xvEPA
                              United States
                              Environmental Protection
                              Agency
                              Municipal Environmental Research
                              Laboratory
                              Cincinnati OH 45268
                              Research and Development
                              EPA-600/S2-81-214  Oct. 1981
Project  Summary
                              Modification  of Spill  Factors
                              Affecting  Air  Pollution:
                              Volume  I. An  Evaluation  of
                              Cooling  as  a Vapor Mitigation
                              Procedure for  Spilled  Volatile
                              Chemicals

                              J. S. Greer, S. S. Gross, R. H. Hiltz, and M. J. McGoff
                               Spilled chemicals that pose a hazard
                              to the land and water ecosystem can
                              also provide a significant vapor hazard.
                              Although the vapors released by such
                              chemicals may ultimately be dispersed
                              in the environment with few long-
                              term effects, they do pose a hazard to
                              life and property downwind of the
                              spill.
                               Among the vapor amelioration tech-
                              niques that have been considered is
                              the use of a coolant to lower the
                              temperature of a spill and reduce its
                              equilibrium vapor pressure. This pro-
                              gram was conducted as a feasibility
                              study of that mechanism.
                               Four potential coolants were exam-
                              ined: water ice, dry ice, liquid carbon
                              dioxide, and liquid nitrogen. Further
                              evaluation based on laboratory studies
                              and limited scaled-up tests established
                              dry ice as the  most versatile coolant
                              choice. Water  ice does not cool suf-
                              ficiently.  Liquid nitrogen and carbon
                              dioxide require large quantities of
                              material and produce a dense obscur-
                              ing cloud that has some adverse impli-
                              cations. Dry ice avoids these problems
                              and is readily available at a reasonable
                              cost, but some method is required for
                              crushing and distributing the dry ice
                              on the spill. A prototype unit was thus
                              developed consisting of a crusher and
                              a pneumatic conveyor to perform
                              these functions.
                                A pool of diethyl ether with 2.23 m2
                              (250 ft2) of surface was cooled to
                              -60°C (-76°F) using 408 kg (900 Ib) of
                              dry ice fed at a rate of 13.6 kg/min (30
                              Ib/min). A measurable reduction in
                              downwind vapor concentration was
                              realized. Pool temperature was still
                              below -10°C (14°F) 2 hr after dry ice
                              discharge was terminated.
                                This program has established the
                              feasibility of the mechanism, but
                              additional work is necessary to estab-
                              lish practicality, define materials to
                              which cooling is applicable, and opti-
                              mize the dispensing equipment.
                                This Project Summary was devel-
                              oped by EPA's Municipal Environmen-
                              tal Research Laboratory, Cincinnati,
                              OH, to announce key findings of the
                              research project that is fully docu-
                              mented in a separate report of the
                              same title (see Project Report ordering
                              information at back).

                              Introduction
                                Many of the chemicals that pose a
                              hazard to the land and water ecosystem
                              when spilled can also provide a signifi-
                              cant vapor hazard. Although the vapors

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released  by such chemicals  may ulti-
mately disperse  into the environment
with little long term effect, they do pose
an immediate hazard to life and property
downwind of the spill. In  addition, a
hazard exists to those responding to the
spill who must remain in the area for the
duration of the incident.
  The vapor hazard from spilled chemi-
cals takes two forms: the release of toxic
fumes that pose a life hazard even at low
concentrations (parts per million), and
the release of flammable vapors where
minimum dangerous concentrations
are usually above 1%. Some chemicals
may exhibit both hazards, but toxicity,
with its lower allowable concentration,
will be the controlling feature.
  The  great difference in minimum
hazard levels creates two distinct prob-
lems. In the case of flammable  vapors,
small increments of reduction  can  be
meaningful. For toxic materials,  the
ability to  provide meaningful mitigation
of the hazard may lie only with reduction
of the equilibrium vapor pressure.
  A number of vapor amelioration tech-
niques have received consideration. A
review of the techniques conducted
under  U.S. Coast Guard sponsorship
shows that most are ineffective. The
techniques of mechanical covers,  in-
duced  air movement, vapor scrubbing,
and vapor phase reaction are in this
category. The techniques of foam blan-
keting and liquid phase modification are
the only ones that in their present state
of development have had any practical
demonstration and can pass the criteria
of cost, availability, deployment, and
application. The degree of vapor control
that can be achieved with these two
techniques is beneficial where flam-
mable vapors are the hazard. But where
the vapor hazard is one of  toxicity and
hazardous vapor  concentrations are in
the parts per million range, such tech-
niques are not adequate.
  Maintenance of vapor levels in the
parts-per-million range appears to
require a mechanism to reduce the
equilibrium vapor pressure. One poten-
tial mechanism  of vapor control may
achieve that end: the use of  a coolant.
Reducing the temperature of the spill
reduces the equilibrium vapor pressure
and the rate of vapor release per unit of
time.
  This technique has been addressed in
two programs, but no systematic inves-
tigation has been conducted. Based on
these  studies,  EPA inaugurated a de-
tailed program to evaluate the potential
of cooling and, if  warranted, to conduct
a simulated spill scenario to define
feasibility.

