Fusion Engineering and Design 87 (2012) 10401044

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Fusion Engineering and Design

journal homepage: www.elsevier.com/locate/fusengdes

Preliminary results from a detritiation facility dedicated to soft

housekeeping waste
X. Lefebvre a,b, , P. Trabuc a,b , K. Liger a,b , C. Perrais a,b , S. Tosti a,c , F. Borgognoni a,c , A. Santucci a,c
a
JET-EFDA, Culham Science Centre, Abingdon OX14 3DB, UK
b
CEA, DEN, Cadarache DTN/STPA/LIPC, F-13108 Saint-Paul-lez-Durance, France
c
Associazione ENEA-Euratom sulla Fusione, C.R. ENEA Frascati, Via E. Fermi 45, I-00044 Frascati, RM, Italy

a r t i c l e i n f o a b s t r a c t

Article history: Nuclear waste management has to be taken into account for fusion machine in tritium experimentations.
Received 7 September 2011 Soft housekeeping waste is produced during both operating and dismantling phases and is contaminated
Received in revised form 15 February 2012 by tritium under reduced (HT) and oxidized (HTO) forms. At CEA Cadarache, a lab-scaled facility has
Accepted 16 February 2012
been built for soft housekeeping detritiation. The tritiated gas exhausted from the process described
Available online 20 March 2012
above is foreseen to be treated by a tubular PdAg membrane reactor, for gaseous tritium recovery.
Since this membrane reactor uses hydrogen as swamping gas the compatibility toward explosive hazard
Keywords:
has to be taken into account. Then, this work presents a double objective. A rst study is presented in
Housekeeping
Detritiation
order to identify the best conditions for the declassication of soft housekeeping waste, without tritium
Tritium recovery. Experiments carried out at 120 C are not efcient enough and do not allow one to choose the
Membrane reactor most efcient carrier gas. Some other tests are being currently performed at higher temperatures (150 C).
Moreover, due to safety issues, the use of air has to be avoided during membrane reactor implementation
phase. Preliminary results obtained with hydrogen hazard-free carrier gases are also presented.
2012 Elsevier B.V. All rights reserved.

1. Introduction
Soft housekeeping waste is produced during both operating
and dismantling phases of fusion reactor and is contaminated by
tritium under reduced (HT) and oxidized (HTO) forms. For exam-
ple, concerning ITER project, the production of 16003800 tons of
housekeeping and process waste is foreseen and can be split as
follows [1]:
20% very low level waste,
75% short lived intermediate level waste,
5% long lived intermediate level waste.
Consequently, this study consists of two main parts: rst of all,
the technical feasibility study is performed with different carrier
gases at different temperatures and ows in order to optimize the
experimental conditions for detritiation efciency. Moreover, in
order to avoid the explosive hazard due to the use of pure hydro-
gen as a swamping gas in the membrane reactor, the study of the
inuence of the type of carrier gas has also been carried out. Then,
the most appropriate carrier gas, presenting the best compromise
between safety and efciency, has been determined.
2. Presentation of the experimental facilities

The higher the waste class, the more expensive and stringent
the storage [2]. Moreover, tritiated waste induces the outgassing
particularity compared to usual nuclear waste. Then, the imple-
mentation of a detritiation facility could be interesting to declassify
this kind of waste.
In this work, the lab-scaled detritiation facility designed by CEA
Cadarache is presented as well as its future coupling with a mem-
brane reactor from ENEA Frascati [3].
Corresponding author at: CEA Cadarache, DTN/STPA/LIPC Bt 208, F-13108
Saint-Paul-lez-Durance, France. Tel.: +33442256415; fax: +33442257287.
E-mail address: xavier.lefebvre@cea.fr (X. Lefebvre).
The housekeeping samples are milled nitrile gloves contami-
nated by tritium and potentially by beryllium. They are placed in a
glass reactor heated at a temperature lower than its melting point.
The carrier gas injected in the glass reactor removes the tritium
that is nally trapped in liquid bubblers and measured via liquid
scintillation (see Fig. 1).
In a second step, the tritiated gas exhausted from the process,
instead of going into the liquid traps, is foreseen to be treated by a
membrane reactor consisting of a tubular PdAg membrane lled
with a Ni-based catalyst, as shown in Fig. 2 [412]. In this way, it
is possible to recover tritium under HT form which can be further
reused in the fusion fuel cycle. The carrier gas containing tritium
coming from the glass reactor is fed into the membrane lumen

