2007 International Nuclear Atlantic Conference - INAC 2007

Santos, SP, Brazil, September 30 to October 5, 2007

ASSOCIAÇÃO BRASILEIRA DE ENERGIA NUCLEAR - ABEN
ISBN: 978-85-99141-02-1

URANIUM HEXAFLUORIDE RELEASE ASSESSMENT

Arivaldo M. do Sacramento1, Vanderley de Vasconcelos1 and Elizabete Jordão3

1
Centro de Desenvolvimento da Tecnologia Nuclear – CDTN/CNEN
C. Postal 941 Cidade Universitária
30 123 970. Belo Horizonte, MG.
ams@cdtn.br
vasconv@cdtn.br
2
Universidade Estadual de Campinas - UNICAMP
Caixa Postal 6066 Cidade Universitária
13 083 970. Campinas, SP.
bete@feq.unicamp.br

ABSTRACT

There are many available vapor cloud dispersion models that can be applied on UF6 release assessments, with a
great variation in capabilities and accuracies. Sometimes it is wise to carry out a gross screening analysis prior
to embarking on a modeling exercise, since it may be that the predicted concentrations are orders of magnitude
below some limits; this screening analysis can also be used to check the magnitudes of the results of subsequent
detailed model applications. This paper is intended to present a simple method which can be used to assess the
possible consequences of UF6 releases and determine the need for preventive and mitigating actions. The
proposed model for atmospheric dispersion is based on the Gaussian plume, which model has been modified to
take account two specific effects: plume rise and/or building wake. The proposed model is validated using data
of an accident that occurred in 1978 at Ohio gaseous diffusion plant, where within one our about 9500 kg of
UF6 escaped outdoors. The results are presented in terms of concentrations of HF and uranium intake.

1. INTRODUCTION

The 48Y cylinder is used for storing and transporting up to 12.5 tons of uranium hexafluoride
(UF6), which is the basic material used to produce enriched uranium for nuclear fuel
elements. At room temperature UF6 is a colorless and subliming solid with a significant vapor
pressure; it has a triple point at 337 K and 0.152 MPa and its sublimation point (329 K, 0.1
MPa) is below this triple point. This has implications for processing, because the pressure and
the temperature must be above the triple point, in order to be handled as a liquid. Thus, any
process using liquid UF6 can be subject to leakage to the atmosphere through any holes. This
event shall be considered as a postulated accident for nuclear fuel cycle facilities that handle
liquid UF6, like uranium enrichment plants. The major concern in accident analysis is the
potential consequence to off-site personnel; therefore the consequences shall be evaluated
beyond the site boundary downwind from the release point. When UF6 is exposed to moist
air, it reacts with the water in the air producing uranyl fluoride (UO2F2) and hydrogen
fluoride (HF); the chemical reaction releases heat, which may make a buoyant plume of these
chemical products and cause it to rise. The chemical toxicity of these products dominates the
radiological one. The permissible exposure levels for soluble uranium compounds are based
on their chemical toxicity. UO2F2 is a particulate that is very soluble in the lungs, and the
uranium acts as a heavy metal poison that can affect the kidneys. HF is an acid vapor that can
cause acid burns on the skin or lungs. In the event of an accidental release its toxicity level
can be reached in minutes. The final goal of this paper is to present a simple method which
can be used to assess the possible consequences of UF6 releases and determine the need for
preventive and mitigating actions.

2. FORMULAS FOR CALCULATING INPUT PARAMETERS

The following discussions provide an overview of the types of input data required by the
model; a set of equations is suggested by this work for calculating some input parameters that
are not generally well understood.

