APTD-1507
NATIONAL INVENTORY
OF SOURCES
AND EMISSIONS:
ARSENIC - 1968
U.S. ENVIRONMENTAL PROTECTION AGENCY
Office of Air and Water Programs
Office of Air Quality Planning and Standards
esearch Triangle Park, North Carolina 27711
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APTD-1507
NATIONAL INVENTORY
OF
SOURCES AND EMISSIONS:
ARSENIC • 1968
by
W. E. Davis § Associates
9726 Sagamore Road
Leawood, Kansas
Contract No. CPA-70-128
EPA Project Officer: C. V. Spongier
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 1971
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The APTD (Air Pollution Technical Data) series of reports is issued by
the Office of Air Quality Planning and Standards, Office of Air and
Water Programs, Environmental Protection Agency, to report technical
data of interest to a limited number of readers. Copies of APTD reports
are available free of charge to Federal employees, current contractors
and grantees, and non-profit organizations - as supplies permit - from
the Air Pollution Technical Information Center, Environmental Protection
Agency, Research Triangle Park, North Carolina 27711 or may be obtained,
for a nominal cost, from the National Technical Information Service,
5285 Port Royal Road, Springfield, Virginia 22151.
This report was furnished to the Environmental Protection Agency
in fulfillment of Contract No. CPA-70-128. The contents of this report
are reproduced herein as received from the contractor. The opinions,
findings, and conclusions expressed are those of the author and not
necessarily those of the Environmental Protection Agency. The report
contains some information such as estimates of emission factors and
emission inventories which by no means are representative of a high
degree of accuracy. References to this report should acknowledge the
fact that these values are estimates only.
Publication No. APTD-1507
11
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PREFACE
This report was prepared by W. E. Davis & Associates
pursuant to Contract No. CPA 70-128 with the Environmental
Protection Agency, Air Pollution Control Office.
The inventory of atmospheric emissions has been prepared to
provide reliable information regarding the nature, magnitude,
and extent of the emissions of arsenic in the United States for
the year 1968.
Background information concerning the basic characteristics
of the arsenic industry has been assembled and included. Pro-
cess descriptions are given, but they are brief, and are limited
to the areas that are closely related to existing or potential
atmospheric emissions of the pollutant.
Due to the limitation of time and funds allotted for the study,
the plan was to personally contact about twenty to thirty percent
of the companies in each major emission source group to obtain
the desired information. It was known that published data con-
cerning emissions of the pollutant was virtually nonexistent,
and numerous contacts with industry during the study ascer-
tained that atmospheric emissions were not a matter of record.
111
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The arsenic emissions and emission factors presented herein
are based on the summation of information obtained from the
one processing company that produced arsenic during 1968, the
copper, lead, and zinc smelters, and the reprocessing com-
panies that handle about fifty percent of the arsenic consumed
in the United States. Arsenic emissions and emission factors
are considered to be reasonably accurate.
IV
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ACKNOWLEDGEMENTS
This was an industry oriented study and the authors express
their appreciation to the many companies and individuals that
contributed information related to the atmospheric emissions
of arsenic.
We wish to express our gratitude for the assistance of the
various societies and associations, and to the many branches
of the Federal and State Governments.
Our express thanks to Mr. C. V. Spangler, Project Officer,
Environmental Protection Agency, Air Pollution Control
Office, for his helpful guidance.
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CONTENTS
SUMMARY
Emissions by Source 2
Emissions by Region 3
Map of Emission Regions 4
Emission Factors 5
SOURCES OF ARSENIC 6
MATERIAL FLOW
Material Flow Chart 8
Mining and Processing 9
Arsenic Imports 10
Consumptive Uses 11
Agricultural 11
Glass Manufacture 13
Wood Preservatives 13
Nonferrous Alloys 13
Other 14
EMISSIONS
Mining and Processing 16
Metallurgical Processing 17
Reprocessing 27
Agricultural 27
Glass Manufacture 29
Wood Preservatives 32
Nonferrous Alloys 33
Other 35
Consumptive Uses 37
Agricultural 37
Coal 41
Oil , 43
Detergents 44
Phosphoric Acid 44
Vil
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Incineration and Other Disposal 47
Sewage and Sludge 47
Iron and Steel 48
APPENDIX A
Companies Dealing in Arsenic and
Arsenic Compounds 50
TABLES
Table I
Arsenic Contamination in a Western
Mining Community 23
Table II
Concentration of Arsenic Near a Copper Mine
in Northern Chile 24
Table III
Suspended Particulate and Arsenic Concentra-
tions in the Air near Cotton Gins in
West Texas 39
Table IV
Average Arsenic Content of Coal Ash 42
Table V
Concentrations of Arsenic in Certain
Detergents and Presoaks 4.6
Vlll
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SUMMARY
The production and use of arsenic in the United States has been
traced and charted for the year 1968. The total consumption
of 28, 000 tons was used as follows: 72 percent by imports
(20, 000 tons), and 28 percent by domestic producers (8, 000 tons).
During the year emissions from metallurgical processing plants
of the primary producers of copper, lead, and zinc were 4,466
tons, and those due to the use of pesticides were 3, 270 tons.
These two emission sources combined account for 82 percent
of the 9,415 tons total emissions.
Arsenic emissions to the atmosphere can be reduced. A decrease
in imports, coupled with an increase in domestic production.,
would result in less emissions. Many nonferrous smelters cur-
rently process ores that contain significant quantities of arsenic.
With a sufficient economic incentive, some would recover the
element rather than treating it as an unwanted by-product.
Emission estimates for processing and reprocessing ope.-atic.ns
are considered to be reasonably accurate. They are based on
estimates obtained through personal contact with the processing
and reprocessing cpmpanies, and on engineering calculations sup-
ported »y data covering smelter gas flow rates and temperatures.
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Source Category
Mining
Metallurgical
Processing
EMISSIONS BY SOURCE
1968
Source Group
Reprocessing
Consumptive Uses
Incineration and
Other Disposal
Copper Smelters
Zinc Smelters
Lead Smelters
Agricultural
Glass
Wood Preservatives
Nonferrous Alloys
Other
Agricultural
Coal.
