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Icone30 1571
Icone30 1571
ICONE30-1571
1 © 2023 by JSME
NRA Nuclear Regulation Authority plants. A major point of discussion when considering the
PC Polycarbonate radiological consequences of fires in nuclear facilities is the
PMMA Poly(methyl methacrylate) airborne release fraction (ARF) values to be considered. In
PuO2 Plutonium dioxide general, this ARF is defined as the ratio between the mass of
UO2 Uranium dioxide particles released in the airborne phase (in the form of an aerosol)
wt weight and the mass of particles initially deposited on the surface under
consideration [10]. This last study proposed a review of values
1. INTRODUCTION reported in the literature for realistic materials and significant
During the production and reprocessing of nuclear fuel rods, discrepancies were discovered for fuels representative of glove
mixed oxide powders composed of plutonium dioxide (PuO2) boxes (i.e., polymers like PMMA or PC). These high disparities
and uranium dioxide (UO2) are handled within static can have significant consequences in terms of decision making
containment devices such as glove boxes (GBs) [1]-[2]. during a crisis, such as the geographical perimeter to be secured.
Throughout their life cycles, the handling and processing of fuel Thus, the Institute for radiological protection and nuclear safety
rods induce the release of contaminants, in the form of micron- (IRSN), in partnership with the Japanese Nuclear Regulation
sized particles, which can be transported and deposited on glove Authority (NRA), has been running since 2019 a research project
box walls potentially made of polymers such as polycarbonate that aims at reducing the uncertainties related to the assessment
(PC) and poly(methyl methacrylate) (PMMA). Accidental fires of the ARF of PuO2 involved in GB fires. This project, named
in nuclear fuel fabrication and reprocessing plants that can occur FIGARO (Fires Involving Glove boxes with Aerosol Release
inside the glove box (through pyrophoric reactions/solvents Occurrences), first includes two complementary parts for
ignition, for example) or outside the glove box from another heat separately studying the various mechanisms involved in the GB
source (electrical cabinet fire...) can cause the rupture of the GB fires and the PuO2 airborne release. These works are especially
containment [3] with a risk of dispersion of the radioactive dedicated to analytical approaches based on small and medium-
elements within the facility and potentially into the environment scale experimental activities for a thorough characterization of
[4]-[5]. The Factory Mutual Research Corporation listed 24 fires the above phenomena. The first part also tackles the development
and 19 explosions between 1956 and 1965 on laboratory GBs and validation of a GB fire model in the IRSN SYLVIA [11] and
operated by the United States Atomic Energy Commission [6]. CALIF3S-ISIS [12] softwares, while the second part also
The most significant contamination accident resulting from a GB includes the development and validation of the aerosol
fire occurred at the Rocky Flats plant in the USA in 1957 [7]. metrology suitable for the ARF measurement during large-scale
Plutonium shavings in a GB located in the Plutonium Recovery tests. Finally, the third part of the FIGARO project aims at
and Fabrication Facility building spontaneously ignited. The fire transposing and validating the analytical works for realistic
spread to the flammable GB materials. The fire rapidly spread assessments of the ARF of PuO2 during large-scale GB fire tests.
through the interconnected GBs and ignited the large bank of This paper first describes the FIGARO project, before
high-efficiency particulate air (HEPA) filters located in a plenum presenting its first outcomes obtained so far.
downstream. Within minutes the first filters had burned out,
allowing plutonium particles to escape from the building exhaust 2. FIGARO PROJECT
stacks. The building exhaust fans stopped operating due to fire This section first describes the small and medium-scale fire
damage, which ended the majority of the plutonium release. characterizations of GB materials (PMMA…), before presenting
Another major fire occurred in the Rocky Flats plant on May 11, the works dedicated to the in-depth characterization of the PuO2
1969, in the Plutonium Processing Facility building [8]. As for airborne release and to the development of a suitable aerosol
the fire of 1957, the spontaneous combustion of plutonium metrology adapted to large-scale tests. The last part addresses the
shavings in the GB was the cause of this disaster. While the fire large-scale GB fire tests devoted to the realistic assessments of
showed marked similarities to the 1957 fire, the level of the ARF of PuO2.
