United States
Environmental Protection
Agency
Air
Office of Air Quality
Planning and Standards
Research Triangle Park NC 27711
EPA-450/4-84-014g
September 1987
National Dioxin
Study
Tier 4
Combustion
Sources
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EPA-450/4-84-014g
National Dioxin Study
Tier 4 Combustion Sources
Project Summary Report
By
Air Management Technology Branch
U.S. ENVIRONMENTAL PROTECTION AGENCY
Office Of Air And Radiation
Office Of Air Quality Planning And Standards
Research Triangle Park, NC 27711
September 1987
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This report has been reviewed by The Office Of Air Quality Planning And Standards, U. S. Environmental
Protection Agency, and has been approved for publication. Mention of trade names or commercial products
is not intended to constitute endorsement or recommendation for use.
EPA-450/4-84-014g
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ACKNOWLEDGEMENTS
Many people and groups contributed to the design and implementation of the
Tier 4 study. The major responsibility for managing the day-to-day activities
for the project rested with the staff of the Air Management Technology Branch
(AMTB) of the U. S. Environmental Protection Agency's (EPA) Office of Air Quality
Planning and Standards (OAQPS). Major input to the design and review of the
program came from a Tier 4 Work Group composed of representatives from various
offices throughout the Agency. Significant input was also provided by the
Pollutant Assessment Branch, OAQPS.
The field work was supported by two Office of Research and Development (ORD)
Laboratories: (1) the Air and Energy Engineering Research Laboratory, Research
Triangle Park, NC, which provided sampling methods support and consultation;
and (2) the Hazardous Waste Engineering Research Laboratory in Cincinnati, OH,
which provided technical and contractual support for the field testing program.
Field support for the collection of samples was also provided by EPA Regional
Offices, many State and local environmental agencies, Radian Corporation, and
various other supporting contractors.
Analytical support was provided by a group of EPA laboratories, collec-
tively referred to as the Troika, comprising ORD's Environmental Monitoring
Systems Laboratory, Research Triangle Park, NC; Environmental Research Labora-
tory, Duluth, MN; and the Office of Pesticides and Toxic Substance's Environ-
mental Chemistry Laboratory, Bay St. Louis, MS.
Radian Corporation, through contracts with EPA, supported the study in
the development of background, design, implementation, and interpretation of
results. Quality assurance support was provided by the Research Triangle
Institute.
The assistance and participation of all these groups and the "behind the
scenes" individuals are acknowledged and appreciated.
iii
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TABLE OF CONTENTS
Page
List of Tables v
Introduction i
Objectives 1
Background 2
Study Design 3
Sample Collection 6
Site Selection 7
Sampling Procedure And Analyses 8
Results 9
Tier 4 Stack Test Results 9
Quality Assurance 12
Results Reported in the Literature 13
Discussion of Stack Test Results 13
Tier 4 Ash Sampling Results 21
Findings and Conclusions 25
Continuing Efforts 27
Additional Information 28
References 30
iv
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LIST OF TABLES
NUMBER
PAGE
1 Combustion Sources Categories Where Ash And Stack
Samples Were Collected ........................................ 5
2 Tier 4 CDD Stack Testing Results ................................ 10
3 Tier 4 CDF Stack Testing Results ................................ 11
4 CDD Emissions Data. From Studies Similar To Tier 4 ............... 14
5 CDF Emissions Data From Studies Similar To Tier 4 ............... 15
6 Tier 4 And Other Sources Listed In Rank Order By 2378-TCDD
Concentrations
7 Toxic Equivalency Factors Used In Estimating 2378-TCDD
Equivalents ....... . ........................................... 1 g
8 Tier 4 And Other Sources Listed In Rank Order by 2378-TCDD
Equivalents [[[ 19
9 Tier 4 Ash Sampling Results ..................................... 22
10 Tier 4 Source Categories With Below Detection Limit
Ash Sample Results ............................................ 24
11 Comparison Of Ash And Stack Emissions At Sources With
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Introduction
This report presents a concise summary of Tier 4, combustion sources, of
the U. S. Environmental Protection Agency's National Dioxin Study. It is
intended to be an overview document which presents in summary form the major
results and conclusions from this study. The major portion of this report is
comprised of the chapter on combustion sources taken from the U.S. Environ-
mental Protection Agency's National Dioxin Study Report To Congress presented
to the Congress in September 1987.
Objectives
In December 1983, the U. S. Environmental Protection Agency (EPA) issued
its National Dioxin Strategy, which was designed (a) to determine the overall
extent of dioxin contamination in the environment and (b) to provide a syste-
matic approach for dealing with dioxin contamination problems. The primary
focus of the strategy was on 2,3,7,8-tetrachlorodibenzo-p-dioxin (2378-TCDD),
which is believed to be the most toxic of the chlorinated dibenzo-p-dioxin
(CDD) compounds.* To implement the strategy, the EPA defined the following
seven categories (or tiers) of sites for investigation:
Tier 1 - 2,4,5-trichlorophenol (2,4,5-TCP) production sites and associated
waste disposal sites. [2378-TCDD is a known contaminant of 2,4,5
trichlorophenols.]
Tier 2 - Sites and associated waste disposal sites where 2,4,5-TCP was
used as a precursor to make pesticidal products.
Tier 3 - Sites and associated waste disposal sites where 2,4,5-TCP and its
derivatives were formulated into pesticidal products.
Tier 4 - Combustion sources.
Tier 5 - Sites where 2,4,5-TCP and pesticides derived from 2,4,5-TCP have
been, or are being, used on a commercial basis.
