Vi,"/
United States
Environmental Protection
Agency
Risk Reduction
Engineering Laboratory
Cincinnati OH 45268
Research and Development
EPA/600/S2-88/056 Jan. 1989
&EPA Project Summary
Engineering Assessment of
EDB Pesticide Destruction
Technologies
Sunil H. Ambekar and Bernard A. Laseke
Under the authority of the Federal
Insecticide, Fungicide, and Rodenti-
cide Act, the U.S. Environmental
Protection Agency (EPA) suspended
and cancelled the registrations and
prohibited the further use, sale, and
distribution of ethylene dibromide
(EDB) pesticide formulations. As a
part of this ban, EPA also assumed
the responsibility for destroying/
disposing of existing EDB stocks.
The project covered by this report
involved an engineering evaluation of
the suitability of various available
technologies for the destruction of
ethylene dibromide pesticides. The
purpose of the study was to highlight
the technical merits and short-
comings, safety, cost, and total time
requirement for each of the alter-
natives considered.
Both thermal and chemical
destruction options were considered.
Evaluation criteria were developed so
that the different options could be
compared on a common basis.
Information was collected on each
candidate process through a
literature search and discussions
with industry experts. Concurrent
with these efforts, bench-scale
tests of the chemical methods were
conducted. Also, a test burn was
made at a commercial facility to
determine the effectiveness of one of
the incineration options. The results
of these tests were factored into this
report. Because the chemical
processes are still in the conceptual
stages, only preliminary process
calculations and cost estimates were
developed for these processes.
Based on the results of this study,
incineration in the presence of sulfur
dioxide appears to be the best
alternative for the safe, effective,
rapid, and economical destruction of
the ethylene dibromide pesticides.
This Project Summary was devel-
oped by EPA's Risk Reduction Engi-
neering Laboratory, Cincinnati, OH, to
announce key findings of the research
project that is fully documented in a
separate report of the same title (see
Project Report ordering information at
back).
Introduction
In September 1983 and February 1984,
the U.S. Environmental Protection
Agency (EPA) suspended the registra-
tions of ethylene dibromide (EDB)
pesticide formulations. Later, further use,
sale, and distribution of these formu-
lations were prohibited. This action was
taken under the authority of the Federal
Insecticide, Fungicide, and Rodenticide
Act (FIFRA). As part of this regulatory
action, the EPA issued orders that halted
the use of EDB-containing material and
requested manufacturers and distributors
to recall all existing EDB products. The
EPA was also required to indemnify all
registrants and other owners of EDB
pesticides for their economic losses and
to take responsibility for the destruc-
tion/disposal of the EDB stocks.
The quantity of formulated EDB
pesticides identified for disposal totalled
approximately 346,000 gallons or 3.7
million pounds, 1.1 million pounds of
which was actually EDB. For purposes of
background information, the various EDB
formulations are divided into four cate-
-------
gories. These categories and their
associated approximate quantities are
shown below:
1.
2.
3.
4.
Category
CS2-containing
formulations
Chloropicnn-contain-
ing formulations
Methyl bromide-con-
taining formulations
Miscellaneous
formulations
Quantity,
103 gallons
132
70
19
125
Technical Approach
The efforts of this study were focused
on the following steps:
1. An engineering evaluation was made,
which involved the identification of
candidate technologies and pro-
cesses, the development of selection
criteria, and the application of
selection criteria to support technical
judgments.
2. Vendor contacts were made to the
various incineration facility operators
to determine interest, feasibility, and
cost to destroy the EDB formulations.
3. Preliminary process designs and cost
estimates were developed for the
selected chemical destruction
processes in order to compare these
processes to the incineration pro-
cesses on an equal basis.
4. Process design and cost packages
were developed by working closely
with the EPA process developers.
Bench-scale performance data were
used to support equipment design
and operating assumptions.
5. The results of a parallel bench-scale
laboratory study were factored into the
analysis to support and expand the
EPA bench-scale work.