contamination was less severe because the HEPA filters in the
exhaust system did not burn (after the 1957 fire, the filter 2.1. Analytical GB fire characterizations
material was changed from cellulose to non-flammable IRSN carried out between 2013 and 2017 a preliminary
fiberglass). A third GB fire occurred again at Rocky Flats series of seven tests to characterize the fire behaviour of a glove
Environmental Technology site on May 6, 2003, in a GB during box (GB) in open atmosphere conditions and to assess the
decommissioning [9]. For the French nuclear fuel fabrication and thermal, chemical and aeraulic stresses that the radioactive
reprocessing plants, 21 incidents related to a fire start on a GB or particles could undergo during the fire [13]. The tests used a GB
a confined enclosure were recorded over the period 1988-2008; of about 1 m3 in volume that was equipped with containment
one third of these incidents led to a loss of their containment. panels made of either PC with glove holes for the handling of
The total activity corresponding to the release of nuclear radioactive material, or stainless steel (Figure 1-A). This GB also
materials, also called "fire source term", is an input to the used PMMA panels (with glove holes) placed over the PC
calculation of the radiological consequences that are required by panels, both representative of the GBs working sides. The
the fire safety analyses to strengthen the appropriate prevention, PMMA panels simulated biological protection panels made of
protection and fire-fighting measures in the related nuclear Kyowaglas (70 %wt of PMMA and 30 %wt of lead) and that
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usually equip the working sides of the GBs in the nuclear scale characterizations using the cone calorimeter and following
industry. a challenging safety protocol including numerous health
measures. Given that such a safety protocol would be
incompatible with the conduct of large-scale GB fire tests in the
IRSN test facilities, a non-toxic surrogate material with fire
behaviour close to that of Kyowaglas must be identified. To this
end, the preliminary small-scale fire characterizations of the
Kyowaglas material are also crucial to figure out the appropriate
surrogate material exhibiting similar fire behaviour.
A B
FIGURE 1: GLOVE BOX USED AS PART OF THE
PRELIMINARY TEST SERIES [13], BEFORE FIRE (A), DURING
FIRE (B).
This test series provided significant insights related to the
combustion regimes in the GB, as obtained in open atmosphere
conditions. The combustion regime in the GB turned out to be
quasi-complete (i.e., with a combustion efficiency close to
unity), promoted by the GB configuration being similar to a
“well-stirred reactor” (Figure 1-B), with swirling flames being A B
observed inside the GB fire source. The mean temperatures
FIGURE 2: CADUCEE EXPERIMENTAL DEVICE (A),
measured between 1000 and 1200 °C inside the GBs for all the
OPERATING PRINCIPLE (B).
tests, notably higher than those of typical turbulent diffusion
flames (about 800-900 °C), also corroborated the combustion
2.1.2. Medium-scale fire tests using a glove box
conditions operating inside a “well-stirred reactor”.
simulator
Furthermore, these outcomes also raised questions related to the
To carefully investigate the complex combustion regimes
effect on the GB combustion regimes, of the air inflow rate in
observed during the preliminary GB fire tests, this part deals with
the GB, the GB configuration (number of fuel panels, the panel
three analytical test campaigns using a medium-scale glove box
type) and under-oxygenated conditions typical of fires in
test simulator, named SIMBAG. The objectives of the first two
confined rooms of nuclear installations. To tackle these matters
test campaigns are to study the impact of thermal and aeraulic
and to supply data supporting the development and validation of
conditions on the combustion regimes in the medium-scale glove
GB fire models, the first part of the FIGARO project therefore
box, for open and confined atmospheres. The last test campaign
addresses analytical combustion studies involving either GB
aims at studying in open atmosphere conditions the impact of the
material samples (PMMA, Kyowaglas…) or a medium-scale
surrogate of Kyowaglas materials on the combustion regimes in
glove box simulator.
the SIMBAG device.