Throughout this report, the abbreviations CDD and CDF are used to indicate
chlorinated dibenzo-p-dioxin compounds and chlorinated dibenzofuran compounds,
respectively. CDFs are compounds similar to CDDs in structure and chemical
activity.
-1-
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Tier 6 - Sites where improper quality control on manufacturing of certain
organic chemicals and pesticides could have resulted in the
inadvertent formation of 2378-TCDD.
Tier 7 - Control sites where contamination from 2378-TCDD was not suspected.
This report summarizes the finding of Tier 4, the portion of the study
dealing with combustion sources. The primary objective of the Tier 4 study was
to determine the potential scope and magnitude of CDD and CDF releases from
combustion sources. The study was designed to determine which combustion source
categories emit CDDs and at what concentrations. The main focus was on releases
to the ambient air; however, other samples, such as ash and scrubber water, were
also obtained to determine if these compounds are released to other media. Be-
cause some combustion sources were known to emit a wide range of CDD and CDF
compounds, Tier 4 samples were analyzed for specific groups (homologues) of CDD
and CDF compounds, as well as for 2378-TCDD, the compound of most specific
concern.
Background
There are millions of combustion sources in the United States. Residential
heating units burn oil, gas, coal and wood for heat. Larger commercial, institu-
tional and utility boilers burn fossil fuels to generate heat and electricity.
Many industrial processes burn fuels and other raw or waste materials to produce
heat and/or recover products of marketable value. Other processes, such as
incineration, use combustion to reduce the volume of unwanted waste products and
to recover heat and other resources. Open fires, both accidental (e. g.., struc-
ture and forest fires) and intentional (i.e., those set for forest management and
agricultural burning), are other examples of combustion sources.
Assessment of CDD and CDF emissions from combustion sources has received
limited study. Previous work included studies of emissions from hazardous waste
incinerators, utility boilers and municipal waste combustors. Even for those
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source categories that have been tested, there is considerable variation in the
extent and quality of testing and in the test methods employed.
Study Design
It was impractical to test all of the combustion source categories under
Tier 4. A study plan was developed that identified those source categories
which were believed to have the greatest potential for emitting CDDs to the
atmosphere. Selection and prioritization of source categories for testing were
based upon a review of CDD related studies reported in the literature, and on
engineering judgment.^»3 Information from this review suggested that the
following conditions were most important for CDD formation:
1. Presence of CDD in the materials being burned;
2. Presence of CDD precursors in the materials being burned (e.g.,
chlorinated phenols, chlorinated benzenes); and
3. Presence of chlorine, fuel and .combustion conditions conducive to
CDD formation, including:
(a) Relatively low combustion temperature (500 - 800°C);
(b) Short residence time of fuel in the combustion zone
(< 1 to 2 seconds);
(c) Lack of adequate oxygen (resulting in incomplete combustion);
(d) Lack of adequate processing of fuels (e. g., burning of wet
garbage); and
(e) Lack of supplemental fuel to promote combustion efficiency.
Based on a relatively subjective determination of which combustion source
categories were most closely associated with these factors, judgments were made
as to the likely potential of various source categories to emit CDDs. Certain
source categories judged to have a relatively low potential to emit CDDs were
not given further consideration for testing. For example, process heaters and
-3-
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gas turbines were believed to have a low potential because of their ' higher
combustion efficiencies and use of fuels with low chlorine content (e.g.,
ry
natural gas).
Analysis of these combustion related conditions suggested that municipal
waste combustors, sewage sludge incinerators and recovery boilers at kraft paper
mills should be tested because these were judged to have potential for CDD emis-
sions and because they were large source categories. Table 1 lists the source
categories identified in the prioritization effort. A more thorough explanation
of the selection and prioritization process is contained in the Tier 4 Project
Plan, which was widely circulated for comment before implementation.^ Some of
the source categories in Table 1 were included primarily on the basis of
reviewer's recommendations. A few source categories (wood stoves and mobile
sources) were included since these sources were being tested for other purposes
and the add on costs for CDD and CDF testing was small. Further adjustments
were made to the initial list of sources to be tested as the study progressed.
Tier 4 sampling efforts focused on source categories that had not been
widely tested. Although some municipal waste combustors were known to emit CDDs,
no additional stack testing of this source category was performed.* Compared to
most other source categories, a relatively large data base already existed. In
addition, other air pollution control agencies, such as the New York Department
of Environmental Conservation and Environment Canada were conducting or planning
studies of municipal waste combustors. Selected stack emission data from
municipal waste combustors are summarized later in this report. In addition,
Tier 4 collected ash samples from municipal waste combustors.
Subsequent to this decision, Congress has directed EPA to provide a report
specifically on municipal waste combustor emissions of CDDs under the require-
ments of Section 102 of the Hazardous and Solid Waste Act of 1984.
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TABLE 1. COMBUSTION SOURCE CATEGORIES WHERE ASH
AND STACK SAMPLES WERE COLLECTED
Source Categories Sampled
Sewage Sludge Incinerator
Kraft Paper Recovery Boiler
Industrial Waste Incinerator
Wire Reclamation Incinerator
Secondary Copper Smelter
Carbon Regeneration Furnace
Drum and Barrel Furnace
Wood Stove
Wood Fired Boiler
Mobile Source
Charcoal Manufacturing Oven
Utility Boiler
Small Spreader Stoker Coal Fired Boiler
Commercial Boiler
Kiln Burning Hazardous Wastes
Open Burning/ Accidental Fires
Sulfite Liquor Boiler
Apartment House Incinerator
Hazardous Waste Incinerator
Hospital Incinerator
Municipal Waste Combust or
Charcoal Grill
Sample Type
Ash
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
Stacka
X (3)
X (3)
X (1)
X (1)
X (1)
X (1)
X (1)
X (1)
X (1)
X (2)
aNumber in parentheses indicates the number of sources in the category which
were stack tested under Tier 4.