Oil
Cast Iron
TOTAL,
N - Negligible (less than 1 ton)
NA - Not Available
Short Tons
2,700
1,390
376
196
638
N
N
3
3,270
743
NA
97
4,466
837
4,013
97
9,415
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Region No. 1
Region No. 2
Region No. 3
Region No. 4
Undistributed
EMISSIONS BY REGION
Number of Smelters
22
4
8
2
Short Tons
3,829
1,317
2,313
1,020
936
TOTAL
9,415
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MAP OF EMISSION REGIONS
PLANT LOCATIONS
+ Arsenic
• Copper
O Lead
<>- Zinc
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EMISSION FACTORS
Mining
Metallurgical Processing
Copper Smelters
Zinc Smelters
Lead Smelters
Reprocessing
Agricultural
Glass
Other
Consumptive Uses
Agricultural
Cotton Gin
Burning Cotton
Gin Trash
Coal
Incineration and Other
Disposal
Cast Iron
0. 2 Ib/ton of arsenic in ore
4. 9 Ib/ton of copper
1. 3 Ib/ton of zinc
0.8 Ib/ton of lead
20 Ib/ton of arsenic used
232 Ib/ton of arsenic used
3 Ib/ton of arsenic used
336. 0 Ib/ton of arsenic used
3. 5 lb/1, 000 bales of cotton ginned
17. 0 lb/1, 000 bales of cotton gir.ned
2. 9 lb/1, 000 tons of coal burned
11 lb/1, 000 tons of metal charged
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SOURCES OF ARSENIC
Arsenic is not an abundant .element, but it is widely distributed
in the earth's crust. Traces of it can be found almost every-
where. It is present in sea water, in coal deposits, and in vir-
gin soils as well as in various ores. The most extensive occur-
ence is with copper, lead, cobalt, nickel, iron, gold, and silver.
Arsenic is generally regarded as a contaminant in the ore and
must be removed during smelting and refining in order to im-
prove the quality of the metal. During 1968 it was produced com-
mercially only at one location in the United States. At many
other locations it was an unwanted by-product. One of the prob-
lems facing the mining industry has been the disposal of large
quantities of crude arsenic produced while purifying other metals.
In the United States arsenic occurs in many ores of ferrous
metals and nonferrous base metals. Gold and silver ores are
often associated with arsenic and contain large reserves of ar-
senic /. Copper ores in Arizona usually contain a small amount
of arsenic, while ores in many other western states contain con-
siderably more. Often lead, copper, and gold ores contair. as
1- Mineral Facts and Problems; U. S. Bureau of Mines; 1965.
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much as 2 or 3 percent arsenic and in a few instances, as much
as 10 or 12 percent.
Copper, lead, and zinc ores and concentrates which are im-
ported and processed in the United States also contain arsenic.
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ARSENIC
MATERIAL, FLOW CHART - 1968
Short Tons - Arsenic (As)
SOURCES
8, OOP
PRODUCER SHIPMENTS
20.000
28,000
IMPORTS
USES
19.500
AGRICULTURAL
5. 500
GLASS MANUFACTURE
4.00
WOOD PRESERVATIVES
400
NONFERROUS ALLOYS
2.200
MISCELLANEOUS
QO
I
CONSUMER
Figure II
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MATERIAL FLOW
MINING AND PROCESSING
During 1968 arsenic was produced commercially in the United
States only at the American Smelting and Refining Company
copper smelter in Tacoma, Washington _/. It was produced as
a by-product of copper smelting not only from copper ores and
concentrates, but also from speiss, flue dust, and sludges re-
ceived from other smelting plants.
Arsenic produced domestically and shipped from producer stocks
daring 1968 totaled about 8,000 tons (As content) _/. It was
produced as arsenic trioxide or arsenious oxide (As,O.), which
^ 3
is often referred to as white arsenic.
1- Minerals Yearbook; Bureau of Mines; 1968.
2- An estimate based on information in the Bureau of Mines
Minerals Yearbooks, 1958 through 1968.
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ARSENIC IMPORTS
During 1968 arsenic imports totaled 20, 000 tons (As content),
consisting principally of white arsenic and metallic arsenic /.
About 37 percent of the white arsenic was imported from
Sweden, 29 percent from Mexico, and 25 percent from France.
Sweden was the major supplier of metallic arsenic.
1- Minerals Yearbook; Bureau of Mines; 1968.
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CONSUMPTIVE USES
The apparent consumption of arsenic in the United States during
1968 has been estimated at Z8, 000 tons (As content) *J.
Arsenic is produced principally in the oxide form (white arsenic)
and used extensively in the manufacture of calcium arsenate and
lead arsenate; smaller quantities are also used in sodium arsen-
ite, sodium arsenate, arsenic acid, and other compounds. Ar-
senic is used primarily for its toxic effect on plants and insects.
It is used to a lesser extent in glassmaking, nonferrous alloys,
wood preservatives, and for numerous miscellaneous purposes.
AGRICULTURAL
During recent years about 70 to 80 percent of the arsenic con-
sumed in the United States has been used in the manufacture of
pesticides, including herbicides, defoliants, fungicides, and in-
secticides. Various forms of arsenic used in these materials
include: calcium and lead arsenate, calcium and zinc arsenite,
arsenic acid, cacodylic acid, and arsenic trioxide (white ar-
senic).
1- Estimated tonnage is based on imports reported in the
Bureau of Mines Minerals Yearbook, 1968, plus estimated
producer shipments.
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Herbicides are used principally to control weed growth. Cal-
cium, sodium and zinc arsenites, plus some organic arsenicals,
are used for this purpose and are usually applied in the form of
a water solution.
The major use of defoliants and desiccants in the United States
is for treatment of cotton prior to machine picking. The prod-
uct most used for this purpose is arsenic acid. Another defoli-
ant is cacodylic acid, but due to higher cost it is consumed in
smaller quantities.
Another important area for use of arsenic is in insecticides.
The most common arsenate products used for this purpose are
calcium and lead arsenate. These may be used either as sprays
or dusting materials which are applied to orchards, gardens,
berries, ornamentals, and field crops in a form that will not in-
jure plants, but chewing insects are destroyed when they eat
leaves which have been treated with the arsenic-containing
sprays or dusting preparations.
It is estimated that 19, 500 tons of arsenic were used for agri-
cultural purposes in the United States during 1968 /.
1- Private communication with the U. S. Bureau of Mines,
Washington, D. C.