2.1.1. Analytical study of solid panel combustion
2.1.3. Model development and validation
A first goal of this work is to investigate the effect of under-
In parallel to the above multi-scale GB fire characterizations
oxygenated conditions on the combustion of vertically-oriented
and the related experimental database development, one main
PMMA slabs. The collected data aim at proposing analytical
goal of the FIGARO project is to develop the abilities of the
correlations that could be implemented in fire softwares for
IRSN softwares to predict GB fires and their consequences in
improving their predictive abilities in the above conditions. This
confined and mechanically-ventilated compartments. This
analytical investigation is conducted using the controlled-
section presents the modelling and validation works planned for
atmosphere calorimeter, named CADUCEE [14], as seen in
the two-zone model SYLVIA software and the computational
Figure 2. This experimental device was first used by Alibert et
fluid dynamics CALIF3S-ISIS software. The simulation of a
al. [15] who especially investigated the impact of under-
glove box fire is complex due to various phenomena occurring
oxygenated conditions on the combustion of horizontally-
in the glove box, its loss of geometry during the fire, large vortex
oriented PMMA slabs and proposed correlations e.g., for the
structures, the strong turbulent mixing triggered by
mass loss rate according to the oxygen concentration.
hydrodynamic instabilities developing near the lower fresh gas
Furthermore, despite the widespread use of biological
intakes and the heat transfer dominated by radiative effects. No
protection panels made of Kyowaglas in the nuclear industry,
theory to date has been put forward on how to model all aspects
few data related to the fire behaviour of this material are
of the problem. A global modelling approach is therefore
available. This is mainly explained by the high toxicity of its lead
proposed, based on the description of the successive main events
compounds [16]. Accordingly, as part of the FIGARO project,
that occur during the development of a GB fire [13]: the flame
the Kyowaglas fire behaviour investigations are limited to small-
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spread over the PMMA/Kyowaglas protection panel (where the observed during the preliminary GB fire tests [13]. A last step
fire is initiated), the melting and relocation of the PC aims at depositing the PuO2 surrogate particles on the PC walls
containment panels at the GB bottom and finally the rapid of the SIMBAG device to determine the impact of the PC
combustion phase that involves the two combustible protection thermal degradation on the related ARF. The associated
panels and the melted PC . The IRSN GB fire database, supplied demonstrative tests are intended to support the specification of
by the ongoing multi-scale fire characterizations, aims at the large-scale GB tests which will assess the ARF of the PuO2
validating the global GB fire model. The latter will be surrogate particles for real fire conditions.
implemented first in the SYLVIA software and afterwards
leveraged in the CALIF3S-ISIS software. 2.2.3. Development and validation of the aerosol
metrology for assessing the ARF at large-scale
2.2. Study of the particle resuspension and This task consists in designing, developing and validating
deposition coefficients the aerosol sampling lines that will allow the ARF assessment of
This section first describes the analytical investigations the PuO2 surrogate during the large-scale GB fire experiments.
related to the PuO2 airborne release at small-scale and next those
at medium-scale using the glove box simulator SIMBAG. The 2.3. GB fire tests
third part describes the efforts devoted to the development of a The third part of the FIGARO project aims at
suitable aerosol metrology adapted to large-scale tests. transposing the previous analytical works to a large scale in order
to validate the fire behaviour of the GB equipped with the
2.2.1. Analytical study of PuO2 surrogates Kyowaglas surrogate panels, and to assess the ARF of the PuO2
Due to its high radiotoxicity, PuO2 powder cannot be used surrogate during realistic GB fires.