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Sample Collection
Two types of testing were considered for each of the source categories
listed in Table 1, stack sampling and ash sampling.
1. Stack Sampling
Stack sampling provides the best quantitative measurement of CDD
emissions; however, it is expensive (e. g., $50,000 to $100,000 per source, not
including analytical costs). Where possible, stack gas samples were collected
both before (inlet) and after (outlet) any pollution control device. Ash, feed
and soil samples were also collected at sites that were stack tested.
Because of the high costs, only thirteen sources could be stack tested.
Three kraft paper recovery boilers and three sewage sludge incinerators were
tested because they appeared to have conditions particularly conducive to CDD
formation. Only one source was tested in each of the other selected source cate-
gories. The focus of the testing program was primarily on sources believed to be
indicative of average to worst case emissions situations.
2. Ash Sampling
Ash samples were primarily collected from air pollution control
devices (flyash) or from the residues of combustion (bottom ash) to provide a
general indication of the presense of CDDs. A secondary objective of the Tier 4
study was to examine possible relationships between ash and stack test results.
If such a relationship could be determined, inexpensive ash samples could be used
in lieu of expensive stack testing to identify source categories with high CDD
and CDF emission rates. Use of ash data is currently limited because observed
correlations between levels of CDDs in fly ash and CDD stack emissions are not
sufficient for quantitative use.2 Generally, ash samples were collected from
three sources within each of the source categories listed in Table 1.
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Site Selection
Selection of test sites for stack and ash sampling was based on a number
of factors. EPA Regional Offices were asked to recommend candidate sources,
based on criteria outlined in the Project Plan. For stack sampling sites, a
technical analysis was conducted to determine fuel composition and combustor
operating parameters for a particular source category that would likely result
in a "representative" to "worst case" emission situation. Candidate sources
were then contacted, and pretest survey visits were made to identify plants
with operations most closely resembling the hypothesized conditions and with
acceptable stack sampling locations.
Once a site was selected for stack testing, a detailed test plan was
prepared which described the physical layout of the source and specified the
locations .where samples would be collected. Each site specific test plan also
identified the number and type of samples to be collected, the sampling methods
to be used, and the quality assurance activities associated with that test site.
These test plans were circulated for review. After the test was completed, a
separate report for each site was prepared describing the actual testing per-
formed and the test results.
Ash sampling sites were generally selected based upon recommendations from
Regional, State and local environmental agencies. Ease of sampling and level
of participation by the agencies were considered in those cases where several
facilities appeared to be of equal interest. Ash samples were collected by State
and local agencies and EPA contractors during the surveys of candidate sources
for the stack sampling program, as part of actual stack sampling, and from
selected additional facilities.
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Sampling Procedure And Analyses
Consistent sample collection procedures were used at all sites. These
procedures are described in three Tier 4 protocol documents. One document
describes the ash sampling procedures; a second, the stack sampling procedures;
and a third, the quality assurance measures and procedures. »^>" The stack test-
ing method used at Tier 4 sampling sites is, with minor modifications, the state
of the art method proposed for use by a joint American Society of Mechanical
Engineers (ASME) and EPA work group for municipal waste combustors. This pro-
cedure, which uses a modified EPA Method 5 sampling train, is described in detail
in the stack test protocol document.-'
EPA's "Troika" of three inhouse laboratories was responsible for the
analysis, as well as for the preparation of the ODD and CDF analytical protocols
and laboratory quality control procedures to be used with Tier 4 sample's.
i
Analytical methods are described in an addendum to a Troika procedures document.^
While the Troika was responsible for all CDD and CDF analyses, an EPA
contractor, Radian Corporation, provided support for the analyses of other
compounds. For example, samples of some of the fuels and other feed materials at
each site were analyzed to determine the presence of possible precursors (e.g.,
chlorinated benzenes, biphenyls and phenols). In addition, continuous emissions
data were collected for various stack gases (e. g., CO, C02> 02) during each
stack test. Procedures used in these analyses are described in a separate
report."
An independent quality assurance program was also conducted for the stack
testing program, to ensure that test results were of acceptable quality. Another
EPA contractor, Research Triangle Institute, conducted the quality assurance
-8-
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program, which included both the auditing of three stack tests and the introduc-
tion of audit samples into the laboratories to evaluate their performance. The
independent quality assurance program is described in a separate report.^
Results
Approximately 350 samples were collected, 20 - 25% of which were for
internal quality assurance purposes. Thirteen sources were stack tested, and
72 sites were tested under the ash sampling program. Collected samples were
sent to the appropriate analytical laboratory in accordance with established
procedures.
1. Tier 4 Stack Test Results
Table 2 contains the ODD results of the 13 sites stack tested, while
Table 3 presents the CDF results. Data presented in these tables represent
concentrations of emissions measured in the stack gases. CDD/CDF stack concen-
trations have been normalized to an oxygen concentration of 3 percent. This
removes the effect of dilution, and is a more appropriate means of comparing
various combustion processes.
