EPA-450/3-74-008
May 1973
NATIONAL EMISSIONS
INVENTORY
OF SOURCES
AND EMISSIONS
OF
TITANIUM
U.S. ENVIRONMENTAL PROTECTION AGENCY
Office of Air and Water Programs
Office of Air Quality Planning and Standards
Research Triangle Park, North Carolina 27711
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EPA-450/3-74-008
NATIONAL EMISSIONS INVENTORY
OF
SOURCES AND EMISSIONS
OF
TITANIUM
by
GCA Corporation
GCA Technology Division
Bedford, Massachusetts 01730
Contract No. 68-02-0601
EPA Project Officer: David Anderson
Prepared for
ENVIRONMENTAL PROTECTION AGENCY
Office of Air and Water Programs
Office of Air Quality Planning and Standards
Research Triangle Park, N. C. 27711
May 1973
-------
This report is issued by the Environmental Protection Agency to report technical
data of interest to a limited number of readers. Copies are available free of
charge to Federal employees, current contractors and grantees, and nonprofit
organizations - as supplies permit - from the Air Pollution Technical Information
Center, Environmental Protection Agency, Research Triangle Park, North
Royal Road, Springfield, Virginia 22151.
This report was furnished to the Environmental Protection Agency by GCA Corp-
oration, Bedford, Massachusetts, in fulfillment of Contract No. 68-02-0601. The
contents of this report are reproduced herein as received from GCA Corporation.
The opinions, findings, and conclusions expressed are those of the author
and not necessarily those of the Environmental Protection Agency. Mention of
company or product names is not to be considered as an endorsement by the
Environmental Protection Agency.
Publication No. EPA-450/3-74-008
11
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ACKNOWLEDGEMENT
The continued cooperation and dedication of Mr. Carl Spangler of
EPA, who served as Program Monitor until his death, is deeply appre-
ciated.
GCA would like to extend thanks to Mr. David Anderson and Mr.
James Southerland of EPA for their cooperation in the preparation of
this study.
In addition, special thanks are also due to Mr. W. Wessell, Com-
modity Specialist, Bureau of Mines, who provided significant technical
inputs to this program.
ill
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TABLE OF CONTENTS
SECTION TITLE ' PAGE
ABSTRACT " vii
I INTRODUCTION . • • 1
.A. PURPOSE AND SCOPE 1
B. CONCLUSIONS 2
II OVERALL U.S. MATERIAL FLOW-CHART FOR TITANIUM 4
A. ORE PRODUCTION . 4
B. INGOT AND METAL PRODUCTION 4
C. ALLOYS AND' CARBIDES 6
D. PIGMENTS PRODUCTION 6
E. CERAMICS, FIBERGLASS AND OTHER USES 7
F. WELDING ROD C.OATINGS 7
G. REPROCESSING OF TITANIUM'METAL 8
H. PIGMENT AND METAL CONSUMPTION 8
III SOURCES AND ESTIMATES OF TITANIUM-CONTAINING
EMISSIONS 9
A. DATA PRESENTATION AND ACCURACY 9
B. DEVELOPMENT OF EMISSIONS ESTIMATES - 1970 15
C. SUMMARY OF PRINCIPAL EMISSIONS 22
IV REGIONAL DISTRIBUTION OF PRINCIPAL SOURCES
AND EMISSIONS 23
V NATURE OF EMISSIONS 27
VI UPDATING OF EMISSIONS ESTIMATES 29
A. VERIFICATION OF CURRENT ESTIMATES 29
B. PERIODIC REVIEW OF ESTIMATES 29
VII REFERENCES 31
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LIST OF TABLES AND FIGURES
TABLE NO.
TITLE
SOURCES AND ESTIMATES OF TITANIUM-CONTAINING
EMISSIONS
SUMMARY OF ?RINCIPAL SOURCES AND EMISSIONS -
TITANIUM
REGIONAL DISTRIBUTION OF PRINCIPAL SOURCES
AND EMISSIONS
PHYSICAL PROPERTIES OF Ti and Ti00
PAGE
10
22
24
27
FIGURE NO.
1
2
TITANIUM 1970 MATERIAL FLOW
EMISSION OF PARTICULATE IN FERROSILICON
PRODUCTION
17
VI
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ABSTRACT
A national inventory of the sources and emissions of the
element titanium was conducted. The study included the preparation
of an overall material flow chart depicting the quantities of titanium
moving from sources of mining and importation through all processing
and reprocessing steps to ultimate use and final dispostion. All
major sources of titanium-containing emissions were identified and
their titanium emissions into the atmosphere estimated. A regional
breakdown of these sources and their emissions was also provided. The
physical and chemical nature of the titanium-containing emissions
was delineated to the extent that information was available, and a
methodology recommended for updating the results of the study every
two years.
Vl l
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I. INTRODUCTION
A. PURPOSE AND SCOPE
The Monitoring and Data Analysis Division, Office of Air Quality
Planning and Standards of the U.S. Environmental Protection Agency (EPA)
has contracted with GCA Technology Division to conduct a national inventory
of the sources and emissions of the element titanium. The purpose of the
study was to define as accurately as possible, based on existing and avail-
able published and unpublished information, the levels, nature and sources
of titanium-containing emissions for defined geographic regions throughout
the United States.
The scope of this program is outlined below:
Develop an overall material flow chart
depicting the quantities of titanium mov-
ing from sources of mining and importa-
tion, through all processing and repro-
cessing steps to ultimate use and final
disposition as far as the movements can
be traced.
Identify all major potential titanium
containing emission sources and estimate
the total quantity of titanium emitted
to the atmosphere from each source.
Emission factors and level and types of
air pollution control will also be provided
for each of these sources to the extent
that available information permits.
Define those sources which contribute at
least 80 percent of the total emissions
of titanium.
Provide a regional breakdown of these
major sources and their emissions.
Present the nature of the titanium-con-
taining emissions for each of these
major sources including a delineation of
their physical and chemical form and
particle size distribution to the extent
that information is available.
Provide recommendations as to a methodol-
ogy for updating the results of this
study every two years.
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B. CONCLUSIONS
1. Material Flow
Based on all available data, 499,000 tons of titanium were
consumed in the U.S. in 1970. As shown in Figure 1, this was almost
entirely new metal, with only 7,000 tons of scrap being recycled. The
sources of the metal were imports and mining of ilmenite, in approximately
equal proportions.