2.1. Atmospheric Dispersion

There are several models available for predicting the concentrations downwind of a single
source; if one is interested in concentrations only along the plume centerline the formula for
ground level concentrations reduces to

  H 2 
χ (x,0,0, H ) =
Q
exp −  
2  (1)
πσ yσ z u   2σ z 

where:
χ is the concentration measured as a mass per volume, such as mg/m3 or µg/m3; Q is the
emission rate, mg/s; u is the average wind speed, in m/s; H , the effective height of source
emission in meters, that is obtained adding the physical source height to ∆H ; σ y and σ Z are
dispersion parameters in y and z directions, respectively, in meters. These parameters can be
calculated using the equations given by Eimutis and Konicek [1]

Frequently the effluent from a short stack or roof vent will be influenced by the aerodynamic
flow pattern around the building(s) with which it is associated. If the effluent is trapped in the
cavity, it will be mixed rapidly into a volume determined essentially by the cross-sectional
area of the structure and the wind speed. An appropriate formula for the downwind
concentration is:

χ (x,0,0, ) =
Q
(πσ yσ z + cA)u (2)

where A is the cross-sectional area of the building normal to the wind and c is a shape factor,
ranging from 0.5, with a relatively streamlined shape, to 2, for a bluff building.

2.1.1. Plume rise

The stream of polluted air downwind of a smoke stack is called a smoke plume; if the plume
is buoyant, or if there is a large effluent out of the top of the smoke stack, the center of the
plume can rise above the initial emission height - this is called plume rise. Buoyancy rise is
sometimes called thermal rise because the most common cause of lower density is higher
temperature and the rise is associated with atmospheric stability. In this work two
atmospheric conditions are considered:

INAC 2007, Santos, SP, Brazil.

• Stable conditions
Whenever the temperature lapse rate is stable Briggs [2] suggests the following equation

∆H = 5.1F 1 / 4 s −3 / 8 (3)

where
F is the buoyancy flux parameter, (m4/s3 )
s is the stability parameter, ( s-2)

• Neutral conditions
A neutral lapse rate implies a different turbulent regime, and the recommended equation
is:

∆H = 21.425 F 3 / 4 u −1 (4)

Formulas to calculate F and s

As explained in item 1 Introduction, when uranium hexafluoride is released in air, it
reacts rapidly with water vapor and forms uranyl fluoride and hydrogen fluoride [5]:

UF6 + 2 H 2 O = UO2 F2 + 4 HF + heat (5)

The UF6 hydrolysis reaction releases approximately 58 kJ/g mole of H 2 O , which heats
the plume and cause plume rise, that can be calculated using parameters F and s [3], as
following:

  
M s 
2  M s  T s c
F = T gwr  1 −  +  − 1 
ps
(6)
Ts  M   T  c p
M 


and

g  ∂T 0,98 
s= + (7)
T  ∂z 100 

where
T : ambient temperature (K);
TS : gas temperature (K);
g : acceleration of gravity 9.8 (m/s2)
w : effluent velocity (m/s)
r : stack radius (m)
M : molecular weight of the air (g)
M S : average molecular weight of the effluents (g)
C P : specific heat of air at constant pressure (cal/K/mol)
C ps : specific heat of effluents at constant pressure (cal/K/mol)

INAC 2007, Santos, SP, Brazil.

∂T
: change in local temperature with height (K/m).
∂Z

2.2. Uranium intake

Uranium intake due to the airborne release of a certain mass of uranium is given by Eq. (8)
[4]

χ
I U = Q × BR  (8)
Q

where
I U inhaled intake of soluble uranium, (mg)
Q is the released quantity, (mg)
BR is the breathing rate, which is 3.33 x 10-4 m3/s

3. ESTIMATION OF INHALED SOLUBLE URANIUM INTAKE AND HYDROGEN

FLUORIDE CONCENTRATION

For the purpose of this work, the release to be evaluated involves the rupture of hot 14-ton
cylinders outdoors, at Portsmouth gaseous diffusion plant; the estimations are based on the
following assumptions: average meteorological conditions- D stability, 4.5 m/s wind speed,
and no rain. At Portsmouth there was a release of 9500 kg of UF6 – equivalent to 6400 kg of
natural uranium; it is assumed that some of the uranium is removed from the air initially by
agglomeration and impaction, thus it is supposed that 4800 kg of uranium becomes airborne.
The corresponding mass of HF is 1620 kg [4].