0920-3796/$ see front matter 2012 Elsevier B.V. All rights reserved.
doi:10.1016/j.fusengdes.2012.02.076
 X. Lefebvre et al. / Fusion Engineering and Design 87 (2012) 10401044
Fig. 1. Schematic representation of the housekeeping detritiation facility.
Fig. 2. Schematic representation of the catalytic membrane reactor.
while a hydrogen (protium) stream is injected in the shell side in
counter-current mode. Since the PdAg membrane is permeable
only to hydrogen isotopes, the exchange reaction occurs over the
Ni-based catalyst:
Ni,400 C
HTO + H2 HT + H2 O
Tritiated gas HT formed by isotope swamping over the catalyst
permeates the membrane to be nally recovered in the shell side
of the membrane reactor. Within the scope of the further study, for
analytic and waste management purposes, the gaseous tritium will
be oxidized in an oven containing a cartridge of copper oxide and
the tritiated water formed is frozen in a liquid nitrogen cold trap.
The samples used in this study were milled nitrile gloves pro-
vided by JET fusion machine. The initial mass activity of the samples
has been assessed to 20 kBq/g, i.e. very close to the British ILW/LLW
threshold (12 kBq/g [13]). However, due to the expected hetero-
geneity of the initial activity of the samples, the residual activity
Fig. 3. Schematic representation of the residue calcination facility.
1041
has been always measured by liquid scintillation counting at the
end of the experiment under the operating mode schematized in
Fig. 3.
First of all, a well-known housekeeping quantity (between 12
and 15 g) was placed in the glass reactor (see Fig. 1). As the sam-
ples might contain some beryllium traces, the sample preparation
was made in a dedicated room for Be handling. Then, the air-tight
reactor was placed in the oven and a leak test was performed by
reading the pressure variation.
The temperature of the oven was regulated and the carrier gas
was injected in the system.
The demineralized water in the bubblers of a MARC 7000
device was changed every 1 or 2 h and a given quantity of this
recovered water is analyzed by liquid scintillation counting.
At the end of the experiment, the activity of the residue was
also measured. The residue housekeeping waste sample was burnt
to ashes in a Hastelloy reactor placed in an oven heated up to 500 C
under laboratory air for 3 h (Fig. 3). The tritium trapped in a MARC
7000 device was also measured via liquid scintillation counting.
The detritiation yield is calculated using the following equation:
n
a
i=1 i
Y (t) = 100 N
a
i=1 i
+ ares
with Y(t), the detritiation yield (%); ai , 3 H removed activity as a func-
tion of time (Bq); ares , 3 H activity of the residue (Bq); n, sampling
number at t-time (dimensionless); N, sampling number at the end
of the experiment (dimensionless).
1042 X. Lefebvre et al. / Fusion Engineering and Design 87 (2012) 10401044

9% Table 1
Ar + 2% O2 Housekeeping initial, after 18 h-experiment tritium activities and detritiation yield
8% Ar + 5% H2 at 120 C and 300 N mL/min gas ow.
Ar + 25% H2O
7% Ar + 40% H2O Carrier gas ai (kBq/g) ares (kBq/g) Y (%)
Air
Detritiation yield (%)

Ar2%O2 23.0 21.3 7.6

6% Ar5%H2 23.0 22.2 3.5
Ar25%H2 O 29.7 28.2 5.0
5%
Ar40%H2 O 29.4 27.9 5.4
Air 10.2 9.4 8.1
4%

3%

2%
Low oxidative (Ar2% O2 ),
1% Low reductive (Ar5% H2 ),
Intermediate oxidative (air),
0%
Humid gases (Arx% H2 O, x = 25 and 40).
0 5 10 15 20
Effective experimental time (hours)