There is considerable variation in the concentrations among the
sources tested under Tier 4. Each of the sources with valid data had detect-
able levels of CDDs and CDFs, although not all had detectable levels of 2378-
TCDD. The reported 2378-TCDD, CDD and CDF concentrations from the secondary
copper smelter are an order of magnitude or more larger than any other source
tested under Tier 4, and as many as two to four orders of magnitude greater
than concentrations from some of the sources. A number of sources have consid-
erably lower concentrations than the secondary copper smelter, but considerably
greater concentrations than a number of other sources. On the other hand, some
sources (e. g., kraft paper recovery boilers) have very small concentrations of
-9-
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2378-TCDD, CDDs and CDFs. For most sources, the CDF concentrations appear to
be related to those of CDDs (i. e., sources which emit high concentration of
CDDs also emit high amounts of CDFs).
2. Quality Assurance
While the sampling and analysis methods used in this study were state-
of-the-art, they are nevertheless evolutionary. During the course of the study,
it was sometimes found that the analysis methods could not cope with high levels
of interfering contamination from other pollutants which caused difficulty in
achieving the desired validity and precision of results. Also, the stack sam-
pling method is currently undergoing validation testing. Preliminary results
indicate that recovery efficiencies from the sampling method may be low and
variable, with possibly less than half of the CDDs and CDFs in the stack
emissions being collected by the stack sampling method. Additional validation
testing is currently underway.
The stack gas samples collected at the secondary copper smelter con-
tained such high levels of CDDs and CDFs that the sensitivity of the analytical
procedures and equipment employed was reduced. Therefore, the results for
this source represent minimum levels, and actual values could have been
considerably higher.*
At the wire reclamation incinerator, the levels of contamination from
other organic compounds in the sample were so high, even after rigorous labora-
tory extraction and sample cleanup procedures, that only estimates of CDDs and
CDFs are available. At the wood stove site, it could not be determined if
CDD's and CDF's were present in any of the three stack test samples, due to
Subsequent to the Tier 4 test, the secondary copper smelter was retested by
the source in conjunction with the State Agency. Results from this retest
found CDD emissions to be one third of the Tier 4 results while CDF emissions
were 70 percent of the Tier 4 values.9
-12-
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similar organic contamination. No results were obtained from the mobile source
exhaust samples because internal reference standards were not added to the
samples prior to the extraction step in the analytical procedure. At a few
other sites, relatively minor problems occurred with a limited number of samples
but these did not affect the analysis or the overall integrity of the data.
3. Results Reported In The Literature
The scientific literature was reviewed to determine what combustion
source stack test studies had been conducted that were similar in scope and
measurement methodology to Tier 4.^-0 CDD and CDF data for 17 sources in the
United States and Canada are presented in Tables 4 and 5. These results have
also been normalized to a 3 precent oxygen concentration.
Table 6 has been prepared to facilitate a comparison of these data with
those obtained under the Tier 4 program. The sources in Table 6 are listed in
descending order of 2378-TCDD concentrations. Eight source tests (seven coal
fired boilers and one cofired boiler firing fuel and refuse) reported in the
literature had "nondetectable" stack gas concentrations of CDOs and CDFs.
Pre-1986 data for six municipal waste combustors are also provided.
4. Discussion Of Stack Test Results
Although it is useful to compare stack concentrations of CDDs and CDFs
among sources, such a comparison does not provide information with respect either
to the ground level concentrations that would result from these stack releases ort
to the relative differences in potential health effects of the various CDD and
CDF homologues. This discussion addresses these points.
The determination of the ground level concentration includes the
impact on dispersion of stack height, gas temperature, stack gas flowrate (i.e.,
the size of the source) and local meteorological conditions, in addition to CDD
and CDF stack concentrations. These parameters were entered into the dispersion
-13-
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-15-
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TABLE 6. TIER 4 AND OTHER SOURCES LISTED IN RANK ORDER
BY 2378-TCDD CONCENTRATION (ng/dscm @ 3% 02)a
Source
Secondary Copper Smelter**
Municipal Waste Combust or - Plant B
Municipal Waste Combust or - Plant E
Industrial Waste Incinerator
Hazardous Waste Incinerator
Municipal Waste Combust or - Plant D
Municipal Waste Combust or - Plant A
*Wood Fired Boiler
Sewage Sludge Incinerator - Plant C
Wire Reclamation Incinerator^3
Sewage Sludge Incinerator - Plant A
Drum And Barrel Furnace
Hospital Incinerator
Municipal Waste Combust or - Plant F
Municipal Waste Combustor - Plant C
Industrial Carbon Regenerator
Municipal Carbon Regenerator
Kraft Paper Recovery Boiler - Plant C
Sewage Sludge Incinerator - Plant B
*Kraft Paper Recovery Boiler - Plant B
Kraft Paper Recovery Boiler - Plant A
Cofired Boiler (coal and municipal waste)
Coal Fired Utility Boilers (7 Plants)
2378-TCDD
170
26
16
4.5
1.4
0.8
0.7
0.28
0.14
0.07
0.05
0.05
NDC
NRd
NR
ND
ND
ND
ND
ND
ND
ND
NR
Total CDDs
16,000
6,400
4,300
630
77
710
53
200
53
440
20
5
330
210
46
3.7
3.3
2.9
1.6
1.2
0.7
ND
ND
Total CDFs
65,000
11,600
5,300
2,400
190
150
260
83
450
580
44
27
735
250
120
3.3
4.8
2.1
28
0.7
0.6
ND
ND
ng/dscm @ 3% 02 " nanograms per standard cubic meter of flue gas, normalized to
3 percent oxygen.
values are estimated. The true values may be higher.