Discussion of Results
  This study establishes the basic
feasibility of the  cooling concept. A
literature search and data evaluation
delineated an extensive list of potential
coolants. Practical considerations of
cost, availability, safety, and field
handling reduced the candidate list to
four materials: wet ice (solid water), dry
ice (solid CO2), liquid  C02, and liquid
nitrogen.
  All four materials are readily available
from many sources on short notice and
at a  reasonable cost. The liquefied
gases, N2 and C02, can achieve signifi-
cant  reductions in the temperature of
the spill, but they are attended  by
certain disadvantages. These gases
require continuous application, and the
effect does not persist if application is
discontinued. The boiling of the liquid
exaggerates the vapor release from the
spilled material, negating some of the
benefits of cooling. Both materials
produce a dense obscuring cloud above
the spill surface. This cloud provides a
nonflammable atmosphere, but it is also
nonbreathable.
  Liquid CO2 can be released to form
solid C02, identified as COa snow. But
conversion is only 15 percent with
current technology, an obscuring cloud
is still generated.
  Wet ice has certain  advantages, but
its capability is limited to 0°C (32°F).  Ice
can react with some materials and will
cause a volume increase because of its
nonvolatility.
  Dry ice,  crushed and applied as a
particulate, initially showed the best
potential for effective, persistent cooling
with small material losses and minimal
cloud formation.  Further evaluation
supported  by laboratory studies and
limited  scaled-up tests were  able to
establish dry ice  as the best coolant
choice. The bases for this selection are
detailed in Table 1. The main comparison
was  the difference of the temperatures
achieved and the rate of  rise  after
coolant application was stopped. A
comparison using ethyl ether is shown
in Figure 1.

Results
  The laboratory results were encour-
aging, but they  were not sophisticated
enough to  establish the feasibility  for
field use. Field application necessitated
a mechanism to convert the standard
form of dry ice blocks (10x10x1 in.; 25
x 25 x 2.5 cm) to a particulate form and a
means for dispensing the particulates to
the spill surface. A review of commer-
cial equipment revealed several types ol
applicable equipment. After a limited
testing program, a commercial shredder/
crusher was selected. The shredder
operation was  modified in terms of the
speed of rotation and the configuration
of the tines to achieve a reasonable yield
of  particles within an acceptable size
range. The distribution covered fine
particulates to coarse material of 0.635
to  1.27 cm (1 /4 to 1 /2 in.). Because of
the problem of sublimation, a  true size
range could not be measured. Efficiency
in terms of material out versus material
in was in the range of 75%.
  Several concepts were evaluated for
dispensing the crushed dry ice. A snow
blower was  originally selected, but its
operation reduced the effective discharge
to 65%.  The  combination of snow
blower/crusher was a poor selection in
real time. The discharge distance was
not sufficient to allow operation from a
restricted location, and the machine
was difficult to manipulate around the
spill. A change was made to a pneumatic
conveyor, which was made up of an
auger feeding the particulate into an air
stream with forced discharge through a
hose.                               *
  The combination unit was  mounted
on a wheeled frame to provide mobility,
but the hose  discharge allowed  an
extended discharge  pattern from a
single location. Some additional mate-
rial losses were encountered,  reducing
efficiency to about  50%.
  Field tests were conducted using
diethyl ether as a spill simulant: 757 L
(200 gal) was spilled into a 7.62- by 6.1 -
m  (25- by 20-ft) impoundment. Dry ice
was charged at a rate of 13.61 kg/min
(30 Ib/min) for 30 min with an effective
application of 6.80 kg/min (15 Ib/min).
  The spill temperature was reduced in
that time to an averge of -60°C (-76°F),
which resulted  in a decrease of the
equilibrium vapor pressure from 440 to
4.0 mm of Hg. An absolute measure of
vapor reduction could not be  obtained
because of wind effects. The available
data show the  effective reduction in the
vicinity of the spill to be at least 75% of
the free spill value. Typical values show
a free spill vapor concentration of
10,000 ppm, which was reduced to 180
ppm by the dry ice application.

Conclusions
  The results of this program show that
dry ice can significantly reduce th

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fable 1.     Cryogen Comparisons
  Cryogen
                  Advantages
                 Disadvantages
 Liquefied
  Nitrogen
 Liquefied
  Carbon
  Dioxide
 Solid Carbon
  Dioxide
Ice
 1. Cheaper than COz on a per-pound basis
 2. Extremely low temperatures possible
 1. No storage losses
 2. Reasonable temperature reduction of spill
 1. Better cost advantage than liquid COz
   or liquefied Nz
 2. Less application loss than with LNZ or liquid
   COz
 3. Rapid cooling of spill
 4. No problems with COz cloud
 5. Can be projected over distances
 6. Readily available
 7. Safer than liquefied /V2 or liquefied COz to handle