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GLASS MANUFACTURE
Arsenic trioxide (As^O-), arsenic hemiselenide (As^Se), ar-
senic pentoxide (As2O_), and arsenic trisulfide (As^S ) are
used in the manufacture of glass.
Approximately 5, 500 tons of arsenic were used in the manufac-
ture of glass during 1968 _/.
WOOD PRESERVATIVES
Various arsenic compounds are used extensively as wood pre-
servatives either alone, or mixed with other substances. Such
compounds include arsenic trioxide, chemonite, ammoniacal
copper arsenite, and chromated copper arsenate.
Arsenic used in wood preservatives in the United States during
1968 totaled approximately 400 tons _/.
NONFERROUS ALLOYS
Arsenic in small, amounts is added to some copper and lead al-
loys to improve corrosion a.nd erosion resistance, raise the
annealing temperature, change the surface tension, harden the
1- Private communication with the U. S. Bureau of Mines,
Washington, D. C.
2- Minerals Yearbook; Bureau of Mines; 1968.
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alloy, or otherwise alter the characteristics of the metal to
make it suitable for certain special purposes.
It is estimated that 400 tons of arsenic were used in nonferrous
alloys in the United States during 1968 _V.
OTHER
Small quantities of arsenic are used in cattle and sheep dips,
pyrotechnics, pigments, semiconductors, poultry feed additives,
Pharmaceuticals, and in treating hides and skins.
Sodium arsenite is the active ingredient in certain cattle and
sheep dips. It is also used to a limited extent for termite control.
Arsenic disulfide and arsenic trisulfide are found in nature but
ordinarily are made artificially. They are used in paint pig-
ments and pyrotechnics. Arsenic disulfide is also used as a de-
pilatory in tanning. Arsenic pentasulfide has a limited use in
paint pigments and pyrotechnics.
There is limited demand for arsenic of extremely high purity
(99.999%) for use as a semiconductor.
1- Private communication with the U. S. Bureau of Mir.es,
Washington, D. C.
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In the past arsenic compounds have been used rather extensively
in medicine, but today the applications are limited. Less than
one percent of the annual arsenic supply is used in pharmaceuti-
cal preparations.
During 1968 the estimated uses of arsenic in this category totaled
2, 200 tons.
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EMISSIONS
MINING AND PROCESSING
Since no ore in the United States is mined solely for the recovery
of arsenic, the emissions to the atmosphere resulting from min™
ing operations are those that occur during the mining and concen-
tration of copper, lead, and other ores that contain arsenic.
Regardless of the type of mine (underground or open-pit), the
mining operations are basically the same: ore removal, ore hand-
ling, crushing, grinding, and concentration. During many of the
operations the ore is wet and emissions to the atmosphere are
virtually nonexistent. The principal emission appears to be that
due to wind loss from tailings.
Arsenic emissions to the atmosphere from sources of mining are
estimated at 0.2 pounds per ton of arsenic handled. This gives a
total figure of approximately 2 tons of arsenic emitted to the at-
mosphere during 1968.
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METALLURGICAL PROCESSING
During 1968 arsenic for the commercial market was produced
at only one location in the United States. It was recovered as
arsenic trioxide from dusts and residues as well as from for-
eign and domestic copper ores and concentrates.
Since most of the arsenic produced is in the form of arsenic tri-
oxide (As-O,) as a by-product of the smelting of other metals,
the production of arsenic is closely associated with the recovery
and treatment of arsenic-bearing flue dusts. As arsenic trioxide
is volatilized during the smelting of copper, lead, zinc, and other
metals, it is concentrated in the flue dust. The crude flue dust
carrying up to 30 percent arsenic trioxide also contains oxides
of copper or lead, and perhaps other metals such as antimony,
zinc, and cadmium.
The crude flue dust recovered during the smelting operation is
further refined by mixing it with a small quantity of pyrite or
galena concentrate prior to roasting. The pyrite or galena pre-
vents the formation of arsenites during roasting, and produces
a clinkered residue suitable for return to the process for recov-
ery of other metals. The gases from roasting are passed
through a series of brick chambers or kitchens, in which the
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temperature varies from 430 F in the first, to 210 F or less in
the last. As the gases cool, arsenic trioxide condenses as a
crude white arsenic, 90 to 95 percent pure. Much of the product
is used in this form without further refinement.
If higher purity is required, the refining is usually carried out
in a reverberatory furnace at a roasting temperature of about
1, 000 F. The vapors first pass through a settling chamber and
then through a series of kitchens. In the settling chamber, the
temperature is maintained above the condensation temperature
of the trioxide. In the kitchens near the furnace a black, amor-
phous mass is condensed which contains about 95 percent arsenic
trioxide. This product is reprocessed. The bulk of the trioxide
is condensed in the other kitchens at temperatures ranging from
250 to 360 F, and most of the dust which exits from the kitchens
is caught in a baghouse. Some of the arsenic escapes; all that
is in the vapor phase, plus a relatively small amount of the dust.
A flowsheet (Figure III) shows the basic steps for production of
arsenic trioxide'at a copper smelter /.
1- Kirk, R. E. and Othmer, D. F. ; Encyclopedia of Chemical
Technology; 2nd Ed. ; Inter science Publishers; New York,
N. Y.; 1963.
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ARSENIC FLOW SHEET
COPPER SMELTER
ROASTER
if
iTORY
CONVERTER
Dust-laden
vapor & gases
Low
arsenic
and
valuable
residue
EXPANSION
CHAMBER
WASTE HEAT
BOILER
BAGHOUSE
COTTRELL
PRECIPITATOR
Fumes
and
dust
ROASTER
High
arsenic
fumes
Valuable
residue
REVERBERATORY
SO2
[to be conveited to
and waste gases
to stark
White arsenic
for market
Figure III
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One of the big problems facing the mining industry has been the
disposal of large quantities of arsenic contained in various ores
mined and processed. The quantity of arsenic available has
greatly exceeded the demand; therefore, most smelters have not
attempted to produce arsenic for the commercial market. There
is no economic incentive to remove it from the flue gas.
At many smelters no attempt is made to controlarsenic emis-
sions, but at others some method of control is required. If the
arsenic content of the ore is low, as it is in copper ores in Ari-
zona, likely there will be no control. The arsenic retained in
the copper product will be within commercial limits and that dis-
charged in the slag and to the atmosphere will be relatively minor.