The principal use of titanium was for pigment (79 percent
of U.S. total) in the form of titanium dioxide Ti02. Metallurgical pro-
cesses used most of the remaining 21 percent of the metal. Of the pigment
used, slightly more than half was used for paints and related materials.
About one fifth of the pigment was used by the paper industry. Several
other industries needing a high quality white pigment used the remaining
material.
2. Principal Emission Sources
Almost 90 percent of the atmospheric emissions of titanium
were not associated with the titanium industry, but result from certain
emission sources termed "inadvertent" sources. The largest of these is
the combustion of large quantities of coal, although coal ash contains
only about .07 percent of titanium. The emission of titanium from coal
combustion was estimated to, be 73,000 tons in 1970, or an amount equal to
almost 15 percent of the titanium consumed in 1970.
Within the titanium industry, three sources were identified
which contributed a total of only about 2 percent of total U.S. emissions.
These were associated with the mining and beneficiation of ilmenite and
with the production and consumption of TiO- pigment. For the most part,
these three emission categories were each distributed over fewer than 14
source locations. This compares with between 1000 and 2000 sources of
inadvertent emissions.
3. Regional Emissions v
The region of the U.S. in which most of the estimated titan-
ium is emitted is Region 5 (Ohio and vicinity) which consumes about 40
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percent of the nation's coal. Regions 3 and 4 (Pennsylvania to Florida)
each contribute about two thirds as much emission as Region 5. The Region
having the most emission per square mile is Region 3, followed closely by
Region 2 (New York to Virginia).
4. Nature of Emissions
Little information describing titanium emissions was found.
Based on the characteristics of the mineral, the metal, and the pigment,
in comparison with the processes contributing the emissions, most of the
emission is probably in the form TiO,,, in particles ranging from 0.1 mi-
crometers up to 10 micrometers. Except for fallout of the largest par-
ticles shortly after emission, there is no reason to expect any unusual
physical or chemical changes in the emitted particles following emission.
5. Degree of Control
The overall level of control of titanium emission is esti-
mated to have been about 80 percent in 1970.' This is largely the result
of an estimated 82 percent control of coal burning emissions. The degree
of control of the largest emission sources within the titanium industry is
variable, ranging from 5 to 90 percent estimated; however, these emissions
are a small portion of the U.S. total.
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II. OVERALL U.S. MATERIAL FLOW CHART FOR TITANIUM
Figure 1 presents a flow diagram depicting the total quantities of
titanium products moving from sources of mining and importation through
the processing and reprocessing steps to ultimate use and final disposition.
Each of these sources is discussed below.
A. ORE PRODUCTION
Ilmsnite (FeO-TiO,,) is the primary source of domestic titanium.
It is found in coastal sands and inland deposits. The only inland mining
operation is at Tahawas, New York and accounts for about one-third the
total concentrate production . The rest comes from coastal dredging
operations, located mostly in Florida.
The Tahawas operation is an open pit mine. The ore is extrac-
ted by drilling and blasting operations, loaded by electric shovels onto
diesel-powered trucks and carried to the beneficiation plant. When the
ore is dredged, the resulting slurry is pumped directly to the benefi-
ciating plant.
The beneficiation process at the Tahawas operation involves
primary, secondary and tertiary crushing, screening, magnetic separation,
grinding and further magnetic separation resulting in a final product
which is 45 percent TiO?. Beneficiation of the dredged slurry from
coastal operations includes dewatering, cleaning, scrubbing, drying and
electrostatic and magnetic separation, and results in a concentrate of
over 60% Ti02.
B. INGOT AND METAL PRODUCTION
Only a small part of the titanium processed in this country
goes into metal production. At present all titanium metal and related
alloys are processed from rutile. There are experimental investigations
of upgrading ilmenite to produce low-grade rutile, but they are currently
in the developmental stage. All rutile used in domestic processes is
imported, about half being used in metallurgical processes.
* Note: Data in Figure 1 and in this section are left unrounded, for pur-
poses of information control. On average, the typical statistic
is accurate to within 10%, in the opinion of the authors.
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7 Scrcp
Figure 1. Titanium 1970 Material Flow
(thousand tons contained Ti)
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The main method for producing titanium metal is the Kroll pro-
cess. In the basic process, Ti Cl, is reacted with Mg in-an inert atmos-
phere forming Ti metal and Mg Clj. Titanium is very susceptible to
attack by N2> 0^, and H2 at elevated temperatures and an inert atmosphere
must be maintained to avoid contamination.
The Ti Cl, necessary to this process is produced by passing
heated Cl? gas up through a bed of a mixture of ground rutile and coke
resulting in the formation of crude Ti Cl, with CO and C02 as by-products.
The Ti Cl, is then purified chemically and by partial distillation.
The titanium sponge metal which results from the Kroll process
is consolidated primarily by means of arc-melting. The sponge is placed
in a water-cooled copper container under an inert atmosphere and heated
by an electric arc. The sponge melts, is then cooled forming titanium
ingots.
C. ALLOYS AND CARBIDES
Titanium-base alloys are manufactured commercially by adding the
alloying metal to titanium sponge during arc-melting. Non-titanium base
alloys of Cu, Ni and Ag use TiH_ as a raw material. They are prepared by
gradual heating of a mixture of the powdered metal and TiH? in a vacuum.
The TiH« used in this process is produced by feeding rutile and Ca H~ into
a furnace with a hydrogen atmosphere at 1830 F. The products, lime and
TiH?, are then separated by leaching. The TiH_ is then ground to a powder.
The hydrogen is driven off under the vacuum and the resulting titanium
metal powder is combined with the base metal of the alloy.
Titanium carbides are prepared by heating Ti02 and carbon in an
atmosphere of H~ or in a vacuum. Ferrotitanium master alloys are produced
like other ferroalloys and are used in producing ferrotitanium steels.
D. PIGMENTS PRODUCTION
Over 987» of all domestic ilmenite is used for pigment production.
Until recently, the major route from concentrated ore to HO^ pigments
was the sulfate process. Another process, the chloride process, has
reached a level of equal importance.
6
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In the sulfate process, ilmenite is decomposed by adding sulfuric
acid in order to remove the FeO component of the concentrate. The reaction
product is dissolved, filtered, hydrolized, filtered again and washed,
conditioned, calcined and the resulting TiO? crystals are ground to the
desired pigment size.