Not detected, generally at less than 1 ng/dscm @ 3Z 02-
dNR - Not reported.
ND
-------
component of Che Human Exposure Model (HEM) to estimate the annual average
ground level concentration in the vicinity of the source. An assumption made
in the application of this model to the Tier 4 data is that the CDD and CDF
emitted from the stack is a gas. The assumption of gaseous behavior is believed
to be a reasonable one for these sources. While different calculated ambient air
concentrations could result from consideration of particle deposition, it is
believed that such effects would not be significant because (1) these sources
are generally low level emitters and (2) the particle size is likely to be small
enough that the effect of deposition on ambient air concentration will not be a
significant factor.
EPA uses "2378-TCDD toxic equivalency factors" (TEF's) to compare the
relative potency of one mixture of CDDs and CDFs with different mixtures of
CDDs and CDFs.1-3- The use of the TEF approach permits an estimation of the car-
cinogenicity of the mixture of CDD and CDF compounds relative to the carcino-
genicity of 2378-TCDD. The TEFs for the various CDDs and CDFs used in this
analysis are presented in Table 7.
The 2378-TCDD equivalents, calculated maximum ground level concentra-
tion and 2378-TCDD equivalent annual emissions for the Tier 4 sources, and for
most of the sources from the literature, are presented in Table 8.* To place
these results in some perspective, the cancer risk from inhalation exposure to
a ground level concentration of 1 picogram per cubic meter of 2378-TCDD equival-
ence is estimated as 3.3 chances in 100,000, (i.e., 3.3 x 10"5) assuming 70 years
of continuous exposure.12 The 2378-TCDD equivalent annual emissions is the
Ground level concentration and annual emissions were not calculated for the
eight sources with nondetectable CDD/CDF emissions. Neither the hospital
incinerator nor the municipal waste combustor, Plant F, is included in Table 8.
-17-
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TABLE 7. TOXIC EQUIVALENCY FACTORS USED IN ESTIMATING
2378-TCDD EQUIVALENTS
Compound(s)
2378-TCDD
Other TCDDs*
Penta-CDDs
Hexa-CDDs
Hepta-CDDs
Octa-CDDs
2378-TCDF
Other TCDFs*
Penta-CDFs
Hexa-CDFs
Hepta-CDFs
Octa-CDFs
Toxic Equivalency Factor
1.0
0.01
0.5
0.04
0.001
0.000
0.1
0.001
0.1
0.01
0.001
0.000
In situations where 2378-TCDD or TCDF were not chemically
analyzed in the sample, total TCDDs and TCDFs will have a
relative potency factor of 1.0 and 0.1, respectively.
-18-
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total burden to the environment from the stack for these sources. It differs
from the maximum ground level concentration by being independent of atmospheric
dispersion.
As with the stack concentration data presented in Tables 2 and 3, there
is considerable variability among the various sources for all three of these
parameters. In general, the sources with the highest stack concentrations of
2378-TCDD, CDDs and CDFs reported in Table 6 also had the highest ground level
concentrations. One notable exception is the sewage sludge incinerator, Plant
C. Stack concentrations at this plant are about two to three orders of magni-
tude less than those of the secondary copper smelter, yet the estimated ground
level concentrations from the two sources differ by less than a factor of two.
The sewage sludge incinerator has a relatively low stack with low temperature
flue gas coupled with a high plant throughput, which leads to a relatively high
ground level concentration impacting a small area very near the plant. On the
other hand, the secondary copper smelter has a relatively tall stack with high
temperature flue gas which results in a comparable ground level concentration,
but at a significantly greater distance from the plant. The area impacted by
this concentration is much greater.
In addition to estimating ground level concentrations, EPA has pre-
pared a preliminary assessment of the potential cancer risks from inhalation
exposure associated with emissions from these facilities. A detailed discussion
of the risk assessment is not included in this report, however, due to the con-
cerns raised by EPAfs Science Advisory Board (SAB) during their review of the
study. The SAB cautioned that risks were likely to be higher than estimated if
other exposure pathways, in addition to inhalation, were considered (e. g., food
chain) and if more sources had been tested. EPA agrees with these comments and
-20-
-------
is currently developing a procedure to consider the risks associated with secon-
dary pathways of exposure. Further testing of other sources may be considered
as the Agency moves forward with its ongoing effort to decide whether CDDs or
CDFs should be listed as a hazardous air pollutant.
The results of the Tier 4 stack test program, along with the prelim-
inary risk assessments, have been provided to the appropriate State air pollution
control agencies for their information and use.
5. Tier 4 Ash Sampling Results
Three different types of ash samples were collected: bottom ash, fly
ash, and scrubber water effluent. Bottom ash is the residue left in the combus-
tion chamber as a result of the combustion process. Fly ash is the material
collected by air pollution control devices which would otherwise be released to
the ambient air. Scrubber water effluent samples are samples obtained from wet
scrubbers, an air pollution control device which uses water to filter both
particulate and gaseous pollutants from the exhaust gas stream.
The results of the ash sample analysis for the 75 sites for Tier 4 are
summarized in Tables 9 and 10. Table 9 presents data from the source categories
with detectable values of 2378-TCDD equivalent while Table 10 is a listing of the
source categories where 2378-TCDD equivalent was not detected in the ash. A
total of 90 samples were analyzed from the 75 sites.
CDDs and CDFs were found in about one third of the bottom ash and fly
ash samples and.one half of the scrubber effluent samples. The highest concen-
trations were typically found in fly ash samples. Ash samples were collected
from 21 different source categories. Twelve of the source categories had one
or more ash samples with a detectable concentration.