If the arsenic content of the ore is high, some method of control
is essential. In some instances the flue dust containing high con-
centrations of arsenic is removed from the smelting process at
regular intervals to prevent excessive arsenic build-up in the
system and in the product. Sometimes the flue dust is sold to a
smelter that produces arsenic, and sometimes it is dumped.
The following six examples demonstrate arsenic problems in
mining ore.
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1 - The Boliden Mining Company in Sweden is one of the world's
largest producers of arsenic. Arsenical gold ore containing 10
percent or more of arsenic is processed; the arsenic output is
sufficient to supply a large share of the world demand. At the be-
ginning of the Boliden operation it was realized that the arsenic
output would be far in excess of demand and that disposal would
be a major problem. First the excess crude arsenic was mixed
with cement, made into blocks, and dumped far out at sea. This
method of disposal proved to be rather expensive and an alter-
nate method was devised. A large concrete storehouse was
erected in 1931 and the crude arsenic was stored close at hand.
Since that time additional storehouses have been constructed as
required.
2 - At other locations the lack of adequate control has resulted
in harmful emissions to the atmosphere. During the years
1903 to 1905 large quantities of arsenic were emitted from a
copper smelter in Montana. The emission rate was reported
as 59,270 Ib/day when the ore processed was 10, 000 tons/day.
Large numbers of animals were killed up to fifteen miles from
the smelter due to eating plants contaminated with arsenic
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trioxide 1>2>3/.
3 - In Nevada a gold smelter was reopened in 1962, but within
five months it became apparent that the electrostatic precipita-
te r equipment was inadequate. Large quantities of arsenic tri-
oxide escaped into the atmosphere. If the dust-collecting system
had operated at 90 percent efficiency as intended, about 15,000
tons of crude arsenic trioxide would have been collected each
year. The analysis of dust samples from the area near the plant
are shown in Table I.
4 - After an air pollution episode at a copper mine in northern
Chile, samples of ore and dust were analyzed and reported as
shown in Table II.
5 - According to a report concerning another copper smelter in
South America, the arsenic in the ore is recovered as crude ar-
senic trioxide and dumped in the open on company property near
1- Harkins, W. D. and Swain, R. E. ; "The Determination of
Arsenic and Other Solids in Smelter Smoke"; J. Am. Chem.
Soc.; 29; p. 9.7.0; 1907.
2- Harkins, W. D. and Swain, R. E. ; "The Chronic Arsenical
Poisoning of Herbivorous Animals"; J. Am. Chem. Soc. ;
3£; p. 928; 1908.
3- Hay wood, J. K.; "Injury to Vegetation and Animal Life by
Smelter Fumes"; J. Am. Chem. Soc.; 29; p. 998; 19^07.
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TABLE I
ARSENIC CONTAMINATION IN
A WESTERN MINING COMMUNITY
Sample
Site
Arsenic
Concentratior
Flue Dust
Roof Dust
Dust
Dust
Dust
Base of stack
Shed near office
Area near drying mill
Roaster area
Sulfide-ore feed
44. 0%
4.4%
2.7%
3. 1%
1.23%
1- Birmingham, D. J., Key, M. M., Holaday, D. A., and
Perone, V. B. ; "An Outbreak of Arsenical Dermatosis in
a Mining Community"; Arch. Dermatol.; 91; p. 457; 1965.
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TABLE H
CONCENTRATION OF ARSENIC
NEAR A COPPER MINE IN NORTHERN CHILE */
Arsenic
" Concentration
Mineral (ore) 0.054%
Concentrated Ore 1.64%
Calcined Ore 0. 30%
Dust from Electrostatic Precipitator 10.36%
Dust from Stack 16. 64%
1- Oyanguren, H. and Parez, E. ; "Poisoning of Industrial
Origin in a Community"; Arch. Environ. Health; 13;
p. 185; 1966.
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the smelter. Based on material balance data and stack sample
analyses, the arsenic emission to the atmosphere is slightly
more than 8 percent. The concentrates contain 12 to 13 percent
copper and 2. 7 percent arsenic. The flue dust in the stack aver-
ages about 25 percent arsenic _/.
6 - One zinc smelter in the United States reported the average
arsenic content of zinc concentrates as approximately 0. 075 per-
cent. The estimated arsenic output from the smelter is as follows.
ARSENIC OUTPUT FROM A
ZINC SMELTER IN THE UNITED STATES
Output Percent
In Products 0. 3
In Saleable Residues 17. 6
In Dust 1.5
To the Atmosphere 80. 6
TOTAL 100.0
Arsenic emissions from copper, lead, and zinc smelters vary
considerably from plant to plant and from year to year. Ar-
senic emission factors for copper smelters range from one
1- Private communication; industrial source.
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pound to 53 pounds per ton of copper, and the average for 1968
was 4. 9. The average emission factor for zinc smelters was
1. 3 pounds per ton of zinc, and for lead plants 0. 8 was the aver-
age.
Emissions from a few of the processing plants that did not pro-
duce arsenic were far greater than those from the one plant that
did produce for the commercial market. Undoubtedly, more ar-
senic would be produced and less emitted to the atmosphere if
there were a greater incentive for smelters to recover the ele-
ment.
During 1968 estimated arsenic emissions to the atmosphere due
to metallurgical processing of arsenic-bearing ores totaled
4,466 tons. The emission estimates are based on material bal-
ance and stack sampling data obtained from industrial sources.
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REPROCESSING
During 1968 about 70 percent of the arsenic consumed in the
United States was used for agricultural purposes, and nearly
20 percent was used in glassmaking. The remainir.g 10 per-
cent was used for various purposes including wood preserva-
tives, nonferrous alloys, animal dips, paints, pyrotechnics,
poultry feeds, and other products.
AGRICULTURAL
The principal use of white arsenic is in the manufacture of the
arsenical pesticides. Some of the compounds are lip'.ed below.