Fig. 4. Soft housekeeping detritiation yield as a function of effective experimental
time for different carrier gases. T = 120 C and Q = 300 N mL/min.
As the samples come from JET, a residual activity of 12 kBq/g of
the waste has been considered for establishing the effectiveness of
the detritiation process. In fact, such a value of waste activity is the
threshold between intermediate level (ILW) and low level waste
(LLW) according to the British regulation [13].
3. Results and discussion
The experiments whose results are presented here have been
carried out during 3 days which correspond to 18 h of experiments
(6 h being the effective working time in each day). In Figs. 46, the
X-axis represents the effective experimental time and the Y-axis the
detritiation yield. The night-gaps between two experimental days
have not been considered in the graphs. The results presented here
only concern the detritiation part of the study using the process
described in Fig. 1 (i.e. without the membrane reactor coupling).
3.1. Inuence of the nature of the carrier gas
In order to identify the respective efciencies of the carrier
gases, several atmospheres have been tested:
The gas feed ow has been xed at 300 N mL/min which cor-
responds to the nominal workow of the membrane reactor. In
order to avoid the housekeeping burning during the experiment,
the temperature has been xed at 120 C.
Fig. 4 shows the behavior of the detritiation yield of soft house-
keeping as a function of the effective experimental time. First of
all, is it possible to observe that none of the 5 plots shown in Fig. 4
reaches a plateau and all obey a quasi linear regime which tends
to demonstrate that the experimental time was not optimized for
these experimental conditions.
The dark dots (diamonds, circles, triangles and squares) of the
graph establishes that the detritiation yield did not exceed 8% what-
ever the carrier gases employed at 120 C during 18 h effective
experimental time. The amount of water in argon does not seem
to have an inuence on the detritiation yield (see dark circles and
triangles in Fig. 4).
Table 1 summarizes the experiments carried out at 120 C and
300 N mL/min carrier gas ow. First of all, it is visible that the
expected heterogeneity of initial activities of the samples is accu-
rate. Indeed, the initial activities vary from 10 to 30 kBq/g. It is
also to notice that none of the Ar-based carrier gases allows the
declassication to LLW after 18 h. Regarding the sample detriti-
ated under air, since its initial activity (10 kBq/g) was slightly lower
than LLW/ILW threshold, it is not possible to conclude if that these
experimental conditions are sufcient to declassify such sample as
LLW.

60%

20%

50% 450 NmL/min. Air

Ar + 2% O2 - 120C 18%
300 NmL/min. Air
Ar + 2% O2 - 150C
Ar + 25% H2O - 120C 16%
Detritiation yield (%)

40% Ar + 25% H2O - 150C

Detritiation yield (%)

14%

12%
30%
10%

8%
20%
6%

10% 4%

2%

0% 0%
0 5 10 15 20
0 5 10 15 20
Effective experimental time (hours) Effective experimental time (hours)

Fig. 5. Detritiation yield as a function of effective experimental time with Ar + 2% Fig. 6. Detritiation yield as a function of effective experimental time with air.
O2 and Ar + 25% H2 O. Q = 300 N mL/min. T = 120 C.
 X. Lefebvre et al. / Fusion Engineering and Design 87 (2012) 10401044 1043

Table 2 Table 3
Housekeeping initial, after 18 h-experiment tritium activities and detritiation yields Housekeeping initial, after 18 h-experiment tritium activities and detritiation yield
at 120 and 150 C (15 h for Ar2%O2 at 150 C). at 120 C for different gas ows.

Carrier gas T ( C) ai (kBq/g) ares (kBq/g) Y (%) Carrier gas Feed ow ai (kBq/g) ares (kBq/g) Y (%)
(N mL/min)
Ar2%O2 120 23.0 21.3 7.6
Ar2%O2 150 17.3 7.6 56.1 Air 300 10.2 9.4 8.1
Ar25%H2 O 120 29.7 28.2 5.0 Air 450 13.1 11.4 13.5
Ar25%H2 O 150 18.8 14.3 23.6