It is presently difficult to interpret the significance of the ash
data from an air pollution perspective. One of the objectives of the study was
-21-
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TABLE 9. TIER 4 ASH SAMPLING RESULTS
Source Category/Source Sampled
Wire Reclamation Incinerator
Source-C
Source- A
Source-A
Source-A
Source-A
Source-B
Source-D
Secondary Copper Smelter
Source-B
Source-A
Wood Fired Boiler
Source-A
Source-C
Source-B
Source-D
Source-A
Source-E
Source-F
Source-G
Source-H
Municipal Waste Combust or
Source-C
Source-D
Source-B
Source-B
Source-B
Source-C
Hazardous Waste Incinerator
Source-B
Source-A
Source-C
Carbon Regeneration Furnace
Source-C
Source-A
Source-B
Sample Type
Fly Ash
Fly Ash
Bottom Ash
Fly Ash
Bottom Ash
Fly Ash
Fly Ash
Fly Ash
Fly Ash
Fly Ash
Fly Ash
Fly Ash
Scrubber Effluent
Bottom Ash (2 Samples)
Fly Ash
Fly Ash '
Fly Ash
Fly Ash
Fly Ash
Fly Ash
Scrubber Effluent
Scrubber Effluent
Bottom Ash
Scrubber Effluent
Scrubber Effluent
Bottom Ash
Scrubber Effluent
Fly Ash
Fly Ash
Scrubber Effluent
2378-TCDD
Equivalent
(ppb)
656a
87
32
21
4
0.3
NDb
117a
13
158
135
51
0.1
ND
ND
ND
ND
ND
142
44
4
3
0.3
0.1
42.9
ND
ND
18
0.1
ND
-22-
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TABLE 9 (CONTINUED). TIER 4 ASH SAMPLING RESULTS
Source Category/Source Sampled
Sewage Sludge Incinerator
Source-C
Source-F
Source-B
Source-A
Source-C
Source-C
Source-D
Source-G
Source-H
Source-I
Source-J
Industrial Waste Incinerator
Source-A
Commercial Boiler
Source-B
Source-A
Hospital Incinerator
Source-D
Source-B
Source-A
Source-D
Source-C
Drum and Barrel Furnace
Source-B
Source-E
Source-C
Source-A
Source-B
Source-D
Sample Type
Scrubber Effluent
Scrubber Effluent
Bottom Ash
Bottom Ash
Bottom Ash
Scrubber Effluent
Scrubber Effluent
Bottom Ash
Bottom Ash
Bottom Ash
Scrubber Effluent
Bottom Ash
Fly Ash
Fly Ash
Fly Ash
Fly Ash
Bottom Ash
Bottom Ash
Bottom Ash
Bottom Ash
Bottom Ash
Bottom Ash
Bottom Ash
Bottom Ash
Bottom Ash
1
Apartment House Incinerator
Source-A
Source-B
Source-C
Source-D
Bottom Ash
Bottom Ash
Bottom Ash
Bottom Ash
2378-TCDD
Equivalent
(ppb)
8
5
0.1
ND
ND
ND
ND
ND
ND
ND
ND
2
1
ND
0.9
0.6
0.4
0.4
ND
0.5
0.3
0.2
ND
ND
ND
0.3
0.1
ND
ND
aThese values are estimated. The true values may be higher.
bND - Not detected, generally less than 0.08 ppb.
-23-
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TABLE 10. TIER 4 SOURCE CATEGORIES WITH BELOW
DETECTION LIMIT ASH SAMPLE RESULTSa
Source Categories Sampled
Charcoal Grill
Charcoal Manufacturing Oven
Kiln Burning Hazardous Wastes
Kraft Paper Recovery Boiler
Open Burning/Accidental Fires
Small Spreader Stoker Coal Fired Boiler
Sulfite Liquor Boiler
Utility Boiler
Wood Stove
Number of Samples
Fly
Ash
-
2
3
6
-
3
-
3
-
Bottom
Ash
2
1
-
-
2
1
-
-
3
Scrubber
Effluent
-
-
-
-
-
4
-
-
Detection limit generally less than 0.08 ppb. Listed
alphabetically.
24-
-------
to determine a correlation between fly ash and stack emission concentrations.
While the presence of CDDs and CDFs in the fly ash appears to be a good indicator
of the presence of CDDs and CDFs in the stack emissions, no quantitative rela-
tionship has yet been observed that could reliably predict the magnitude of CDD/
CDF emissions in the stack gases.
A comparison of the data from sources with both fly ash and stack test
samples is provided in Table 11. This table illustrates the apparent lack of
correlation between the two types of samples. For example, the secondary copper
smelter* which had significantly higher stack concentrations than any other
source, has fly ash concentrations more than an order of magnitude lower than
some other sources. Other sources with relatively low stack emissions had
fairly high fly ash concentrations. At this time, ash data do not appear to be
a reliable indicator of the relative magnitude of CDD/CDF emissions in the
stack. Fly ash samples, on the other hand, are believed to be fairly reliable
indicators of the presence of CDDs/CDFs in stack emissions.
The ash sampling results have been transmitted through EPA's Regional
Offices to the appropriate State and local agencies for their consideration.
Although of limited usefulness for air pollution control purposes, the data do
provide a measure of the level of contamination in the ash that is disposed of
as a solid waste.
Findings And Conclusions
This investigation Included a review of information in the literature, as
well as a special sampling program designed to collect data for combustion
source categories believed to have the greatest potential to emit CDDs and CDFs.