for conducting experimental studies regarding its resuspension
potential under the complex thermal stresses representative of 2.3.1. GB fire tests involving the Kyowaglas surrogate
fires. Nevertheless, few data regarding the criteria associated Tests are planned to validate the fire behaviour of the GB
with the choice of surrogates for PuO2 particles have been equipped with the Kyowaglas surrogate panels. To this end,
presented so far. The first goal here is therefore to identify the IRSN previously requested SP Fire Research of Sweden to
major properties of particles impacting their airborne release conduct a fire test with the same 1 m3 volume GB as the one used
fraction during thermal degradation of the PC material. This for the preliminary tests [13] but equipped with Kyowaglas
material composing the containment panels of the GBs where the protection panels. This test was carried out under a calorimeter
radioactive particles can be deposited. Based on this work, the hood where lead-contained releases can be handled. The
next step targets to identify a surrogate of PuO2 powder with the validation of the Kyowaglas surrogate panels therefore relies on
adequate properties regarding the airborne release. These efforts the expected fire behaviour similarity between the GB tests
also include the methodology for controlling the size dispersion conducted as part of this task and that performed at SP Fire
and morphology to get the appropriate PuO2 surrogate powder. Research.
Afterwards, experiments with the PuO2 surrogate particles are
planned to be conducted in the ARTEMIS test bench [10] at 2.3.2. GB fire tests involving both the Kyowaglas and
small-scale to identify the experimental conditions PuO2 surrogates
corresponding to the highest ARF. Finally, as part of the last This part deals with the tests that will involve both the
phase of the FIGARO project, large-scale GB tests with wall Kyowaglas and PuO2 surrogates to provide an assessment of the
deposits of the PuO2 surrogate will be carried out for assessing ARF of the PuO2 surrogate for realistic GB fires. These tests are
its ARF under real fire conditions. planned in open atmosphere conditions and in confined and
mechanically-ventilated conditions to investigate the impact of
2.2.2. Preliminary study of particle transport using the the test conditions on the ARF assessment. The former
medium scale glove box SIMBAG and the PuO2 conditions correspond to a maximum oxygen availability in the
surrogate related test facility for a full GB fire development, while the
Some preliminary tests at medium-scale using the SIMBAG latter induce a reduced oxygen availability in the associated test
device have been designed to validate metrology points and to facility for a potentially limited fire development, as it was
assess by some demonstrative tests the transport of the PuO2 observed for another type of fuel [17]. The collected data will
surrogate particles in the GB during its thermal degradation. For support the validation of the abilities of the IRSN SYLVIA and
this purpose, three steps were designed. First, the particle CALIF3S-ISIS softwares, both using the earlier developed GB
transport in the GB will be studied by conducting a particle fire model, to simulate large-scale GB fire tests and their
tracing and the related transfer coefficient at the outlet of the consequences in confined compartments. In addition, the data
SIMBAG device will be assessed. Next, it is proposed to deposit related to the ARF of the PuO2 surrogate will be capitalized in
the PuO2 surrogate particles on the steel walls of the SIMBAG the IRSN BADIMIS database [18] which aims at collecting the
device (instead of the PC walls) to determine the impact of the available resuspension factors and those obtained in the present
turbulent flows on the related ARF. To this end, the SIMBAG experiments. These efforts will contribute to support the safety
tests aim at reaching the near-complete combustion regime as analyses regarding the potential release of PuO2 particles during
4 © 2023 by JSME
accidental GB fires in nuclear fuel fabrication and reprocessing confers a substantial thermal stability on the Kyowaglas. In
plants. To this end, the BADIMIS database could provide input addition, at the end of the cone calorimeter test, lead oxide beads
data for simulations by the SYLVIA software of the transport and start to form on the surface of the residue, as seen on Figure 4-
deposit of the PuO2 particles in the rooms and ventilation B, due to the oxidation of metallic lead.
networks of nuclear facilities.