The chloride process uses rutile to produce Ti Cl, . This is
converted directly to Ti CL through a vapor phase reaction between Ti Cl,
and steam at 400°C. Solid phase Ti 0- particles precipitate into a duSt
chamber, are collected and ground to specification.
E. CERAMICS, FIBERGLASS AND OTHER USES
In the production of ceramic material, titanium functions as
an opacifier in the frit. The frit is made by fusing various minerals in
a smelter and quenching them rapidly in water. This quenching shatters
the mixture into small glass particles called frit which are then dried
and ground in a ball mill. The primary applications for the frit which con-
tains TiOp is in enameling iron and steel and in glazing pottery.
Rutile is used in the production of fiberglass. It is added
to molten glass in an oven. The glass is then dropped through a small
orifice in the bottom of the furnace and blown into filaments which are
wound onto a plastic tube and drawn into a smaller diameter.
Ti Cl, in contact with moist air reacts with the water vapor
to form Ti Cl ' 5EnO which on further reaction with water forms titanium
4 2
hydroxide and HC1. The titanium hydroxide particles are of visible size
and quite opaque. This reaction and its resulting visible manifestation
makes Ti Cl, ideal for sky-writing and for smoke screens.
Titanium also finds uses in photography, electronics, and syn-
thetic gem manufacture.
F. WELDING ROD COATINGS
Rutile is also used in welding rod coatings. It is mixed in a
slurry and placed in a press with the rod to be coated. The rod and coating
are then extruded and fired to drive off the water so that the coating
will not explode upon use.
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G. REPROCESSING OF TITANIUM METAL
Only the purest scrap titanium can be used. It is melted down in
an inert atmosphere by an arc-melting process to form ingots, or embrittled
and pulverized in a mercury bath to form a high grade titanium powder.
H. PIGMENT AND METAL CONSUMPTION
Titanium dioxide pigments are blended in an appropriate vehicle
in the production of such items as paint, varnish, lacquer, paper, floor
coverings, rubber, printing ink, roofing, ceramics, and plastics.
Titanium metal has found extensive use in the aerospace industry
in the production of jet engines, air frames, missiles, etc. Because of
its susceptibility to attack by nitrogen, oxygen, and hydrogen at elevated
temperatures, all casting and joining is done under the protection of an
inert atmosphere. In machining and grinding, the titanium must be kept
immersed in a coolant to prevent it from fusing with the tool.
Ti 0~ and Ti 0 are found in small traces in coal and fuel oil and
there are some emissions during the burning of these fuels.
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III. SOURCES AND ESTIMATES OF TITANIUM-CONTAINING EMISSIONS
A. DATA PRESENTATION AND ACCURACY
Table 1 presents a summary of the data from which titanium
emissions were estimated for all major potential sources. Each of the
columns comprising this table will be discussed below.
1. Emission Factors
Except where indicated, this gives the pounds of total parti-
culates emitted per ton of production. Such considerations as:
. variations in process conditions among
individual plants comprising a source
category
. inaccuracies in existing data
. a limited quantity of existing data,
may, however, result in an average emission factor for a source category
varying by more than an order of magnitude from the value presented. In
recognizing the need to indicate the level of accuracy of these emission
factors., a reliability code is presented along with each emission factor
value appearing in the Table. This reliability code system is described
below and is based on the system utilized in EPA Document No. AP-42, "Com-
pilation of Air Pollutant Emission Factors":
A: (Excellent)
This value is based on field measure-
ments of a large number of sources.
B: Above Average
This value is based on a limited
number of field measurements.
C: Average
This value is based on limited data
and/or published emission factors
where the accuracy is not stated.
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TABLE 1
SOURCES AND ESTIMATES OF TITANIUM-CONTAINING EMISSIONS
1. MINING & BENEFICIATION
Open Pit Mining
Beneficiation
Open Pit
Dredging
2. METAL PROCESSING
Metal Ingots
Carbides
Alloys:
Titanium-Base
Ferrotitanium
Steel Production
Uncontrolled
Particulate
Emission Factor ,
(Ib/ton) (kg/kg x 10J)
.2 .1
38 19
9.5 4.75
0 0
0 0
0 0
150 75
25 12.5
Reli-
abil-
ity
Code
(D)
(B)
(D)
(D)
(C)
Pro-
duction
Level
(tons/yr)
1,850,000
152,000
308,000
„
-
-
5,872
(tons of
alloy)
2,590
(TK>2 con-
sumed as
Ferrotit.
in steel
mfg.)
in
Emissions
15
*
*
_
-
-
457,
*
Reli-
abil-
ity
Code
(A)
(B)
(B)
(C)
(-)
Emissions
Before
Controls
30
2,890
1,460
0
0
0
200
31
Esti-
mated
Level of
Emission
Control
0
90
90
.
-
-
407.
787.
Ti02
Emissions
After
Controls
(tons/yr)
30
289
146
0
0
0
120
7
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TABLE 1. (cont.)
3. OTHER MINERAL USES
Welding Rod Coating
Ceramics
Fiberglass
Pigment Production
Sulfate Calcining
Grinding
Drying & Sacking
4. PIGMENT CONSUMPTION
Paints, etc.
Other Uses
5. INADVERTENT EMISSIONS
Coal Burning
Coal Cleaning
Uncontrolled
Particulate
Emission Factor ,
(Ib/ton) (kg/kg x 10 )
0 0
16 8
2 1
150 75
.35 .175
NA ' NA
15 7.5
15 7.5
NA NA
NA NA
Reli-
abil-
ity
Code
(D)
(C)
(C)
(B)
(C)
(D)
(D)
Pro-
duction
Level
(tons/yr)
.
370
27,000
344,000
655,000
655,000
385,000
270,000
33,800,000
U.E.
2,000,000
U.E.
7, Ti02
in
Emissions
.
*
*
1007,
1007=
1007
*
*
1 . 27,
0.12%
Reli-
abil-
ity
Code
(B)
(A)
(A)
(A)
(A)
Ti02
Emissions
Before
Controls
0 .
3
27 ;
25,000
115 ;
NA
2,880
2,020
405,000
2,400
Esti-
mated
Level of
Emission
Control
.
67%
0%
(controls
generally
not used)
97%
107,
99.57.
107,
57,
827
857,
Ti02
Emissions
After
Controls
(tons/yr)
0
1
27
750
104
3,275
2,600
1,920
73,000
360
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TABLE 1. (cont.)