AGRICULTURAL PESTICIDE COMPOUNDS
Sodium arsenate Cacodylic acid
Lead ar senate Calcium a r sen.it e
Calcium a r senate Zinc arser-.ite
Zinc, a.rser-i.te Sodium arsenite
Arsenic acid Di sodium mer.bl a.ir
All these compounds are produced from arsenic trio-vide ^r..d :Lv.e
m-iE.ufactu.ring process is relatively simple. Arsenic, acid is
produced by reacting arsenic trioxide with nitric arid. Ca!;.r.m
arser.ate is prodxi.ced by reacting arsenic acid with lime; If i.d
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arsenate by reacting a.rsenic acid with litharge (lead oxide). Ar-
senic trioxide reacted with sodium hydroxide produces sodiutn
arsenite.
Since the production of arsenic compounds is simple, many of the
manufacturers of pestidices commence their operation with the
purchase of arsenic trioxide and other basic materials. They pre-
pa.re the arsenic compounds, then formulate and package the pesti-
cides. Some of the manufacturers are large, others are small,
and size seems to be the most important factor govern.irie the gen-
eral type of equipment used to prepare the compounds and pesti-
cides. When the operation is small, arsenic trioxide is usually
received .in casks or barrels a.nd unloaded by hand.. Reactions are
often carried out in closed vessels. The principal problem from
the standpoint of atmospheric emissions stems from dusting dv.r-
ing handling of the materials.
Majiy of the large manufacturers are prepared to handle bulk ma-
terials. At one location a.rsenic trioxide is received in railroad
cars and dumped directly below into a receiving tank where it is
reacted with nitric acid to produce arsenic acid.
Reports from pesticide manufacturers indicate that arsenic
losses a.re small. None of the reactions result in significant
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vapor emissions to the atmosphere and most of the dusting situa-
tions are usually handled by air pollution control systems consist-
ing of hoods, ducts, exhaust fans, and baghouses. The dusts
handled are in the 0. 5 to 10 micron range.
Manufacturers state their material records indicate no detectable
losses of arsenic during processing; however, it is evident there
is a slight atmospheric emission which is estimated at 20 pounds
per ton of arsenic processed.
During 1968 arsenic emissions to the atmosphere due to the manu-
facture of pesticides totaled 196 tons.
GLASS MANUFACTURE
Arsenic is used in nearly all types of glass. It aids in the re-
moval of bubbles during manufacturing and acts as a stabilizer
of selenium in decolorizing crystal glasses.
The proportion of arsenic used is very small, seldom as much as
10 pounds per ton of glass and usually not more than 2 pounds per
ton. In window glass the amount used generally ranges from 1/4
pound to 5 pounds per ton /.
1- Tooley, F. V. ; Handbook of Glass Manufacture; Ogden Pub-
lishing Company; New York, N. Y.; 1953.
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-30-
Of the five major types of glass produced commercially, soda-
lime glass is the most widely used. It is well suited for window
glass, plate glass, containers, electric light bulbs, and many
other inexpensive articles. It accounts for about 90 percent of
all glass production and is produced on a massive scale in large,
direct-fired, regenerative furnaces that operate continuously.
Glass furnaces are usually directly fired with oil or natural gas
and heat is reclaimed in checkerwork regenerators. Raw ma-
terials are charged at one end of the furnace and molten glass
is pulled from the other end. Glass temperatures are as high
as 2, 700 F in the furnace, but usually near 2, 200 F at the dis-
charge.
There are two principal sources of particulate matter in the ex-
haust gases: raw materials entrained in combustion gases, and
materials from the melt. Particulates expelled from the furnace
are the result of many physical and chemical reactions that occu:
during melting. The reactions are so complex that predictions
of losses cannot be based on temperature and vapor pressure
data alone. One significant factor affecting the quantity of par-
ticulates is the production rate. As the production rate of the
furnace is increased, the particulates also increase in quantity.
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-31-
The people in the glass industry that were contacted during this
study provided general information concerning glassmaking, the
use of arsenic, methods of operation, and the use of air pollu-
tion control equipment, but they could not provide specific data
regarding arsenic emissions to the atmosphere. Stack tests
were not available showing the arsenic content of the exhaust
gases, and material balance records were not sufficiently accu-
rate concerning the minor constituents of the melt.
Particulate emissions average about 2 pounds per ton of glass
produced based on good operation _/ and the arsenic trioxide
content of the particulate has been reported as 7. 71 percent /.
Based on the following, the emission factor for arsenic is 232
pounds per ton of arsenic used in the manufacture of glass.
1- Duprey, R. L. ; Compilation of Air Pollutant Emission
Factors Public Health Service Publication No. 999-AP-42;
1968.
2- Air Pollution Engineering Manual; Public Health Service
Publication No. 999-AP-40; Table 212; 1968.
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= 32-
ARSENIC EMISSION DATA
GLASS MANUFACTURE
Particulate emission (Ib/ton of glass) - 2
Arsenic trioxide content of particulate (percent) - 7.71
Arsenic content of arsenic trioxide (percent) - 76
Arsenic used in glass (Ib/ton of glass) - 1
Total arsenic in glass (tons) 1968 - 5, 500
During 1968 arsenic emissions to the atmosphere resulting
from the manufacture of glass totaled 638 tons.
WOOD PRESERVATIVES
Wood preservatives that contain arsenic compounds have been
used during the past thirty or forty years for the treatment of
telephone poles, mine timbers, and other wood materials.
Wolman salts and Osmosalts are wood preservatives that con-
tain about 25 percent sodium arsenate. Bolidensalt BIS, a zinc-
chromium arsenate, contains 20 percent arsenic acid and 21 per-
cent sodium arsenate. Bolidensalt BIS Copperized also contains
20 peicent aisen.ic acid and 21 percent sodium arsenate. Bolid-
ensalt K33, a nonionic copper-chromium arsenate, contains 42
percent arsenic acid.
These compounds are used in solution and arsenic emissions to
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the atmosphere that occur are principally those resulting from
handling the dry materials during the initial processing steps.
People in industry that were contacted regarding the manufacture
and use of wood preservatives stated that there are no detectable
emissions of arsenic during processing.
During 1968 arsenic emissions to the atmosphere resulting from
the manufacture of wood preservatives are considered to be neg-
ligible.
NONFERROUS ALLOYS
Arsenic occurs naturally in many copper ores and may be per-
mitted to remain after the refining process in concentrations of
about 0. 3 percent. Sometimes the element is added intention-
ally in amounts up to 0. 5 percent and marketed under the name
of "arsenical copper".