6. A trial burn of two EDB formulations
was separately contracted for by the
EPA to obtain more information on
incineration in the presence of sulfur
dioxide (SOj) to facilitate bromine
scrubbing. Data from this test were
then factored into the evaluation of all
alternatives.
Evaluation Criteria
The aim of the evaluation was to
highlight the technical merits and
shortcomings, safety, cost, and total
required time for each of the alternatives
considered. To provide a common basis
to compare different process options, the
following evaluation criteria were
developed in consultation with the EPA:
- Status - Commercial, Pilot Scale, or
Conceptual
- Accessibility
- Past Experience
- Need for Development and Testing
- Preprocessing
- Process Safety
- Toxic Emissions
- Residues
- Need for New/Additional Equipment
- Extent of Corrosion
- Process Compatibility with Pesticides
- Secondary Environmental Impact and
Health Considerations
- Mechanical Reliability
- Transportational Access to Facility
- Storage and Handling of Pesticides
and Residues
- Cost
- Permitting
- Probability of Success
- Time for Completion
Information was collected on each
candidate process so that each item in
the evaluation criteria could be ad-
dressed. This entailed an exhaustive
literature survey, discussions with
industry experts, process calculations,
and preliminary cost estimates.
Cost Estimating Procedure
Process economics is an important
factor in the ultimate selection of a
technology. For comparison of the cost-
effectiveness of each option, unit costs
($/lb of pesticide) were established for
each process option. Unit costs for
technologies already commercialized
(incineration and cement kiln incin-
eration) were obtained by contacting
vendors for their best possible estimates.
With regard to chemical destruction, both
available process options available are
still in the conceptual stages. Based on
laboratory-scale results, preliminary
flow sheets were developed, and then
preliminary process design and prelim-
inary cost estimates were made.
Technologies Evaluated
The following technologies were
selected in this engineering evaluation as
possible candidates for the elimination of
EDB pesticide formulations:
(1) Incineration in a waste incinerator
under oxidizing (excess air) condi-
tions (conventional incineration)
(2) Starved-air incineration
(3) Incineration in the presence of sulf
dioxide or sulfur-containing waste
(4) Incineration in a cement kiln
(5) Chemical destruction by the ATE
process
(6) Chemical destruction with the zir
process
Conventional Incineration
(Excess-Air Incineration)
Conventional incineration is the mo
common way of destroying hazardoi
substances. Numerous commercial ha.
ardous waste incinerators are operatin
successfully throughout the United State
and worldwide. Some of these operatin
systems are transportable, which make
them convenient for the destruction <
hazardous wastes at specific sites.
This process uses combustion t
oxidize hazardous materials to harmles
or less toxic materials. Products (
incineration consist of combustion gase
and, in some cases, solid residues. Th
combustion products usually requir
secondary treatment, such as we
scrubbing, particulate collection, or th
use of afterburners. Unlike fluorine an
chlorine, which generate primaril
hydrogen halides upon combustion i
excess air, brominated wastes general
bromine when incinerated, which i
difficult to remove from the flue gases b
currently operational gas-processin
techniques. Caustic is typically used a
the scrubbing medium in many haa
ardous waste incinerators; however, it i
believed that a caustic solution may nc
remove bromine as readily as it doe
hydrogen bromide. Therefore, modifice
tion of the incinerator operating cor
ditions (e.g., addition of sulfur) will b
required to prevent significant amounts c
bromine emission into the atmosphere.