3.1.1. Analytical study of solid panel combustion These insights contributed to support the identification of a
The first step of the combustion study of vertically-oriented surrogate of Kyowaglas. Thus, a composite made of PMMA and
PMMA samples (Figure 3) was performed in the controlled- magnesium dihydroxide (MDH, Mg(OH)2) was selected from
atmosphere calorimeter CADUCEE device (Figure 2) by varying several candidates. MDH is indeed an efficient flame retardant
the oxygen (O2) concentration from 21 to 17 vol%. The size of that significantly reduces the heat release rate (HRR) [20]. In
the PMMA sample was either 200×200, 400×400 or addition, the cone calorimeter tests conducted for the Kyowaglas
600×600 mm2. This first step highlights, for all the considered material and PMMA-MDH composite samples of variable
PMMA sample sizes, that one of the key combustion parameters composition showed that the closest HRRs between these two
(the fuel mass loss rate) exhibits a linear behaviour versus the materials were obtained for a MDH mass fraction in the 12-15 %
oxygen concentration in the 17-21 vol% range. range. These outcomes are illustrated in Figure 5 that gives the
HRRs for the Kyowaglas material and e.g., for the composite
sample composed of 12 %wt of MDH. This figure also provides
the HRR for PMMA, confirming its strong reduction by both
lead (Kyowaglas) and MDH (Kyowaglas surrogate) materials.
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was to study, in open atmosphere conditions, the impact of the device. Four fire tests were carried out in the confined and
change of thermal and aeraulic conditions on the combustion mechanically-ventilated room 3 of the DIVA facility, as shown
regimes in the SIMBAG medium-scale GB simulator. To this on Figure 7.
end, fourteen medium-scale tests using the SIMBAG device
were conducted under the large-scale calorimeter (Figure 6-A)
located in the wide (2000 m3 in volume) and well-ventilated
SATURNE facility. The SIMBAG device is composed of 3
parts:
the analytical GB (Figure 6-B) with its containment panels,
the air supply system (Figure 6-C) for controlling a part of the A B
air inflow rate in the analytical GB,
the vertical gas burner (Figure 6-D) that simulates the FIGURE 7: THE MULTI-ROOMS AND MECHANICALLY-
VENTILATED DIVA FACILITY (A) THAT HOSTED THE SIMBAG
combustion of the GB protection panel.
SIMULATOR IN ROOM 3 (B).
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material, the regression of the material thickness under the effect duct heated at 150°C (Figure 8-C), before being sampled under
of its pyrolysis or the swelling of the material under the effect of well-mixed conditions at 2 m from the inlet.
the temperature are not considered. In addition, the aeraulic
effect on flame spread is not regarded (limitation of zone models)
and the soot concentration inside the flame is assumed to be
homogeneous over the height of the flame (no local effect of the
flame radiation on the fuel surface). Finally, uniform ignition
along the width of the wall (1D flame propagation) is assumed.
Based on the Quintiere formulation of the flame spread
velocity, ܸ [22], in open atmosphere, that supposes a C
thermally-thick behaviour of the material, we considered a time
dependence on the ambient gas temperature for confined fires,
Tg(t), and a correction factor, (O2). The latter takes into account
the impact of the compartment oxygen depletion on the decrease
of the flame radiative heat flux incident to the fuel surface and
"
obtained in well ventilated conditions, ݍሶ . These considerations
give the following equation for ܸ:
A B
మ
" ఞ(ை )ቁ ఋ
ସቀ̇ ೝ FIGURE 8: THE ARTEMIS EXPERIMENTAL TEST BENCH,
మ
ܸ(= )ݐ మ (1) OVERVIEW (A), THERMAL DEGRADATION ZONE (B), HEATED
గ൫ೞఘೞೞ൯൫் ି் ሺ௧ሻ൯
ZONE (C).
where c is the heated fuel distance (m), ksscps, the thermal The aerosol sampling filters are next analyzed by inductively
inertia of the wall (W2.s.m-4.K-2) and Tig, the ignition temperature coupled plasma mass spectrometry (ICP-MS) after each test to
of the wall (K). The validation of these models was performed in determine the mass of released contaminant particles on the
particular on IRSN bench-scale fire tests involving PMMA slabs sampling membrane. To assess the ARF properly, such mass
[23]. measurements need to consider the loss of particles within the
The next steps of the GB fire model development will focus test bench, as detailed in [24]. The current analytical study
on the modelling of the PC containment wall relocation and its highlighted the main significant influence on the ARF of the
impact on the radiative heat transfers towards the existing fuel median geometric diameter and density of particles. For
walls, their preheating by the hot gas layer in the GB and finally illustration, Figure 9 provides e.g., the ARF dependance
the modeling of the relocated PC combustion. The efforts according to the median geometric diameter for all the studied
devoted to the development of this GB fire model in the SYLVIA contaminants powders.
software will be next capitalized in the CALIF3S-ISIS software.