3.1. Estimation of Hydrogen Fluoride Concentration

. .
 h2 
exp −
Q e  Q ×106 ÷1800 = 6.37 × 10 4
χ = and = 1620 ×4.5
mg
π σ yσ z u  2  πu 3,1415 m3
 2σ z 

Table 1. Input parameters

Distance x σy σz σ yσ z  he 
2  h
exp − 12  e


2

(meters)    σ z
  

σ z 
700 54.6 23.9 1304.94 0.70 0.704
10000 60.6 133.0 80145.80 0.02 0.989

INAC 2007, Santos, SP, Brazil.

 Table 2. Hydrogen fluoride concentration using the above input parameters.

Distance x
(meters)
χ ( )
mg
m3
22.4
× 20.01 = χ ( ppm )

700 34. 22.4

× 20.01
= 39.

10000 0.8 22.4

× 20.01
= 0.9

3.2. Estimation of Inhaled Soluble Uranium Intake

Table 3. Amount of soluble uranium inhaled, using equation 8

x
χ
Q
( )
s
m3
× ( )
Q mg × BR ( )
m3
s
= IU (mg )

700 3.81x10-5 4800x106 3.33x10-4 60

10000 8.72x10-7 4800x106 3.33x10-4 1

4. CONCLUSIONS

In this work it was presented a simple method that can be used to assess the possible
consequences of UF6 releases; in order to demonstrate the use of dispersion model, a typical
scenario have been proposed, in which 4800 kg of uranium and 1600 of HF become airborne.
The stability class D with 4.5 m/s wind speed was used as a meteorological input data,
because this input is traditionally used, when evacuation distances for accidents involving
toxic chemicals are evaluated. Tables 4 and 5 list the obtained results using the simple model
and the results that are shown on NUREG 1140; the discrepancies between the two
approaches are due to the values of breathing rate and the dispersion parameters used. The
IDLH – Immediately Dangerous to Life or Health-established by NIOSH is 30 ppm; with the
simple model a value of 39 ppm was estimated, which can be a signal that a more
sophisticated model may be used.

INAC 2007, Santos, SP, Brazil.

 Table 4. Uranium intake due to the airborne release of 4800kg of uranium

Uranium intake (mg)

Distance NUREG Gaussian
(meters) 1140 model
700 28 60
10000 0.5 1

Table 5. HF exposure due to the airborne release of 1620 kg of HF.

HF exposure (mg/m3)
Distance NUREG Gaussian
(meters) 1140 model
700 41 34
10000 0.8 0.8

ACKNOWLEDGMENTS

The authors would like to express their gratitude to Center of Development of Nuclear
Technology – CDTN/CNEN, that sponsored this work, and to the colleagues of
CDTN/CNEN and State University of Campinas – UNICAMP who were involved with this
work.

REFERENCES

1. Eimutis, E. C. and Konicek, M. G.. “Derivation of continuous functions for lateral and
vertical atmospheric dispersion coefficients”. Atmospheric Pergamon Press, 6, pp.859-
863 (1972)
2. Hanna, S. R. “Plume Dispersion and Concentration Fluctuations in the Atmosphere”,
Encyclopedia of Environmental Control Technology, Volume 2, Texas (1989).
3. Slade D. H., Meteorology and Atomic Energy, TID-24190, U.S. Atomic Energy
Commission, Washington, DC, (1968)
4. U.S. Nuclear Regulatory Commission. Regulatory Analysis on Emergency Preparedness
for Fuel Cycle and other Radioactive Materials Licensees, NUREG/1140, Washington,
DC (1989).
5. McGuire, S. A. Chemical Toxicity of Uranium Hexafluoride Compared to Acute Effects of
Radiation. NUREG/1391, U.S. Nuclear Regulatory Commission, Washington, DC
(1991).
6. McKenna, T. at al. Response Technical Manual, Volume 1 NUREG/BR-0150, U.S.
Nuclear Regulatory Commission, Washington, DC (1996).

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