6. Oil Burning
Residual
Distillates
7. INCINERATION
8. Non Metallic
Minerals
U.S. TOTALS
Uncontrolled
Particulate
Emission Factor
(Ib/ton) (kg/kg x 10 )
NA NA
NA NA
NA NA
NA NA
Reli-
abil-
ity
Code
Pro-
duction
Level
(tons/yr)
123,000
U.E.
1 A 6, 000
U.E.
100,000
U.E.
6,900,000
(con-
trolled
emissions)
7, Ti02
in
Emissions
. 057.
.00657
4.27.
**
Reli-
abil-
ity
Code
(A)
(B)
(B)
(D)
Ti02
Emissions
Before
Controls
62
10
4,200
**
4'46,328f
Esti-
mated
Level of
Emission
Control
0
0
377=
**
Ti02
Emissions
After
Controls
(tons/yr)
62
10
2,650
3,000
**
S3,351
i
NA = Not Applicable
U.E. = Uncontrolled Emission
* Emission factor multiplier equal to tons of T
-•'••••- See Text
t Does not include pigment drying and non-metallic minerals
processed or handled annually
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D: Below Average
This emission factor is based on
engineering estimates made by know-
ledgeable personnel.
2. Level of Production Activity
This column depicts the quantity of material produced
(unless otherwise stated) 'annually. When multiplied by the emission
factor an estimate of the total particulate emissions for that source
in Ibs. .per year is obtained.
The values in this column are based on the material flow
calculations presented in Section II. Consequently, they have the same
+ 10% accuracy as do the material flow values.
3. 'Percent Metal inJEmissions
The method of analyzing or assaying a dust sample for the
amount of metal it contains determines to a large extent the reliability
of the data. For example, analytical chemistry techniques for dust con-
taining substantial fractions of metal can be accurate to within a small
percentage. On the other hand, optical spectroscopy methods for determining
concentrations on the order of parts per million can be inaccurate by a
factor of 2. Because of this variability, the reliability codes discussed
above for the emission factors are also utilized to estimate the relative
accuracy of the percentage values listed in column 3.
4. Level of Emissions before Control
The values in this column are derived by multiplying the
values in columns 1-3. The result is converted to tons/year of emissions
before control.
5. Estimated Level of Emission Control
The overall effectiveness of control for a source category
is based on two factors:
. the portion of the processes which are under control
. the typical degree of control
13
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For example, if 60% of vertical roasters have some type of particulate
emission control, and these include both scrubbers and precipitators such
that the apparent weighted average efficiency of control is 857=,, the over-
all control effectiveness is estimated to be 60 x 85 = 51%.
The accuracy of control efficiency data varies with the
degree of control. For a wet scrubber operating at 80% efficiency, i.e.
passing 20% material, the actual emission may safely be assumed to be
between 15 and 25% because of the relative ease of making determinations at
this level. Thus the emissions after control may be assumed to be accurate
within + 5/20 or 25%. On the other hand, for a baghouse reported as being
99% efficient, or passing only 1% of the material, the actual emission may
vary from 0.5 to perhaps 270 because it is frequently difficult to make low-
level measurements with accuracy. In such a case, the resulting emission
data could be in error by a factor of 2.
Unless otherwise specified, it is assumed that the reported
overall level of particulate control applies equally to all titanium-
containing particles, independent of size, resistance and other important
collection parameters. This assumption results in a correct estimate of
titanium emissions after control when the particulate is chemically homo-
genious, i.e., titanium is contained in the same concentration in all par-
ticles. If however, titanium is concentrated in certain particles and in
addition, the efficiency of the control equipment is not uniform for all
particles, then the utilization of an average control level is less valid
for calculating titanium emissions after control. Data on the preferential
control of titanium-containing particles is seldom available, but is
included in this report when possible.
The accuracy of estimating the level of control for a
specific category is dependent on the quality of available data. The
investigators feel that, in general, the level of control data will con-
tribute an accuracy to the resulting emissions estimates within + 25
percent.
14
-------
6. Level of Metal Emissions After Control
The values in this column are derived by multiplying the
values in column 4 by the value (100 minus estimated level of control).
B. DEVELOPMENT OF EMISSIONS ESTIMATES - 1970
Estimates of particulate emissions to the atmosphere in 1970 in
the U.S. are developed in the following paragraphs and summarized in Table
1. Table 1 indicates that more titanium emissions result from operations
outside the titanium industry than from within the industry. The princi-
pal emissions estimates developed in Table 1 are summarized in Section C.
1. Mining and Beneficiation
No emission factors for the drilling, blasting, and loading
of titanium ore were found. A figure of 0.2 Ibs/ton emission developed in
(2~)
other hard-rock mining operations is used in place of direct data. On
the basis of 15 percent Ti09 in the rock and no control of the mining
(1)
emissions, the estimated release of titanium to the atmosphere is 30
tons per year. The Tahawas mine in New York, the only open pit mine in
the U.S., accounts for about one-third of the ilmenite mined in the U.S.
The remainder, produced by dredging, entails low emissions as it is largely
a wet process. A conservative emission factor of 25 percent of the factor
for the open pit mine was assumed.
Beneficiating operations are reported to involve the follow-
ing emission factors:
. crushing, screening, fines milling
recrushing & rescreening
. conveying, general screening and
handling
. drying.
An overall emission factor of 38 Ibs. of particulate per ton
of ilmenite produced (46% TK>2) is estimated from data provided by an
ilmenite producer. This factor, however, applies only to hard-rock
beneficiation. It is estimated that only about 25 percent as much emission
results from the beneficiation of dredged materials, as there are no
15
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crushing and screening operations as in the mining of hard rock. A 90 per-
cent level of emissions control was also assumed for these benef iciation
processes. The resulting estimated net emission to the atmosphere by
benef iciation is about 435 tons.
2. Metal Processing
a. Metal and Ingot Production
The major process involving titanium metal production
is the Kroll process which has two steps; the production of TiCl, using
the fluidized bed method, and the reduction of TiCl^ by Mg to form MgCl2
and Ti sponge. The sponge is then consolidated to form the solid metal.
