in the Appendix.
Off-highway mobile sources are comprised of a mix of gasoline and
diesel engines (22). Motorcycles, lawn and garden, and outboards are all
gasoline engines. Farm equipment is 61.9 percent gasoline powered, con-
struction equipment is 44 percent gasoline powered, and industrial equipment
is 78 percent gasoline powered. The exhaust hydrocarbon classification data
in Table 8 expresses these percentages. The exhaust emissions from gasoline
engines are the same as the previously discussed automotive emissions, and
the exhaust emissions from diesel engines are the same as the previously
discussed diesel truck engines. The reclassifications of the hydrocarbons
from the groups of combined gasoline and diesel engines are presented in
Tables 23, 24, and 25 1n the Appendix.
21
-------
4.0 SUMMARY
A detailed inventory of organic emissions has been developed for the
St. Louis AQCR. The inventory has been incorporated into the RAPS data base
and is stored on EPA's Univac 1110 computer at Research Triangle Park,
North Carolina.
The inventory consists of a listing of all industrial point source
emissions in excess of one ton per year, a listing of stationary area sources
such as gasoline marketing and dry cleaning operations, and a compilation of
mobile sources including surface transportation, railroad, river vessels,
airports and off-highway mobile sources.
Emission data are available for each source category, either as total
hydrocarbons or broken down into five structural categories: paraffins,
olefins, aromatics, aldehydes and non-reactives. Appropriate factors were
developed for the St. Louis area and applied to the hydrocarbon emission
data. These classification factors are also stored on the Univac computer.
As a consequence, an emission inventory for the five categories of organics
is now available for the St. Louis AQCR. A summary of the total emission
broken down into the five structural categories is shown in Table 12.
22
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L
-------
REFERENCES
1. Haws, Richard C., Paddock, Richard E., and Nasser, Charles C., The
Regional Air Pollution Study (RAPS) Grid System. EPA-450/3-76-021,
Research Triangle Park, North Carolina, December 1975.
2. Trijonis, J. C. and K. W. Arledge. Utility of Reactivity Criteria in
Organic Emission Control Strategies for Los Angeles. EPA Contract
Number 68-02-1735, TRW Environmental Services, December 1975.
3. National Research Council Committee. Chemistry of Coal Utilization.
Edited by Lowry, 1945, Vol. III.
4. Smith, William M. Evaluation of Coke Oven Emissions. Presented at
78th General Meeting of American Iron and Steel Institute, May 28, 1970.
5. United Nations Economic Committee--Europe. Air Pollution by Coking
Plants. 1968.
6. Sachanen, A. N. The Chemical Constituents of Petroleum. Reinhold,
New York, 1945.
7. E. I. DuPont de Nemours and Company, Inc., Petroleum Chemicals Division.
Road Octane Survey. Winter 1975-1976 and Summer 1976.
8. Private communication, Ed Sullivan, Amoco Oil Company, Wood River,
Illinois, March 21, 1977.
9. Danielson, John A. (ed.) Air Pollution Engineering Manual. AP-40,
U.S. Environmental Protection Agency. May 1973.
10. Gaynes, Norman I. Formulation of Organic Coatings. 1967.
11. Spicer, C. W. and A. Levy. The Photochemical Smog Reactivity of Diesel
Exhaust Organics. Report to the Coordinating Research Council from
Battelle Columbus Laboratories, May 1975.
12. Patterson, R. M., R. D. Wang and F. A. Record. Airport Emission
Inventory Methodology. EPA Contract Number 68-02-0041, GCA Corporation,
December 1974.
13. Private communication, Mike Elbl, Illinois Environmental Protection
Agency, Collinsville, Illinois, March 24, 1977.
24
-------
14. Private communication, Raymond J. Connor, Assistant Technical Director,
National Paint and Coating Association, Washington, D.C., March 24,
1977.
15. Holden, R. E. and W. E. Zegel. Residential and Commercial Area Source
Emission Inventory Methodology for the Regional Air Pollution Study.
EPA-450/3-75-078, Environmental Science and Engineering, Inc., September
1975.