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candidates, since its density (9680 kg/m3) is close to that of PuO2
(11,460 kg/m3), and its thermal stability was proven up to
1200°C which is the maximum temperature measured in the GB
during the near-complete combustion regime [13]. The last effort
in HfO2 powder characterization was to control the appropriate
size dispersion and morphology. To this end, a process was
specified for conditioning the particles to reach aerodynamic
diameters which, on the one hand, must be compatible with the
geometric diameters leading to measurable ARFs (Figure 9), on
the other hand, must not too strongly limit their penetration from
the GB up to the sampling devices located at the exhaust of the A B
large-scale test facilities.
Experiments will be conducted with the conditioned HfO2 FIGURE 10: THE SATURNE (A) AND PLUTON (B) TEST
FACILITIES.
powder using the ARTEMIS test bench to confirm the
experimental conditions corresponding to the highest ARF.
These insights will support the specification of the final GB tests
that will be performed for assessing the ARF of the HfO2
particles under real fire conditions.
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panels showed that the HRR was slightly lower than that The first two complementary parts of the FIGARO project
measured for the test conducted at SP Fire Research, which used that studied separately the various mechanisms involved in the
the same GB but equipped with Kyowaglas protection panels. GB fires and the PuO2 airborne release are nearly completed.
Accordingly, additional composite panels were supplied by First, the surrogates of Kyowaglas and plutonium dioxide were
casting with a lower MDH content of 11 % wt and a last test was identified based on in-depth analytical investigations to obtain
conducted with such panels (Figure 13). This test and that carried similar fire behaviour between Kyowaglas and its surrogate and
out with the Kyowaglas panels give identical HRR peaks, as seen similar properties in terms of ARF between plutonium dioxide
on Figure 14. This figure also highlights that, outside the and its substitute. In addition, the analytical studies conducted
incubation stages, the HRR time evolutions around the fire peak with the medium-scale SIMBAG simulator provided valuable
are also very close. insights for improving knowledge of the complex and
unexpected combustion regimes that were observed during the
preliminary GB fire tests. These tests, complemented by the
study dealing with the effects of under-oxygenated conditions on
the combustion of GB materials (PMMA…) in the CADUCEE
controlled-atmosphere device, provide an experimental database
devoted to the proposal and/or validation in open and confined
conditions of fire models such as the glove box model developed
in this project. The transposition and validation of the analytical
works, as desired in the third and last part of this project, was
remarkably achieved for the Kyowaglas surrogate, which
exhibited fire behaviour very similar to Kyowaglas at both small
FIGURE 12: PMMA-MDH FIGURE 13: VIEW FROM
PANELS MADE BY CASTING. THE REAR KYOWAGLAS
and large-scale. The last challenge will regard the large-scale
SURROGATE PANELS ARF assessments of the PuO2 surrogate for realistic GB fire
WHEN THE GB FIRE FAST conditions. To this end, the suitable aerosol metrology was
GROWS. implemented in the large-scale test facilities, and the first
qualification tests of this metrology showed satisfactory
outcomes.
ACKNOWLEDGEMENTS
The authors are very grateful to the Nuclear Regulation
Authority (NRA) of Japan for its partnership in the FIGARO
project. The authors also express their gratitude to
P. Wiszniowski from the IRSN aerosol physics and metrology
laboratory, S. Pons, G. Basso, V. Cozar and the other members
of the technical team of the IRSN fire experimentation
laboratory, for their assistance in the development and
implementation of the aerosol metrology and the achievement of
the experiments.
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