The production of TiCl, is assumed to be well controlled as chlorine gas
would escape in large quantities if it were not. The reduction and con-
solidation steps are done under the protection of an inert atmosphere and
are also assumed to be clean.
b. Titanium-Base Alloys and Carbides
Titanium-base alloys are produced in an inert atmos-
phere and emissions are again assumed to be negligible.
c. Ferrotitanium
Figure 2 indicates that in the case of ferrosilicon
production, the greater the concentration of silicon the greater the
emission. Lacking better data, one can assume that the same data applies
to ferrotitanium production. Using the typical titanium content of 27
percent, an emission of 150 Ibs/ton is estimated. Of this, 27 percent
is assumed to be titanium, or 40 Ibs/ton, equivalent to 67 Ibs/ton of
Ti00- A production estimate of 5,872 tons in 1970 is based on the reported
(4)
consumption of ferrotitanium in steel production. This results in 200
tons before control, or 120 tons after an estimated 40 percent control.
d. Steel Production
Using the figure for total annual ferrotitanium use in
steel production and a weighted emission factor developed along with a
weighted level of control:
(4)
Tonnage of Ferrotitanium used in steel: 5,872
16
-------
Emission Factor: 25 Ibs. ferrotitanium emissions/
ton(5) ferrotitanium utilized
Level of control: 787=,
There results an estimated emission after control of only 7 tons.
S 500
400
5
2 £ 3OO
g
200h
100
7
10 .20 30 40 50 60 70 80 90 100
% iCOMPOSITION OF Si IN ALLOY
Figure 2. Emission of Particulate in Ferrosilicon
Production (Reference 3)
Little data is available on the titanium content of
particulate from the principal iron and steel processes. Open hearth
fumes are reported to contain 0.17 percent titanium; and electric furnace
fumes, 0.03 percent titanium. These data would produce estimates of
about 1000 and 9 tons of TiO? emission per year, respectively. These
estimates are not included in Table 1 because of the tentative and incom-
plete nature of the data, the other iron and steel processes being un-
represented. Further investigation of titanium emissions from these
sources is recommended.
e. Metal Fabrication
Atmospheric emissions are assumed to be negligible, as
all forging, casting, and joining of titanium is done under an inert
17
-------
atmosphere and most machining is done in the presence of a liquid coolant
which would capture most of the potential emissions.
3. Other Basic Processes
a. Welding Rod Coatings
This involves utilizing rutile in a wet slurry and
gradual drying to slowly remove the water without cracking the coating.
Titanium compound emissions are again assumed to be zero.
b. Ceramics
The mineral equivalent to approximately 370 tons of
TiO
u was used to opacify frit. Using an uncontrolled emission factor of
(3)
16 lbs/tonv , the total uncontrolled TiCL emission is estimated to be 3
tons. Using a conservative control estimate of 2/3 gives a controlled
emission estimate of 1 ton of TiO~.
c. Fiberglass
The major particulate emissions in fiberglass manu-
facture are from the glass melting oven. TiCL is added to already melted
glass in the oven. Generally no controls are used. Uncontrolled emission
factors are:
1 Ib/ton: recuperative heat exchanger
3 Ib/ton: regenerative heat exchanger^
An average factor of 2 Ibs/ton is assumed. Consumption figures of TiO,,
for fiberglass are not available, but it is assumed that 90 percent of
the "ceramics, fiberglass and other miscellaneous uses" category in
Figure 1 is for fiberglass, or approximately 27,000 tons TiO?. Estimated
TiO? emissions therefore are 27 tons.
d. Pigments Productions
Nearly all emission from pigment production is from the
calcining and subsequent grinding operations, and hence is practically 100
percent TiO,,. Of the two processes used in the production of titanium
pigment, the sulphate process contributes a little over half of the pro-
duction (52.5%). The essential difference in this process is the
18
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added step of calcining in producing Ti02> Reports of emissions tests of
titanium pigment calciners indicate 30 to 230 Ibs/ton before control, with
/Q\
an average of 150 Ibs/ton. ' The calciner controls reported average
about 97% efficiency.
The chloride process is closed up to this point, and
it is assumed that any par.ticulate1 emissions from the process are negligible.
Subsequently, the pigment from both processes; is ground, dried, and sacked.
The grinding operation is relatively closed, producing only 0.35 Ibs/ton
before control. ^ ' Because littl'e dust is generated, control measures
are limited to an estimated. 10 percent., resulting in an estimated 55 tons
of TiO» emission to the atmosphere. I"n:the spray drying process, it is
evident that all of the material is at one time an aerosol. Test reports
range from 90 to 99.9 percent control, a- range of two orders of magnitude
in the effect on emission, estimates.^ It is assumed here that 0.5 per-
cent of the product escapes- the control measures which are used on every
drier, resulting in an emission estimates of 3',275 tons. It is further
assumed that the sacking process is sufficiently integrated with the dryer
and its emission control equipment., that the above estimate applies to the
overall process.
e. Miscellaneous
TiO_ also finds, usea *'n artificial gem manufacture,
photographic plates, sky writing, and smoke screens. Only the last two
contribute any real emissions. These are such a small percentage of the
total they are neglected here.
4. Pigment Consumption
a. Paint, Varnish, Lacquer, and Ink
In the EPA emissions: manual, two processes involving
pigment use are paint and ink production. Both processes involve grinding
the pigment into the vehicle, and the emission estimates are identical.
There are no chemical reactions involved. Most of the emission is due to
handling the dry pigment, and is estimated at 0.5 to 1.0 percent of the
(3)
pigment used. At a rate of 0.75 percent (15 Ibs/ton) and a paint and
19
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ink pigment consumption of 384,.000 tons of Ti09,'the emission estimate
before control is 2880 tons. Control of the pigment handling processes
is estimated at 10 percent, resulting in a net'einission of 2600 tons.
b. Other Pigment Consumption
The other processes using pigments, indicated in Figure
1, are all basically similar to the above, i.e. all involve mixing a dry
pigment into a material to be colored. Using the same emission factor, a
consumption of 270,000 tons of TiO?, and an estimated control effective-
ness one half that for paint production because of the miscellaneous
nature of the processes, the net emission is estimated to be 1920 tons.
5. Inadvertent Sources
a. Coal Combustion
Coal consumption in 1970 amounted to about 517,000,000
(4)
tons. ' The particulate generated has been estimated at 33,800,000 tons,
of which 82% was controlled, leaving 6,100,000 tons of emission to the
atmosphere. Thus, even a small concentration of titanium in the coal
flyash would result in a large net emission of titanium. This concentra-
tion figure is reported to be 0.72 percent (= 1.27» TiO«) based on spectro-
(9)
chemical analyses of 373 different samples of coal from across the U.S.