The findings from this investigation are presented below.
(a) CDDs and CDFs have been detected in the stack emissions from most,
though not all, combustion source categories tested to date. All of the sources
-25-
-------
TABLE 11. COMPARISON OF ASH AND STACK EMISSIONS
AT SOURCES WITH CONCURRENT MEASUREMENTS
Source
Wood Fired Boiler
Municipal Waste Combustor - Plant C
Secondary Copper Smelter
Industrial Carbon Regenerator
Kraft Paper Recovery Boiler C
Kraft Paper Recovery Boiler A
2378-TCDD Equivalents
Fly Ash
(ppb)
158
142
13
0.1
ND
ND
Stack Emissions
(ng/dscm @ 3% 02)a
29
5.7
3900b
0.31
0.12
0.01
ng/dscm @ 3Z Oo » Nanograms per standard cubic meter of flue gas,
normalized to 5 percent oxygen.
°These values are estimated. The true values may be higher.
-26-
-------
stack tested under Tier 4, and most of the combustion source categories tested by
others reported in the literature, had detectable concentrations of CDD's and
CDF's.
(b) There is considerable variability in the emission rates among
source categories. For example, measured CDD emissions ranged more than four
orders of magnitude from "nondetected" at seven coal fired power plants tested
(detection limit at less than 1 ng/dscm) to approximately 16,000 ng/dscm of
total CDDs at a secondary copper smelting facility. Most of the combustion
source categories fell within an intermediate range, generally two to three
orders of magnitude less than the concentrations at the secondary copper smelting
facility.
(c) EPA has not yet determined the magnitude of the potential popula-
tion risk from these sources. An effort is underway to consider risk from all
routes of exposure (e. g., inhalation, ingestion, dermal contact) and for
evaluating procedures for estimating nationwide impacts from these sources.
(d) The presence of CDD/CDF in the fly ash from a control device
appears to be a good indicator of the likely presence of CDD/CDF in the stack
emissions. However, at the present time, it does not appear that the ash samples
can be used to reliably estimate the magnitude of CDD and CDF stack emissions
from a source. Continued use of expensive stack test methods appears necessary.
Continuing Efforts
Although the Tier 4 study has been completed, the Agency plans a number of
continuing efforts with respect to CDD emissions from combustion sources. These
Include:
-27-
-------
(a) EPA has a project underway to respond to the requirements of Sec-
tion 102 of the Hazardous And Solid Waste Act of 1984 concerning CDD emissions
from municipal waste combustors. This effort is intended to identify design and
operating guidelines to minimize CDD emissions.
(b) On July 7, 1987, EPA published in the Federal Register an Advance
Notice of Intent to Propose Regulations on air emissions from new or modified
municipal waste combustors under Section lllb of the Clean Air Act. EPA intends
to regulate one or more designated pollutants thus invoking Section 11Id of the
Clean Air Act.
(c) EPA plans to continue its evaluation of CDD/CDF emissions from
various sources. EPA has not yet determined whether CDD/CDF should be listed
as a hazardous air pollutant under Section 112 or other wise regulated under
other Sections of the Clean Air Act.
(d) EPA is continuing its efforts to standardize and refine stack
sampling and analysis procedures to reflect improvements in the state of the
art. The recommended ASTM stack test methodologies for municipal waste com-
bustors are currently being validated by the Agency.
Additional Information
Including this report, a total of twenty-two reports have been published
under this study. "National Dioxin Study Tier 4 - Combustion Sources" is
common to the title of each report. Abbreviated titles together with the EPA
Report Numbers are presented below.
TITLE REPORT NUMBER
Project Plan 450/4-84-014a
Initial Literature Review 450/4-84-014b
Sampling Procedures 450/4-84-014c
Ash Sampling Program 450/4-84-0144
Quality Assurance Project Plan 450/4-84-014e
-28-
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Quality Assurance Evaluation
Project Summary Report
Engineering Analysis Report
Final Literature Review
Test Report Site 1 SSI-A
Test Report Site 2
Test Report Site 3
Test Report Site 4
Test Report Site 5
ISW-A
SSI-B
BLB-A
BLB-B
Test Report Site 6 WRI-A
Test Report Site 7 WFB-A
Test Report Site 8 BLB-C
Test Report Site 9 CRF-A
Test Report Site 10 MET-A
Test Report Site 11 DBR-A
Test Report Site 12 SSI-C
Test Report Site 13 WS-A
450/4-
450/4-
450/4-
450/4-
450/4-
450/4-
450/4-
450/4-
450/4-
450/4-
450/4-
450/4-
450/4-
450/4-
450/4-
450/4-
450/4-
84-014f
fi4-014g
84-014h
84-014i
84-014J
84~014k
84-0141
84-014m
84-014n
84-014o
84-014p
84-014q
84-014r
84-014s
84-014t
84-014u
84-014v
Readers seeking more detailed information should obtain the specific
report(s) of interest. The Engineering Analysis Report (EPA-450/4-84-014h) is
the primary detailed technical report resulting from the Tier 4 study.
-29-
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REFERENCES
1. Dioxin Strategy, Office of Water Regulations and Standards and the Office
of Solid Waste and Emergency Response, U. S. Environmental Protection
Agency, Washington, DC, November 28, 1983.
2. National Dioxin Study, Tier 4 - Combustion Sources: Initial Literature
Review And Testing Options, EPA-450/4-84-014b, Office of Air Quality
Planning and Standards, U. S. Environmental Protection Agency, Research
Triangle Park, NC, October 1984.