One use of arsenical copper is in building automobile radiators
and other copper units that are soldered together. Since the an-
nealing temperature of the alloy is higher than the soldering tem-
perature, loss of strength is negligible. Another use is in heat
exchangers and condenser tubes.
Arsenic is also found in many lead ores and is used in small
amounts YLn certain lead alloys. Small additions of arsenic will
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-34-
harden lead and change its surface tension. Two of the best
known uses for arsenical lead are in the manufacture of bat-
teries and munitions. One munitions manufacturer reports the
use of two types of antimonial arsenical lead; type A containing
2 to 2-1/2 percent arsenic, and type B containing 1. 15 to 1.25
percent arsenic. The two types are melted together to obtain
the desired characteristics. For use in batteries arsenic is
added principally to form hard lead which is used for battery
grids, posts, and cable sheathing.
Arsenic is also used as an alloying material to produce arseni-
cal lead babbits. This babbit is hard with a fine uniform struc-
ture that resists fatigue and is used in internal combustion, en-
gines where relatively high temperatures are encountered.
Arsenic may be added in small quantities to brass to prevent
dezincification and minimize season cracking.
Alloying and melting operations cause some emissions, but man-
ufacturers claim there is no need for special air pollution con-
trol equipment. According to the information obtained from in-
dustry, arsenic emissions to the atmosphere are approximately
one pound per ton of arsenic processed.
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-35-
During 1968 atmospheric emissions due to the processing of
arsenic alloys wexe less than 1/4 ton, and are considered neg-
ligible.
OTHER
As stated elsewhere in this report sodium arsenate, arsenic di-
sulfide, arsenic trisulfide, and arsenic pentasulfide are used in
paint pigments, pyrotechnics, cattle and sheep dips, pharmaceu-
ticals, poultry feed additives, and other miscellaneous products.
A small amount of high-purity arsenic is used in semiconductors.
Some semiconductor compounds are formed by alloying arsenic
with aluminum, gallium, and indium. Gallium arsenide is used
in the production of tunnel and varactor diodes, transistors,
solar cells, and experimental lasers. Indium arsenide also is
used to produce experimental lasers as well as Hall-effect and
infrared devices. "A minute amount of arsenic is used in some
germanium and silicon devices. Some low-melting glasses con-
taining high-purity arsenic are useful in semiconductor and in-
frared applications.
Information obtained from industrial sources varies consider-
ably regarding arsenic emissions to the atmosphere; however,
all agree that the principal emission is due to handling of dry
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-36-
arsenic compounds. Average emissions are estimated at 3
pounds per ton of arsenic processed.
During 1968 arsenic used in reprocessing miscellaneous products
totaled 2,200 tons; atmospheric emissions were an estimated
3. 3 tons.
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-37-
CONSUMPTIVE USES
Household and commercial products contain arsenic, even
though it is not purposely added in the manufacturing process.
Arsenic in detergents is one example; another is arsenic in
coal. It occurs naturally in coal at an average concentration
about the same as in the earth's crust. It also occurs naturally
in the phosphates that are used in the manufacture of detergents.
AGRICULTURAL
Insecticides, fungicides, herbicides, and desiccants are widely
used and are applied as sprays or dusts under many different
conditions by aircraft and ground equipment. All the factors
affecting the application have been discussed in the literature
at great length; the droplet size, the spray drift, the fluid
properties, the meteorological factors, the air movement, tite
nozzle types, the evaporation, and numerous other subjects.
There is a wealth of general information that has been published,
but virtually none that is specific regarding the amount of spray
or dust that is not effective. The pesticide industry as a whole
merely answers that there are too many factors involved. A
few documents have been located which contain some specific
data relating to emissions that occur during cotton ginning opera-
tions.
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-38-
The concentration of dust and arsenic observed near a cotton
gin in Texas has been reported as shown in Table III, and the
arsenic content of the particulate averages about 0. 03 percent.
Another study shows that the particulate discharged from gin-
ning operations is 11.7 pounds per bale of cotton ginned _/.
Published statistics show that the production of cotton during
1968 was 10, 948, 000 bales (500 pounds per bale) *J.
ARSENIC EMISSIONS FROM COTTON GINNING
Cotton production 1968 (500 Ib. bales) 10,948,000
Particulate discharge - Ib/bale of cotton
ginned 11.7
Arsenic content of particulate - percent 0.03
The particulate discharge was approximately 64, 000 tens, and
arsenic emissions were about 19 tons.
The burning of cotton gin trash is also known to be a source of
arsenic emissions to the atmosphere. It has been reported that
the trash averages about 700 pounds per bale of cotton produced
1- Air-borne Particulate Emissions from Cotton Ginning Opera-
tions; U. S. Public Health Service; Taft Engineering Center
Technical Report A60-5; I960.
2- Agricultural Statistics - 1969; U. S. Dept. of Agriculture.
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-39-
TABLE III
SUSPENDED PARTICULATE AND ARSENIC
CONCENTRATIONS IN THE AIR NEAR COTTON
GINS IN WEST TEXAS - 1964
Range of
Distance Suspended
from Gin Particulate
(ft) Concentrations
(/ug/m3)
150 - 300a 5,000 - 76,000
1: 200 - l,400a 385 - 187
2,200 - 8: 000a 217 - 42
b 67 - 783
Range of Arsenic per
Arsenic /***§
Concentrations Participates
(yMg/m3) Ratio x 104
0.6 - 141 1.2 - 18.5
.07-0.08 3.7 - 2. 1
.10-0.01 4.6 - 2.4
Average
0.0003
a - Measurement downwind from the gin
b ~ Measurement upwind from the gin
1- Control and Disposal of Cotton-ginning Wastes; A Symposium; Public
Health Service Publication 999-AP-31; May 3-4, 1966.
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and that about 37 percent of the trash is burned _/. Another
report shows that arsenic lost from leaf trash during combus-
tion averages about 76. 6 percent /. Based on the assumption
that the arsenic content of the trash is the same as that of the
particulates emitted during ginning, calculations show 425 tons
of arsenic in the trash burned, and 326 tons of arsenic emis-
sions to the atmosphere.