The net estimated emission of titanium from this source is 73,000 tons of
Ti02 in 1970, the largest estimate in this study.
b. Coal Cleaning
Subsequent to mining, coal, is crushed, segregated,
washed, and dried, and in this last process emissions are estimated to be
about 300,000 tons per year. This is after control at an estimated 85
percent, resulting in a before-control emission estimate of about
2,000,000 tons per year. At a 10 percent ash content of coal and 1.2 per-
cent in Ti02 in the ash, this is equivalent to 360 tons of TiO- emitted
to the atmosphere.
c. Oil Combustion
There are traces of titanium in residential and commer-
cial grade fuels, .004 percent according to "Emissions from Fuel Oil
20
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Combustion", and 0.03% in residual utilities fuels, according to the
(1
same source.
respectively.
same source. These are equivalent to .0065 and .05% Ti09,
Emission figures have been developed for fuel oil burn-
ing. Emissions from residual, industrial and electric utilities amount to
123,000 tons while emissions from residential and commercial use are
(2)
146,000 tons. Both sources are uncontrolled, resulting in emissions of
62 and 10 tons of TiCL, respectively.
d. Inc inerat ion
The fly ash from, typical municiple incinerators contains
a great deal of mineral particulate matter of which an estimated 4.2% is
Ti07. Total estimated mineral, particulate emissions from incinerators
(12)
in 1970 was about 100,000 tons.. ' According to the same source, total
mineral particulate emissions from incinerator stacks was about 63,000
tons, indicating 37% control. This results in an estimated 2,650 tons of
TiO» released by incineration.
e. Non-metallic Mineral Production
Emissions after control equipment have been estimated as
follows for a variety of major U.S. industries.
Crushed stone (about 0.5%) 4.6x10 TPY
Cement 0,9xl06 TPY
Lime 0.6xl06 TPY
Clay O.SxlO6 TPY
Fertilizers 0.3x10 TPY
Total 6.9xl06 TPY
No analyses of these particulates for titanium content were found except
tver
(13)
in the case of cement, which was approximately 0.01 percent. However
the earth's crust is reported to contain about 0.44 percent titanium.
Applying these percentages to the total emission above results in an
estimated t itanium emission range of 690 to 30,000 tons per year. Table 1
includes a token emission of 3,000 tons of TiO_, with an accompanying
indication that the estimate is a weak one needing further investigation.
21
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C. SUMMARY OF PRINCIPAL EMISSIONS
Table 2 summarizes the major sources and estimated emissions of
titanium, as developed in Table 1 and the accompanying discussion. The
sources are grouped in two categories, those directly originating with
the industries using titanium as a material; and inadvertent sources.
The latter category is by far the larger, due to the small but significant
amount of titanium contained in domestic coals.
TABLE 2
SUMMARY OF PRINCIPAL SOURCES AND EMISSIONS - TITANIUM
Inadvertent Sources
Coal Burning
Non-Metallic Minerals
Incineration
Titanium Industry Sources
Pigment consumption
Pigment production
Benef iciation of ore
U.S. Tons/Year of Equiv. TiO^
-— •• - — - - - - f_
73,000
(3,000 est.)
2,650
4,520
4,080
465
% of U.S.
82.6
3.4
3.0
5.1
4.6
0.5
99.2
22
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IV. REGIONAL DISTRIBUTION OF PRINCIPAL SOURCES AND EMISSIONS
For purpose of showing geographical distribution, the U. S. was divided
into ten regions identical to the Regional Branches of EPA:
Connecticut, Maine, Massachusetts, New Hampshire,
Rhode Island, Vermont
II New Jersey, New York, Puerto Rico, Virgin Island
III Delaware, Maryland, Pennsylvania, Virginia, West
Virginia, District of Columbia
IV Alabama, Florida, Georgia, Kentucky, Mississippi,
North Carolina, South Carolina, Tennessee
V Illinois, Indiana, Michigan, Minnesota, Ohio,
Wisconsin
VI Arkansas, Louisiana, New Mexico, Oklahoma, Texas
VII Iowa, Kansas, Missouri, Nebraska
VIII Colorado, Montana, North Dakota, South Dakota,
Utah, Wyoming
IX Arizona, Caifornia, Nevada, Hawaii, and the South
Pacific
X Alaska, Idaho, Oregon, Washington
Emissions from the principal sources listed in Table 2 are distributed
among these ten regions, as shown in Table 3. Also the number of plants
producing the emissions is shown in the table when such information was
available.
The accuracy of the distributions by region varies with the category.
The number of plants per category ranged from one to several thousand in
this study. When the number of plants was less than 100, an attempt
was made to identify each plant and plant location, and include it in one
of the ten regions. When production or capacity figures for these plants
were available, total production or capacity for each region was computed,
and the U. S. emission estimate for that category was distributed by region
accordingly. When production or capacity figures were not available, the
emission was distributed by the number of plants in each region. If the
23
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TABLE 3
REGIONAL DISTRIBUTION OF PRINCIPAL SOURCES AND EMISSIONS
Principal Sources
Inadvertent Sources
Coal burning
Non-metallic minerals
Incineration
Titanium Industry Sources
Pigment
Pigment production
Benef iciation of ore
Totals
EPA Region
1
0.7
510
5.8
174
16.6
440
0
0
0
0
0
0
1124
1 .1
2
5.7
4160
12.5
375
24.2
640
27
1220
3
1100
2
349
7844
8.9
3
21.7
15840
11.5
345
17.7
470
28
1270
6
1220
1
29
19174
21.6
4
21.0
15330
15.7
470
11.8
312
23
1040
3
840
3
87
1807<9
20.5
5
41.1
30000
21.6
650
24.0
635
5.4
245
3
200
0
0
31730
35.8
6
_LA
1020
10.0
300
3.5
93
0
0
0
0
0
0
1413
I. fa
7
4.1
3000
5.5
165
1.4
37
13.3
600
1
610
0
0
4412
5.0
8
3.3
2410
2.7
81
0.3
8
0
0
0
0
0
0
2499
2.8
9
0.7
510
11.3
340
0.5
11
3.3
150
1
110
0
0
1121
1.3
10
0.3
220
3.2
96
0
0
0
0
0
0
0
0
316
0.4
Total (units) Reference
100% (Coal shipped) (4) '
73,000 (TPYO
100% (Population) (14)
. (3,000) (TPY)
100% (Incin. Capacity) (12)
2,650 (TPY)
100% (Pigment Production) (1 5)
4,520 (TPY)
17 (Flants) C1.5>
. 4,080 (TPY)
6 (Plants) (4)
465 (TPY)
87,715 (TPY)*
99.2 (% of U.S.)