3. National Dioxin Study, Tier 4 - Combustion Sources, Project Plan, EPA-
450/4-84-014a, Office of Air Quality Planning and Standards, U. S.
Environmental Protection Agency, Research Triangle Park, NC, February
1985.
4. National Dioxin Study, Tier 4 - Combustion Sources, Ash Program, EPA-
450/4-84-014d, Office of Air Quality Planning and Standards, U. S.
Environmental Protection Agency, Research Triangle Park, NC, January
1985.
5. National Dioxin Study, Tier 4 - Combustion Sources, Sampling Procedures,
EPA-450/4-84-014c, Office of Air Quality Planning and Standards, U. S.
Environmental Protection Agency, Research Triangle Park, NC, October
1984.
6. National Dioxin Study, Tier 4 - Combustion Sources, Quality Assurance
Project Plan, EPA 450/4-84-014e, Office of Air Quality Planning and
Standards, U. S. Environmental Protection Agency, Research Triangle
Park, NC, June 1985.
7. Analytical Procedures And Quality Assurance Plan For The Analysis Of
Tetra Through Octa Chlorinated Dibenzo-p-dioxln And Dibenzofurans In
Samples From Tier 4 Combustion And Incineration Process, Addendum To
Analytical Procedures and Quality Assurance Plan for the Analysis of
2,3,7,8-TCDD in Tier 3-7 Samples of the U. S. Environmental Protection
Agency's National Dioxin Study, EPA/600/3-85/019, Environmental Mon-
itoring Systems Laboratory, U. S. Environmental Protection Agency,
Research Triangle Park, NC, May 1986.
8. National Dioxin Study, Tier 4 - Combustion Sources, Quality Assurance
Evaluation, EPA-450/4-84-014f, Office of Air Quality Planning and
Standards, U. S. Environmental Protection Agency, Research Triangle
Park, North Carolina, January 1986.
9. National Dioxin Study, Tier 4 - Combustion Sources, Final Test Report -
Site 10 Secondary Copper Recovery Cupola Furnace MET-A, EPA-450/4-84-014s,
Office of Air Quality Planning and Standards, U. S. Environmental Protec-
tion Agency, Research Triangle Park, NC, April, 1987.
-30-
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10 National Dioxin Study, Tier 4 - Combustion Sources, Final Literature
Review, EPA-450/4-84-0141, Office of Air Quality Planning and Standards,
U. S. Environmental Protection Agency, Research Triangle Park NC June
1986. '
11 Interim Procedures For Estimating Risks Associated With Exposures To
Mixtures Of Chlorinated Dibenzo-p-dioxin and - Dibenzofuran (CDDs and
CDFs), EPA/625/3-87/Q12. Risk Assessment Forum, IJ. s. F.nv-t rnnm0nt:ai
Protection Agency, Washington, DC, March 1987.
12 Health Assessment Document For Polychlorinated Dibenzo-p-dioxin. EPA-600/
8-84014f, Office of Health and Environmental Assessment, U. S. Environ-
mental Protection Agency, Washington, DC, September 1985.
-31-
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TECHNICAL REPORT DATA
(Please read Instructions on the reverse before completing)
i. REPORT NO.
EPA-45Q/4-84-014g
3. RECIPIENT'S ACCESSION NO.
4. TITLE AND SUBTITLE
National Dioxin Study Tier 4
Project Summary Report
- Combustion Sources
5. REPORT DATE
September 1987
6. PERFORMING ORGANIZATION COOE
7. AUTHOR(S)
Edward J. Lillis, James H. Southerland,
William H. Lamason and William B. Kuykendal
8. PERFORMING ORGANIZATION REPORT NO,
3. PERFORMING ORGANIZATION NAME ANO AOORESS
Air Management Technology Branch (MD-14)
Monitoring And Data Analysis Division
Research Triangle Park, NC 27709
10. PROGRAM ELEMENT NO.
11. CONTRACT/GRANT NO.
12. SPONSORING AGENCY NAME ANO AOORESS
U.S. Environmental Protection Agency
OAR, OAQPS, MDAD, AMTB (MD-14)
Research Triangle Park, NC 27711
13. TYPE OF REPORT AND PERIOD COVERED
Final
14. SPONSORING AGENCY COOE
15. SUPPLEMENTARY NOTES
Input to the National Dioxin Strategy Report To Congress
This report presents the Agency's finding on the assessment of dioxin emissions
from combustion sources under Tier 4 of the National Dioxin Strategy. The primary
objectives of Tier 4 are outlined in the report. The report describes the informa-
ation the Agency collected at the request of Congress to improve the current under-
standing of combustion sources which emit dioxin to the ambient air. The tasks used
to collect the information are outlined, including stack testing, ash sampling and
data analysis. References to other documents which describe methods, procedures and
detailed analyses are identified.
The report finds that small amounts of chlorinated dibenzo-p-dioxins and
dibenzofurans are emitted from many combustion sources, with only a few sources
emitting larger amounts. These sources include municipal waste incinerators,
secondary copper smelters and sewage sludge incinerators.
17.
KEY WORDS ANO DOCUMENT ANALYSIS
DESCRIPTORS
b.IDENTIFIERS/OPEN ENDED TERMS
c. COSATI Field/Group
CDF
Dioxins
Furans
TCDD
TCDF
2378-Tetrachlorodibenzo-p-dioxin
Tier 4
Sewage Sludge
Secondary Copper
3mdit!H
Combustion Sources
Unlimited
19.
Hnrl
20.
21. NO. OF "PAGES
38
22. PRICE
Unclassified
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