There are many sources of arsenic emissions due to the use of
pesticides other than those discussed above. There are emis-
sions that occur during the application of sprays and dusts, the
incineration of pesticide containers, and evaporation. In order
to estimate these emissions, the problem was discussed with
people knowledgeable with the application of pesticides. In
most instances they were reluctant to estimate losses; how-
ever, a few did express an opinion. As a result, the atmos-
pheric emissions of arsenic due to the use of pesticides during
1968 have been estimated at 3,270 tons, including 19 tons from
cotton gins and 326 tons from burning cotton gin trash.
1- Control and Disposal of Cotton-ginning Wastes; A Sympos-
ium; Public Health Service Publication 999-AP-31;
May 3-4, 1966.
2-Aboul-Ela, M. M. and Miller, C. S. ; "Studies of Arsenic
Acid \Residues iii Cotton"; Texas Agricultural Experiment
Station; Texas A & M University; MP 771; June, 1965.
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COAL
The arsenic content of various samples of coal has been reported
as shown in Table IV, and the average concentration in domestic
coal is about 5.44 ppm. Coal consumed in the United States dur-
ing 1968 was 508, 990, 000 tons (bituminous and anthracite) V;
therefore, the arsenic in coal was about 2, 770 tons.
During combustion arsenic was discharged with the bottom ash
and the fly ash. With respect to fly ash, a study has been made
regarding emissions from coal fired power plants and the emis-
sions of arseni<: ha.ve been recorded. Arsenic concentrations in
fly ash samples taken from the stack (alter fly ash collection)
ranged from 0. 11 to 1. 6 grains per scf x 10"* /. Based on
508, 990, 000 tons of coal consumed, a.n arsenic concentration of
0. 64 grains per sc.f x. .10"^, and ]60 scf of flue ga.s per pound of
coal, the a.rser.ir emissions i.r. the United States during 1968 due
to the combos:.!on of coal totaled 74.3 to.is.
1- Minerals Yearbook; Bureaii of Mines: 1968.
2- Cuffe, St'-iiJey T. a.j.d Gerstle, Rirha.rdW.; "Emissions
from Coil Fiired Power Plants": Public Health Service
Publication No. 999-AP-.35; 1967.
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-42-
TABLE IV
AVERAGE ARSENIC CONTENT OF COAL ASH
Region
Frequency of As Content Ash Content As Content
Detection - % of Ash - % of Coal - % of Coal - %
Eastern Province
Interior Province
Western States
67
41
16
0.0107
0. 0049
0.0012
9.3
10.5
9.8
0.000995
0.000520
0.000118
Average Arsenic Content in Coal
0.000544
NOTES - The above table based on "Spectrochemical Analyses of Coal Ash
for Trace Elements"; Table 1; Bureau of Mines RI 7281; July 1969.
Averages were calculated for all samples tested using zero for
arsenic contents below the limit of detection.
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-43-
OIL
During this study numerous oil analyses were obtained that re-
cord the metal content of various crude and residual oils. Some
of this information was obtained during a literature search, but
most of it was unpublished data furnished by major oil companies
and large users of residual oil. The data obtained included analy-
ses of more than 400 samples of crude and residual oils from the
Middle East, South America, and the United States. Most of the
analyses showed the percent of vanadium, nickel, and copper,
but not the arsenic content. Only one group of 110 tests of domes-
tic crude oil included data concerning arsenic.
In 97 tests the arsenic was below the limit of detection, but in 13
tests the arsenic content ranged from 8 to 2, 380 ppb. The aver-
age for the 110 tests was 42 ppb _/.
During 1968 the total new supply of oil in the United States was
4, 922 million barrels _/; about 79 percent was produced in the
United States. Based on an average arsenic content of 42 ppb,
1- Uranium and Other Metals in Crude Oils; Geological Survey
Bulletin 1100; U. S. Government Printing Office; Washington,
D. C.; 1961.
2- Crude Petroleum, Petroleum Products, and Natural Gas
Liquids: 1968; Mineral Industry Surveys; Petroleum
Statement; Annual.
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-44-
the arsenic in the oil was about 36 tons; however, it is doubtful
that this data is sufficiently accurate for estimating emissions.
The arsenic content of imported residual oils is likely the most
important factor not included in the above figures.
DETERGENTS
Arsenic has been detected in several common presoaks and
household detergents that are marketed in the United States.
The concentrations in various types are tabulated in Table V.
It has been confirmed that the arsenic is not added intention-
ally; it occurs naturally in the phosphates that are used in the
manufacture of the detergents.
Atmospheric emissions of arsenic that may occur due to use
of detergents is considered as negligible.
PHOSPHORIC ACID
The phosphoric acid used for producing phosphates for foods,
drugs, and detergents is normally made by the thermal pro-
cess. Although the raw acid may contain arsenic, lead, and
other heavy metals a very pure acid can be produced by treat-
ment with a sulfide to precipitate the metal ions /.
1- '"Atmospheric Emissions from Thermal-Process Phosphoric
Acid Manufacture"; Public Health Service Publication No.
AP-48; 1968.
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-45-
The phosphorus which is a basic raw material for the thermal
process is usually made by reducing phosphate ore in electric
furnaces. Therefore, it is likely that there are significant
atmospheric emissions of arsenic during the production of
phosphoric acid. The data to determine the magnitude of the
emissions were not available during this study.
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-46-
TABLE V
CONCENTRATIONS OF ARSENIC
IN CERTAIN/ DETERGENTS AND PRESOAKS ll
A.
B.
C.
D.
E.
F.
G.
H.
Detergent
Type
EP
HDED
HDD
HDED
HDED
EP
DA
EP
Arsenic
Average
34
32
9
15
41
7
2
59
Concentration
(ppm)
Range
31-43
SD
8-10
SD
38-45
6-9
1-3*
51-73
'•'Lower limit of detection
NOTE: Abbreviations are:
EP - enzyme presoak
HDED - heavy duty enzyme detergent
DA - detergent aid
HDD - heavy duty detergent
SD - single determination
1- Angino, E. E. , Magnuson, L. M. , Waugh, T. C.,
Galle, O. K. and Bredfeldt, J. ; "Arsenic in Detergents:
Possible Danger and Pollution Hazard"; Science; 168;
pp 389-390; Apr. 17, 1970.