Tons per year, TiO,, emitted to the atmosphere
-------
number of plants was very small or there was reason to believe that certain
plants were larger or produced more emission, distributions were weighted
accordingly.
On the other hand, when the estimated number of plants was greater
than about 100, and the distribution of plants was not known, the regional
breakdown was made on a different basis, such as population, geographical
area, or shipments reported, as most appropriate for that category. Whether
the distribution was by plant size, number of plants, or another statistic,
the distribution is believed to be accurate to within 10 percent in most
cases.
The basis for the Table 3 distribution of the inadvertent (i.e.
non-titanium industry) sources is: coal combustion, according to shipments
of coal by states of destination; non-metallic production, by population;
and incineration, by reported incinerator capacities per state. As
discussed earlier, the estimate for non-metallic mineral production is weak
and needs further investigation.
Titanium industry emission sources are distributed as follows:
emissions from pigment production are distributed
by region, according to the reported total plant
capacity in that region.(15)
Region: 123 4 56 789 10 Total (TPY)
Sulphate Capacity: 0 133 164 46-12 0 108 0 0 0 463,000
Chloride Capacity: 0 87 68 144 32 0 0 0 27 0 358,000
821,000 (TPY)
Due to a lack of capacity data, emissions from the five bene-
ficiation plants which produce ilmenite from beach sands were
all assumed to be equal; i.e., 146 -r 5 = 29 tons/year.
There is only one open pit ilmenite mine in the U. S., in Tahawas,
New York, and so all emissions from open pit mining were allocated
to Region 2.
. Pigment consumption is assumed to be distributed according to pigment
production, because the largest fraction of the pigment consumed is for
paint, and most of the companies producing the pigment are paint
companies. It is in effect assumed that the consumers of pigment
for other than paint uses are located near the pigment producers.
25
-------
The overall distribution by region is also shown in Table 3, with
Region 5 estimated to produce the most emissions of titanium followed by
Regions 3 and 4. These are the coal consuming regions of the U. S.
Table 3 is strongly weighted by the single emission from coal combustion,
in the absence of which, Region 2 would be first with the most emission.
Considering the geographical areas of these regions, Region 3 pro-
duces the most emission per square mile (0.16 tons per square mile-year)
followed closely by Region 2.
26
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V. NATURE OF EMISSIONS
The emissions of titanium and titanium dioxide are largely dependent
on their properties, shown in Table 4.
TABLE 4
PHYSICAL PROPERTIES OF Ti and TI02*
Tl
Melting Point 1668°C 1640°C
Boiling Point 3260°C 2700°C
Density 4.51 g/cc 4.2 g/cc
Atomic Weight 47.9 a.w.u. 79.9 a.w.u.
Heat of Vaporization 106.5 kg-cal/g-atom ----
Mineral hardness, ILMENITE: 5.5, std. minerology scale. («FeO-Ti02).
Probably the most important property from the emissions standpoint is the
boiling, or vaporization point, which is substantially higher than the
combustion temperatures of coal or incinerator refuse. This indicates that
the emission in both cases probably has the same physical and chemical form
as the feed material. In fact, this is probably true of nearly all the
principal emissions discussed above.
Beneficiating and non-metallic mineral operations involve mechanical
pulverization and in this type of process the hardness of the material
affects the fineness of any particles produced. Because ilmenite is a
moderately hard material, the pulverization must be an intense process pro-
ducing a moderate amount of fine particles. Hard-rock mining of ilmenite
is estimated to produce particles of 5 micrometers average diameter, ranging
from 1/2 to 10 micrometers. ' The upper size limit is a strong function
of the distance from the source.
Pigment handling processes, including incineration of paper containing
titanium oxide pigment coatings, will produce emissions of TiO^ particles
- (16)
* Perry's Chemical Engineers Handbook, 4th Edition, Table 3-169.
27
-------
somewhat dependent on the particle size. One pigment manufacturer estimated
for this study that the pigment produced is 0.1 to 1.0 micrometer in diameter,
with an average diameter of I/A micrometers. Another estimate gives nearly
all particles being under 0.2 micrometers, with about 2 percent ranging up to
0.40 micrometers. The size of the pigments produced varies with the
market.
Fine particles, those 1 micrometer diameter and smaller, may be
expected to travel considerable distances before being deposited or beine
washed out of the air by natural processes. About 9.8 percent of the total
U.S. emission of TiO» is as pigments most of which is in particles smaller
than 1 micrometer. Thus the emissions of pigment probably contribute to the
average ambient titanium concentration in the U.S. In addition, the combus-
tion of distillate oils, and of gasoline (.01 to 0.1 ppm Ti content)^ ' which
produce more finely divided particulate, may influence background air
quality despite the smaller total mass emitted.
There is no reason to suspect any unusual activity of titanium-
containing particles following emission, including agglomeration or chemical
reaction with atmospheric components in the cases of some particulate. It
appears that TiO« is a relatively stable and unreactive material in all
respects.
Ti09 has recently been approved as a food additive by the Food and
Drug Administration, and has been used for some time as a cosmetic. Its
common use as abrightener of domestic papers is further indication that
TiO? is considered not harmful.
28
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VI. UPDATING OF EMISSIONS ESTIMATES
The following recommendations are made for periodically updating the
estimates made in this study:
A. VERIFICATION OF CURRENT ESTIMATES
1. Verify that the fraction of titanium contained in
flyash from stacks of coal combustion plants is
essentially unchanged from the fraction contained
in coal ash produced in laboratory analyses of coal
(9)
samples. There is no reason to suspect any sub-
stantial change. However, the assumption that
there is no change has strong bearing on the con-
clusions of this program.
2. Determine a better average titanium concentration
for the emissions generated.by the non-metallic
minerals industry, in particular from crushed stone.
3. Verify the relatively low emissions control prac-
tices of the pigment producing and consumption
industries, and of the ilmenite beneficiating
plants.