Incineration in Presence of
Sulfur Dioxide or Sulfur-
Containing Waste
This option entails burning halogenatei
waste in a conventional incinerator in thi
presence of sulfur dioxide or sulfur
containing wastes. Under the incinerate
operating conditions, sulfur dioxide react:
with the halogen produced durini
incineration to form hydrogen halide am
sulfuric acid. During the Rollins test buri
on EDB stock, 10 percent sulfuric acii
(H2SC-4) was used as the source o
sulfur. Under the kiln conditions, thi
H2SC-4 decomposes as follows (Equa
tions 1 and 2):
-------
2 H2S04
2 S03
2H2O
A
2S03
2 S02 + 02
(1)
(2)
At high temperatures, the equilibrium
reaction is displaced to the right, which
favors decomposition. The bromine
resulting from oxidation of EDB reacts
with S02 and water to form hydrogen
bromide (HBr) and H2S04.
C2H4Br2 + 302---A_
2 C02 + 2H2O
Br2
(3)
Br2 -t-S02 + 2 H20 ------ >
2 HBr + H2S04 (4)
The resulting acids can be easily
removed in the scrubbers, eliminating
the problem of halogen emissions
Starved-Air Incineration
This option uses the same equipment
and entails the same process flow as the
conventional incineration process The
only difference lies in the process
conditions in the incinerator Unlike
conventional incineration, starved-air
incineration uses less than stoichiometric
quantities of air for combustion purposes.
The bromine/hydrogen bromide
chemical equilibrium favors hydrogen
bromide formation under reducing
conditions (less oxygen) with high water
vapor in the furnace Because hydrogen
bromide is more easily scrubbed than is
bromine, the possibility of toxic
emissions due to bromine is lessened
Thus, conceptually, starved-air incin-
eration appears to have the potential to
destroy brommated wastes.
Cement Kiln
The primary cost factor in the pro-
duction of cement is energy, which
accounts for as much as 40 percent of
the total cost To offset escalating fuel
costs, cement kilns use hazardous waste
fuels, however, not all incinerable waste
can be burned in a cement kiln Cement
kilns, which operate at 2000° to 2300°F,
have a history of successful incineration
of chlorinated waste without any harmful
emissions. The hydrogen chloride and
chlorine generated in the furnace react
with the raw materials (lime and some
sodium and potassium in the ore) to form
chloride salts. The alkaline conditions in
the kiln cause the reactions to be rapid
and complete. Thus, although many kilns
are not equipped with wet scrubbing
systems, the kiln acts as its own
scrubber to minimize toxic emissions.
Similar results are expected with bro-
minated wastes.
ATEG Process
The ATEG process, developed by the
EPA involves a reaction between EDB
and sodium hydroxide (NaOH) in the
presence of a phase transfer catalyst,
tetraethylene glyco! (TEG) to yield
acetylene, bromide salts, and water.
Laboratory-scale studies on this
reaction system were carried out by the
EPA and the major findings were as
follows
- The reaction proceeds m two steps,
with vinyl bromide as an intermediate
product. A very small percentage of
the vinyl bromide reacts further in the
reactor to yield acetylene The vinyl
bromide had to be treated in a
scrubber with the KTEG solution (KOH
dissolved in TEG, diluted by water) to
achieve complete conversion to
acetylene. Thus, the reaction mecha-
nism is as follows'
Br-CH2-CH2-Br + NaOH >
Br-CH = CH2 + NaBr + H20 (5)
Br-CH = CH2 + KOH >
CH^CH + KBr + H20 (6)
The overall reaction mechanism may be
represented as follows
Br-CH2-CH2-Br + 2 NaOH >
CH^CH + 2 NaBr -t- 2 H20 (7)
- Laboratory tests seem to indicate
relatively rapid reaction between the
reactants
- Carbon disulfide (CS2), a constituent of
some of the pesticide formulations,
was found to react quantitatively with
the ATEG to form a viscous sludge
that inhibited the EDB destruction
reaction.
- Chloropicrin, a major constituent m
some formulations, was found to react
with the catalyst TEG, inhibiting the
EDB destruction reaction.
Therefore, the constituents that impede
the reaction will have to be removed to
successfully dispose of the pesticide
formulations. It is believed that distillation
of the CS2 formulations should not be a
problem, although distillation of chloro-
picrm formulations could be difficult. An
advantage with distillation is that the
products of distillation could be sold at
market value and improve the overall
process economics.