 1. Safest to use
 2. Most readily available
 3. Can be projected
 1. Vapor losses occur on storage
 2. Nz cloud significantly reduces visibility
   and oxygen levels in vicinity of spill
 3. Larger quantities needed to cool spill than
   with solid COz
 4. Not as cost effective as solid COz
 5. Hazardous liquid may be entrained by Nz vapors

 1. Higher liquid COz losses occur upon
   application to the spill
 2. COz cloud significantly reduces visibility and
   oxygen levels in vicinity of spill
 3. More expensive than solid COz based on the
   amount actually applied to the spill

 1. Storage losses occur
 2. Grinding necessary before application
 1. Temperature of the spill is not reduced
   sufficiently
2. Increases the liquid volume of the spill when
   the ice melts
Liquefied
 Nitrogen
 1. Cheaper than COz on per pound basis
 2. Extremely low temperatures possible
Liquefied
 Carbon
 Dioxide
Solid Carbon
 Dioxide
Ice
 1. No storage losses
2. Reasonable temperature reduction of spill
 1. Better cost advantage than liquid COz
   or liquefied Nz
2. Less application losses than with LNz or
   liquid COz
3. Rapid cooling of spill
4. No problems with COz cloud
5. Can be projected over distances
6. Readily available
7. Safer than liquefied NZ or liquefied C02 to handle

1, Safest to use
2. Most readily available
3. Can be projected
1.  Vapor losses on storage
2.  Nz cloud significantly reduces visibility
   and oxygen levels in vicinity of spill
3.  Larger quantities needed to cool spill than
   solid COz
4.  Not as cost effective as solid COz
5.  Possible entrainment of hazardous liquid by
   Nz vapors

1.  Higher liquid COz losses upon application
   to the spill
2.  COz cloud significantly reduces  visibility and
   oxygen levels in vicinity of spill
3.  More expensive than solid COz on the basis of
   amount actually applied to the spill

1.  Storage losses
2.  Grinding necessary before application
                                                                      1.  Temperature of the spill is not reduced
                                                                         sufficiently
                                                                      2.  Increases the liquid volume of spill when the
                                                                         ice melts

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     20
    -20
    -40
 2
 Cb
 |  -60
   -80
  -100
  -120
                                               9.3 m2 (100 ft2) pond
                                               208 I (55 gal) diethyl ether
     -40
-20
20      40      60

     Time, min.
                                                      80
                                                 WO
120
Figure 1.    Subscale field test results with ethyl ether—temperature versus time
             (9.3 m2(100-ft2) pond, 208 L (55 gal) diethyl ether).
temperature of a spilled liquid with a
concomitant reduction in the vapor
release rate. Crushing the dry ice to an
acceptable particulate  level  and dis-
tributing it over the spill surface can be
achieved by state-of-the-art techniques.
  The equipment evolved in this pro-
gram required further  optimization.
Further study must be done on opera-
tion, configuration, and materials of
construction. The tests that have been
conducted are not sufficiently extensive
to show  clearly a practical,  efficient
operation in a  real-time  spill scenario.
But they do support continued investi-
gation and evaluation of the cooling
concept.
  The cooling concept is primarily suited
for use with materials that pose a toxic
vapor hazard rather than  a flammable or
explosive vapor hazard. In most cases,
aqueous foams provide effective mitiga-
tion for such materials.
  Foams are a  well developed technol-
ogy in common use by emergency
organizations, but they cannot provide
                           the degree of vapor control  necessary
                           where toxic levels are in the parts per
                           million range. This study provides a
                           basic guideline for further evaluation of
                           coolants.
                             The full report was submitted in
                           partial fulfillment of Contract No. 68-
                           03-2648,  Task 9A. by MSA Research
                           Corporation under subcontract to Rock-
                           well International under sponsorship of
                           the   U.S.  Environmental   Protection
                           Agency.

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J. S. Greer. S. S. Gross, P. H. Hiltz, and M. J. McGoff are with MSA Research
  Corporation, Evans City, PA 16033.
John E. Brugger is the EPA  Project Officer (see below).
The  complete report, entitled "Modification  of Spill Factors  Affecting Air
  Pollution: Volume I. An Evaluation of Cooling as a Vapor Mitigation Procedure
  for Spilled Volatile  Chemicals," (Order No. PB 82-108 382; Cost: $9.50,
  subject to change) will be available only from:
        National Technical Information Service
        5285 Port Royal Road
        Springfield, VA  22161
        Telephone: 703-487-4650
The EPA Project Officer can be contacted at:
        Oil and Hazardous Materials Spills Branch
        Municipal Environmental Research Laboratory—Cincinnati
        U.S.  Environmental Protection Agency
        Edison, NJ 08837

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United States
Environmental Protection
Agency
Center for Environmental Research
Information
Cincinnati OH 45268
Postage and
Fees Paid
Environmental
Protection
Agency
EPA 335
Official Business
Penalty for Private Use $300

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