B. PERIODIC REVIEW OF ESTIMATES
1. The Bureau of Mines estimates for material flow,
industry practices, and trends provide the best
estimates of the size of the industry.
2. EPA activities are currently generating the best
emissions data and should be reviewed:
a. Overall industry studies, e.g. References (19).
b. The Source Test Program, in which specific
individual plant emissions are measured.
This information provides emission factors
29
-------
for specific examples of typical industry
operations, and also provides some analyses
of the particulate usually including trace
metal content and particle size.
c. NEDS (National Emissions Data System) is
steadily being enlarged and improved. This
system can provide emission factors for
specific plants and plant operations, the
type of particulate control equipment in use,
and the actual, or estimated, control effic-
iency. The system may eventually be expanded
to include description of the emissions.
3. The titanium industry should be consulted for its
opinion and suggestions on the most recently published
estimates. This may be best accomplished by interviewing
the Titanium Commodity Specialist, Division of Non-
ferrous Metals, Bureau of Mines in Washington; or,
interviewing one or more of the principal companies
in the industry.
4. Literature should be reviewed, using (a) industrial
views as published from time to time in Chemical
Engineering, for example, and (b) environmental views
as summarized in Pollution Abstracts, for example.
5. Individual companies or plants may be approached for
opinions, data, or cooperative tests of their own
operations, it is difficult to obtain fresh information
in this way, due to the natural reluctance of plants to
discuss environmental problems. However, data thus
obtained have a relatively high degree of reliability.
6. State agencies in which specific plants are located
may be able to provide useful information } and should
be contacted.
30
-------
VII. REFERENCES
1. Personal communication with members of the titanium industry.
2. Davis, W.E., National Inventory of Sources and Emissions; Barium,
Boron, Copper, and Zinc, Section III, Copper, Report EPA Office
of Air Programs Contract No. 68-02-0100, April, 1972.
3. Compilation of Air Pollutant Emission Factors. E.P.A., February
1972.
4. Minerals Yearbook. 1969, Vol. I-II, Bureau of Mines, 1971. Also,
Noe, Frank E., Minerals Yearbook, 1970, Reprint, Titanium,
Washington, Bureau of Mines, 1972.
5. Vandergrift, A.E., et al., Particulate Pollutant System Study,
Volume III, Handbook of Emission Properties, May 1971.
6. EPA Source Test Reports. From analysis of selected test reports,
emission factors and/or particulate analyses data were obtained to
supplement the data found in the literature.
7. Dammartino, Nicholas R., Troubled Times for TiO?, Chemical Engineer-
ing, May 1, 1972.
8. NEDS (National Emissions Data System) information, furnished by
EPA to supplement literature information.
9. Abernathy, R.F., et. al., Major Ash Constituents in U.S. Coals,
Bureau of Mines, U.S. Dept. of the Interior, Dept. of Investigation
No. 7240, 1969.
10. Smith, Walter S., Atmospheric Emissions from Fuel Oil Combustion,
November 1962.
11. Proceedings of 1970 National Incineration Conference, A.S.M.E.,
1970.
12. Arthur D. Little, Inc., Cambridge, Mass., Systems Study of Air
Pollution from Municipal Incinerators, 1970.
13. Fairbridge, R.W., ed., The Encyclopedia of Geochemistry and
Environmental Sciences Series, Vol. IVA, Van Nostrand Reinhold Co.,
N.Y., 1972.
14. U.S. Bureau of Census, Statistical Abstracts of the U.S., 1970.
15. U.S. Dept. of the Interior, Federal Water Pollution Control
Administration, The Economics of Clean Water, Contract No. 14-12-595,
March 1970.
16. Perry, R.H., et. al., Perry's Chemical Engineers Handbook, 4th
Edition, McGraw Hill, Inc., New York, 1963.
17. Remington, J.S., and Francis, W., Pigments: Their Manufacture,
Properties, and Use, Leonard Hill Limited, London, 1954.
31
-------
18. Lehtnden, D.J., Jungers, R^H., and Lee, R.E., The. Determination of
Trace Elements in Coal, Fly Ash, Fuel Oil, and Gasoline, Part I,
presented at- the.Ami. Chemical Soc. Mtg., Dallas,, Texas, April,
1973.
19. Poole, W.K.,, and Johnson,. D.R.,. Estimating Population; Exposure to
Selected Metals- Titanium (Final Report)!Research Triangle inst.,
Research Triangle Park, N.C., NIEHS Contract No. PH-86-65-109,
RTIRpt. AU-229', Rept. NIH-ES-2434, 101P, March 1969.
32
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TECHNICAL REPORT DATA
(Please read Instructions on the reverse before completing)
1. REPORT NO. 2.
EPA-450/3-74-008
4. TITLE AND SUBTITLE
National Emissions Inventory of Sources
Emissions of Titanium
7. AUTHOR(S)
9. PERFORMING ORGANIZATION NAME AND ADDRESS
GCA Corporation
GCA Technology Division
Bedford, Massachusetts 01730
12. SPONSORING AGENCY NAME AND ADDRESS
Environmental Protection Agency
Research Triangle Park, N. C. 27711
3. RECIPIENT'S ACCESSION-NO.
5. REPORT DATE
and May 1973
Ullu 6. PERFORMING ORGANIZATION CODE
8. PERFORMING ORGANIZATION REPORT
NO.
10. PROGRAM ELEMENT NO.
2AE132
11. CONTRACT/GRANT NO.
68-02-0601
13. TYPE OF REPORT AND PERIOD COVERED
Final
14. SPONSORING AGENCY CODE
15. SUPPLEMENTARY NOTES
16. ABSTRACT
A national inventory of the sources and emissions of the element titanium
was conducted. All major sources of titanium-containing emissions were identified
and their titanium emissions into the atmosphere estimated. Also, a method for
updating the results of the study every two years was recommended.
17. KEY WORDS AND DOCUMENT ANALYSIS
a. DESCRIPTORS
Titanium
Air Pollution
Emission
Inventories
Sources
18. DISTRIBUTION STATEMENT
Release Unlimited
b.lDENTIFIERS/OPEN ENDED TERMS
19. SECURITY CLASS (This Report)
Unclassified
20. SECURITY CLASS (This page)
Unclassified
c. COSATI Field/Group
21. NO. OF PAGES
32
22. PRICE
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