Based on the data available, a flow
sheet was developed in consultation with
the EPA. The process was proposed to
be a batch operation consisting of a
reactor, a packed bed scrubber (to treat
reactor gases) system, and a reactor
effluent dewatermg (filters) and storage
system Preliminary process calculations
and cost estimates were then developed
to evaluate the process.
Two economic options have been
considered for this process. The first
involves building a completely new
facility with all new equipment. The
second involves using some process
equipment available at the GARD facility
(reactors, flare, and stack) to be used
along with some new equipment.
Zinc Process
This process entails a classical organic
reaction for the dehydrohalogenation of
halogenated orgamcs. Metallic zinc
reacts with EDB at ambient temperatures
to produce ethylene gas and zinc
bromide. The reaction is represented as
follows
Zn + Br -CH2-CH2-Br ->
ZnBr2 + CH2 = CH2 (8)
The reaction has been demonstrated
only on a laboratory scale by the EPA.
The Laboratory-scale studies resulted in
99 + percent EDB destruction. During
these experiments, optimal results were
obtained by using 100- to 200-mesh
zinc powder slurned in distilled water and
a little hydrochloric acid. The reaction
temperature was not allowed to exceed
113°F
The reaction is exothermic, with very
high heat of reaction. It has been
suggested that the reaction temperature
-------
should be maintained below 113°F to
avoid any possibility of runaway reac-
tions.
Like the ATEG process, a conceptual
flow sheet was developed for this
process. It was proposed to operate the
process as a batch operation. Preliminary
process calculations and cost estimates
were developed to evaluate the process.
Two capital investment alternatives are
possible for this process. The first
alternative entails the construction of a
completely new facility with all new
equipment. Under the second alternative,
some equipment from the GARD facility
would be used in conjunction with new
equipment.
Results and Discussion
The results of the engineering
evaluation are summarized in Table 1.
From a technical standpoint, both
starved-air incineration and destruction
m an existing incineration facility without
any modifications appear to be infeasible
because of the bromine emissions that
would exit through the stack.
Incineration in the presence of sulfur-
containing waste holds an excellent
promise for the elimination of bromine
emissions. The test burn results show
that this option meets the destruction
standards for POHCs (DREs greater than
99.9999 percent) and emission standards
(bromine below detection limits and
bromide about 20 ng/dscf in the stack).
Also, continuous monitoring data for
CDs, 02, CO, NOX, and S02 were
reportedly well within the established
standards. Bromine mass balance results
seem to indicate that all the bromine
exits the system in the scrubber water.
Also, the fact that a currently operating
incineration facility in Europe is
successfully using this technology to
destroy halogenated waste lends
credibility to this option. Moreover, this
option offers the advantage of speedy
disposal of the entire EDB stock
(probably less than a year) at a
competitive cost. This is especially
important in view of the urgency of the
situation.
Cement kiln incineration appears to be
a promising option; however, extensive
testing would be required to establish the
performance capabilities and optimal
waste feed rates. The optimal waste feed
rate would have to be determined so as
to eliminate bromine emissions in the
flue gases while not having an adverse
effect on product quality. If the allowable
feed rate was low, the overall time to
complete the job would be higher This,
in turn, could increase the overall cost of
this option; however, no definitive
estimates can be made until after test
burns are performed.
The ATEG process has shown
excellent capability to eliminate the EDB
in bottoms obtained from the distillation
of the CS2 formulations. Previously the
treatment of chloropicrin formulations
with the ATEG process was regarded
infeasible because of fear of forming
unknown, and perhaps more hazardous
compounds. However, preliminary tests
seem to suggest that it may be possible
to treat these formulations, without
reacting the chloropicrin, by using a 30
percent caustic solution. This approach,
however, needs further testing to prove
its validity The bench-scale tests seem
to indicate that the presence of other
constituents in the pesticide formulations
interfere with the EDB destruction. Thus,
extensive tests would also be required to
study the feasibility of treating the
miscellaneous formulations, without
preprocessing them. Despite the
promising results on the laboratory scale,
the ATEG process could create
operational problems because of its
complexity. The process involves:
- A two step reaction.