16. Littman, F. E. and Kevin Isam. Stationary Industrial Area Source
Emission Inventory. Rockwell International, EPA Contract No. 68-02-2093
T0108D, July 1976.
17. Wigg, E. E., R. J. Campion and W. L. Petersen. The Effect of Fuel
Hydrocarbon Composition on Exhaust Hydrocarbon and Oxygenate Emissions.
Society of Automotive Engineers Report Number 720251, presented to the
Automotive Engineering Congress, Detroit, Michigan, January 10-14, 1972.
18. Dishart, K. T. and W. C. Harris. The Effect of Gasoline Hydrocarbon
Composition on Automotive Exhaust Emission. Proceedings at American
Petroleum Institute, Division of Refineries, 1968, Vol. 48, pp. 612-642.
19. Eccleston, B. H. and R. W. Hum. Comparative Emissions from Some Leaded
and Prototype Lead-Free Automobile Fuels. Bureau of Mines, RI Number
7390, May 1970.
20. Kopczynski, S. L., W. A. Lonneman, T. Winfield and R. Seila. Gaseous
Pollutants in St. Louis and Other Cities. J. Air Pollution Control
Association, 2_5:251, 1975.
21. Compilation of Air Pollutant Emission Factors. AP-42, U.S. Environ-
mental Protection Agency, Supplement 5, December 1975.
22. Hare, Charles T. Methodology for Estimating Emissions from Off-Highway
Mobile Sources for the RAPS Program. EPA 450/3-75-002, October 1974.
-------
APPENDIX A
RAPS Hydrocarbon Classification for Types of Sources
26
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TECHNICAL REPORT DATA
(Please read Instructions on the reverse before completing}
1. REPORT NO.
EPA-600/4-78-028
3. RECIPIENT'S ACCESSION NO.
4. TITLE AND SUBTITLE
REGIONAL AIR POLLUTION STUDY
Point and Area Source Organic Emission Inventory
6. PERFORMING ORGANIZATION CODE
5. REPORT DATE
June 1978
7 AUTHOR(S)
R.W. Griscom
8. PERFORMING ORGANIZATION REPORT NO.
9. PERFORMING ORGANIZATION NAME AND ADDRESS
Rockwell International
Air Monitoring Center
11640 Administration Drive
Creve Coeur, MO 63141
10. PROGRAM ELEMENT NO.
1AA603 AA-09 (FY-77)
11. CONTRACT/GRANT NO.
68-02-2093
Task Order 108 I
12. SPONSORING AGENCY NAME AND ADDRESS
Environmental Sciences Research Laboratory - RTP, NC
Office of Research and Development
U.S. Environmental Protection Agency
Research Triangle Park, NC 27711
13. TYPE OF REPORT AND PERIOD COVERED
Einal
14. SPONSORING AGENCY CODE
EPA/600/09
15 SUPPLEMENTARY NOTES
16 ABSTRACT
An inventory of organic emissions from stationary and mobile sources
has been assembled for the St. Louis Air Quality Control Region. The inventory
covers point and area sources for process, combustion and evaporative emissions.
A breakdown into five categories had been assigned to each source type. The
categories are (1) paraffins, (2) olefins, (3) aromatics, (4) aldehydes, and
(5) non-reactives. This report describes how this classification has been
determined for hydrocarbon emissions in the St. Louis AQCR and provides sufficient
reference data to derive alternative schemes as required. The breakdown was made
part of the RAPS Emission Inventory System, which is stored on the EPA's Univac
computer at Research Triangle Park, N.C.
17.
a
KEY WORDS AND DOCUMENT ANALYSIS
DESCRIPTORS
*Air pollution
*0rganic compounds
*Emission
*Environmental surveys
*Sources
b.IDENTIFIERS/OPEN ENDED TERMS C. COSATI Field/Group
St. Louis, MO
13 B
07 C
05 J
Ifl DISTRIBUIION STATEMENT
RELEASE TO PUBLIC
19 SECURITY CLASS (This Report)
UNCLASSIFIED
21. NO. OF PAGES
58
20 SECURITY CLASS (Thispage}
UNCLASSIFIED
22. PRICE
EPA Form 2220-1 (Rev. 4-77) PRFVIOUS EDITION is OBSOLETE
52
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