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-47-
INCINERATION AND OTHER DISPOSAL
Nearly all the uses of arsenic are such that very little remains
for disposal. After it is used in pesticides, paint pigments,
pyrotechnics, and many other products, a small amount remains
in the shipping containers; in many instances this arsenic is
disposed of by burning. The emissions resulting from this source
have been included under Reprocessing and Consumptive Uses,
SEWAGE AND SLUDGE
A recent report concerning the burning of sewage and sludge in-
dicates that the burning rate in the United States is about 2, 000
tons per day, and the mercury content ranges up to 30 ppm /.
The arsenic content is not stated.
Another report published in 1970 shows the arsenic concentra-
tion in the raw sewage input at a sewage treatment plant in
Kansas to range from 2 to 3.4 ppb /.
1- Private communication from the Federal Water Pollution
Control Authority. (Investigations being conducted during
1971; therefore, data is subject to revision.)
2- Angino, E. E., Magnuson, L. M. , Waugh, T. C.,
Galle, O. K. and Bredfeldt, J. ; "Arsenic in Detergents:
Possible Danger and Pollution Hazard"; Science; 168;
pp 389-390; Apr. 17, 1970.
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-48-
The arsenic content of the sewage burned in the United States
was not available for this study, but it is believed that some ar-
senic is present in most sewage and that the concentration in sew-
age burned (dry) is considerably higher than in raw sewage. Ar-
senic emissions to the atmosphere due to the burning of sewage
may be in the order of Z to 10 tons per year.
IRON AND STEEL
During this study spectrographic analyses of dust samples from
foundries have been examined; they all indicate arsenic and many
other elements are contained in the dust. This information con-
firms that foundries, and possibly steel mills, are sources of
arsenic emissions to the atmosphere.
The cupola is the most used method for producing cast iron.
The rate of particulate emissions from gray iron cupolas has
been reported as 4 to 26 pounds per ton of process weight not
including emissions from handling, charging, or other non-
melting operations.
Based on the information obtained from industry the particulate
emission factor is estimated at 22 pounds per ton of process
weight, including melting and non-melting operations. The
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-49-
arsenic content of the particulate is about 0.07'percent / and
the degree of emission control approximately 25 percent.
During 1968 the pig iron and scrap used by iron foundries totaled
16, 788, 000 short tons z/. Arsenic emissions to the atmosphere
due to the production of cast iron were 97 tons.
1- Private communication with industrial source.
2- Minerals Yearbook; Bureau of Mines; 1968.
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-50-
APPENDIX A
COMPANIES DEALING IN ARSENIC
AND ARSENIC COMPOUNDS
CALIFORNIA
Electronic Space Products, Inc.
LOCATION
Los Angeles
DISTRICT OF COLUMBIA
Hercules, Inc.
Washington
ILLINOIS
Division Lead Company
Summit
MISSOURI
Mallinckrodt Chemical Works
St. Louis
NEW JERSEY
J. T. Baker Chemical Company
Rhodia, Inc.
Sylvan Chemical Corporation
Phillipsburg
New Brunswick
Englewood Cliffs
NEW YORK
Alloys Unlimited, Inc.
American Smelting and Refining Co.
Anglo-American Metal & Ferro
Alloy Corporation
Asarco Intermetallics Corporation
Ascher Alloys, Inc.
Atomergic Chemetals Company
Belmont Smelting and Refining Works
City Chemical Corporation
Gallard-Schlesinger Chemicides, Inc.
International Selling Corporation
Melville
New York City
New York City
New York City
Brooklyn
Carle Place, L. I.
Brooklyn
New York City
Carle Place, L. I.
New York City
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-51-
Kawecki Chemical Company
McKesson Chemical Company
Mutchler Chemical Company, Inc.
Phillip Brothers Chemicals, Inc.
Republic Chemical Corporation
J. A. Samuel and Company, Inc.
Semi Alloys, Inc.
United Mineral & Chemicals, Inc.
New York City
New York City
New York City
New York City
New York City
New York City
Mount Vernon
New York City
OHIO
The Harshaw Chemical Company
Cleveland
PENNSYLVANIA
Bram Metallurgical Chemical Company Philadelphia
The O. Hommel Company Pittsburgh
Pennsylvania Coal Products Company Petrolia
Rare Metal Products Company Atglen
Semi-Elements, Inc. Saxonburg
TEXAS
Industrial Materials Company
Houston
WASHINGTON
Cominco American Incorporated
Spokane
WISCONSIN
The Ansul Company
Marinette
(Thomas Register; Dec. 1968 Ed. )
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BIBLIOGRAPHIC DATA
SHEET
1. Report No.
APTD-1507
3. Recipient's Accession No.
4. Title and Subtitle
National Inventory of Sources and Emissions: Arsenic - 1968
5' Report Date
May 1971
6.
7. Author(s)
8. Performing Organization Rcpt.
No.
9. Performing Organization Name and Address
W. E. Davis & Associates
9726 Sagamore Road
Leawood, Kansas
10. Project/Task/Work Unit No.
11. Contract/Grant No.
CPA 70-128
12. Sponsoring Organization Name and Address
ENVIRONMENTAL PROTECTION AGENCY
Air Pollution Control Office
Durham, North Carolina
13. Type of Report & Period
Covered
14.
15. Supplementary Notes
16. Abstracts
The inventory of atmospheric emissions has been prepared to provide reliable informa-
tion regarding the nature, magnitude, and extent of the emissions of arsenic in the
U. S. for the year 1968. Background information concerning the basic characteristics
of the arsenic industry has been assembled and included. Brief process descriptions
are given, but they are limited to the areas that are closely related to existing or
potential atmospheric emissions of the pollutant. The arsenic emissions and -mission
factors presented are based on the summation of information obtained from the one
processing company that produced arsenic during 1968, the copper, lead, and zinc
smelters, and the reprocessing companies that handle about fifty percent of the
arsenic consumed in the United States.
17. Key Words and Document Analysis. 17o. Descriptors
Air pollution
Emission
Inventory
Sources
Arsenic
Industrial plants
Reprocessing
Meturgical furnaces
Mining
Consumption
17b- Identifiers/Open-Ended Terms
Year 1968
United States
Utilization
17e. COSATI Field/Group
138
18. Availability Statement
Unlimited
19. Security Class (This
Report)
UNCLASSIFIED
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a8UNCLASSIFIF.D
21. No. of Pages
58
22. Price
FORM NTIS-33 (REV. 3-721
USCOMM-OC 110S2-P72
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