- Number of reactants (NaOH, KOH,
TEG)
- It is found to be sensitive to a number
of operating parameters like the TEG
concentration, caustic concentration,
temperature, etc.
- Handling of potentially hazardous
substances like vinyl bromide, etc.
- The process forms a wide range of
byproducts, which could make dis-
posal of the effluents difficult
It is therefore evident that the process
would need very extensive testing to
eliminate uncertainties and operational
difficulties and establish the optimal
operating conditions, prior to design and
scale-up. This could take considerable
time, causing a delay in the overall
disposal of the EDB pesticides.
Bench-scale tests with the zinc
process show excellent promise with
pure EDB. Disposal of the chloropicrin
formulations seems to be a problem
because of unacceptable levels of DREs,
formation of unknown products, high zinc
consumption, and high hydrochloric acid
consumption. Reaction of zinc with the
CS2 formulations show that the carbon
disulfide reacts rapidly with the zinc,
resulting in very poor destruction of EDB.
In all the tests with the zinc process, long
reaction times were required to achieve
substantial EDB destruction. Even lone
reaction times may be required
achieve 99.99 percent destructions. T\
could potentially make the proce
infeasible. Therefore, more tests wot
be required to determine:
- Ways to achieve 99.99 perce
destruction with all formulations, wil
out any preprocessing. CS2 may ha
to be removed prior to treatment.
- Ways to reduce the acid and zn
consumption, especially with tl
chloropicrin formulation.
- Feasibility of an azeotropic distillatii
of chloropicrin formulations usir
alcohol, as suggested by IT, if tl
99 99 percent destruction of tt
formulation is not possible.
- The overall reaction time. This is ;
exothermic reaction. Thus, if tt
reaction rate is fast, then heat transf
will control the overall rate and vie
versa. This will affect the proce;
design and cost.
It is therefore evident that this proce;
would need thorough pilot-plant testir
to establish its feasibility and optimu
operating conditions prior to design ar
scale-up. The process is more compk
than previously envisaged.
Conclusion
At this point in time, incineration in tr
presence of sulfur dioxide seems to t
the most viable and rapid way i
disposing the pesticide formulations at
cost comparable to or lower than othi
methods. Successful trial burns for th
method have been completed. As
result, the destruction process can b
initiated immediately. The overall time f<
disposal should be less than six month
In view of the urgency for disposing i
the pesticides, this process appears to fc
clearly the best choice.
The full report was submitted in parti
fulfillment of Contract No 68-03-338
by PEI Associates, Inc , under th
sponsorship of the U.S Enviornment.
Protection Agency.
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Sun// H. Amberkar and Bernard A. Laseke are with PEI Associates, Inc., Cincinnati,
OH 45246.
Edward R. Bates, is the EPA Project Officer (see below).
The complete report, entitled "Engineering Assessment of EDB Pesticide
Destruction Technologies," (Order No. PB 89-110 118/AS; Cost: $21.95,
subject to change) will be available only from:
National Technical Information Service
5285 Port Royal Road
Springfield, VA22161
Telephone: 703-487-4650
The EPA Project Officer can be contacted at:
Risk Reduction Engineering Laboratory
U.S. Environmental Protection Agency
Cincinnati, OH 45268
United States
Environmental Protection
Agency
Center for Environmental Research
Information
Cincinnati OH 45268
BULK RATE
POSTAGE & FEES PAID
EPA
PERMIT No. G-35
Official Business
Penalty for Private Use $300
EPA/600/S2-88/056
0001961 HWER
LIBRARY REGION V
US EPA
230 S DEARBORN ST
CHICAGO IL
60604
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