3.2. Inuence of the temperature and the natural tritium outgassing occurs much more easily with
fresh samples. Nevertheless, these two points excluded, the slope
The previous section has shown that the initial experimental is higher for higher feed ows (0.32%/h for 300 N mL/min, 0.46%/h
conditions (T = 120 C and 300 N mL/min gas ow) were too mild for 450 N mL/min).
to declassify the housekeeping waste. Thus, in order to optimize Despite that, Fig. 6 establishes that the higher the feed ow,
the operating conditions and anyway to avoid the combustion of the higher the detritiation yield. Furthermore, the gap between the
the housekeeping sample, experiments have been carried out at detritiation yields obtained using these two feed ows tends to
150 C. At this moment of the study, we were only able to compare demonstrate that the tritium contamination is mainly on the waste
the inuence of temperature with Ar + 2% O2 and Ar + 25% H2 O, the surface.
experiments using the other carrier gases being currently carried Table 3 sums up the results obtained for the detritiation of
out. soft housekeepings under air at different gas ows. As already
Fig. 5 shows the comparison of the detritiation yields as a func- mentioned in Section 3.1, due to the mild initial activities, it
tion of time for two different carrier gases at 120 C (dark dots) is impossible to conclude about the possibility to declassify the
and 150 C (light dots). It is visible that a reasonable temperature waste treated at 300 N mL/min. This conclusion is also valid for a
increase of 30 C leads to a considerable rise of the detritiation yield. 450 N mL/min-gas ow. Indeed, the initial activity of the sample is
Indeed, for both Ar2%O2 (diamonds) and Ar25%H2 O (triangles) clearly too close to the ILW/LLW threshold.
the detritiation yield has increased nearly vefold (5.023.6% for
Ar25%H2 O, 7.656.1% for Ar2%O2 ).
It is also interesting to observe that a slope break occurs after 3.4. Safety considerations
15 h for the 150 C Ar + 25% H2 O experiment, enlightening the
beginning of equilibrium between tritium removal and residual Considering that the membrane reactor which will be coupled
activity of the sample. with the existing detritiation facility uses hydrogen (protium) as
The residual activities listed in Table 2 show that 15 h have a swamping gas and that the efciency of the isotopic exchange
been enough to declassify to LLW the soft housekeeping treated by depends on the temperature (the optimal temperature has been
Ar2%O2 at 150 C. On the contrary, using Ar25%H2 O at 150 C does determined at around 400 C), it appears essential to assess the
not allow to declassify the waste yet. Nevertheless, if the behavior explosive hazard between hydrogen and Ar2%O2 which is the
of this experiment remained the same as its end (yield increase of most efcient carrier gases among those listed above.
approx. 0.75%/h), the declassication to LLW might be reached after Fig. 7 shows a detail of the ammability limits of a ternary nitro-
extra 13 h experimental time. gen/oxygen/hydrogen mixture as a function of the temperature.
The ammability regions have been determined by the CAST the-
3.3. Inuence of the carrier gas ow ory [14], ambient temperature (70 F) excepted. In this case, up to
400 C (752 F, corresponding to the working temperature of the
This study was useful for two different reasons. First of all, deter- membrane), the ammable region is never crossed.
mining the inuence of the residence time on the detritiation yield
allows one to assess the ow within an industrial detritiation facil-
ity and then the cost of the gas consumption, especially coupled
with a membrane reactor, where air cannot be used for safety rea-
sons. Moreover, this study has also allowed one to determine the
contamination mode of these housekeeping by tritium. Indeed, a
detritiation yield increasing with carrier gas ow would have indi-
cated that the sample was contaminated by tritium on its surface
while a constant detritiation yield would have shown that the most
part of tritium had penetrated the waste.
At this time of the study, only experiments with air have been
carried out. More experiments performed with other carrier gases
are foreseen to conrm the following conclusions which can be only
considered, up to now, as tendencies.
Fig. 6 shows the behavior of the detritiation yield as a function of
time for two different air ows. It is visible that the beginning of the
curves is quasi superposed for the 6 rst hours, which corresponds
to the rst day of experimentation. It is also remarkable to observe
that the following black diamond shown a jump, probably due to
a tritium degassing during the night. This phenomenon occurred
again during the second night stop (see the next-to-last black dia-
mond in Fig. 6). This is only visible on the 450 N mL/min experiment Fig. 7. Detail of ammable region limits of a ternary O2 /H2 /N2 mixture as a function
because that one has been carried out before the 300 N mL/min one of the temperature ( F) [14].
1044 X. Lefebvre et al. / Fusion Engineering and Design 87 (2012) 10401044
4. Conclusion and prospects
In this study, the detritiation efciencies of low activity-soft
housekeeping by different carrier gases at different temperatures
and ows have been assessed. In the future, it appears essential to
perform the same study on much higher sample amounts and much
higher tritium contaminated housekeeping waste as expected dur-
ing the ITER project.
The initial goal of this study was to demonstrate the tech-
nical feasibility of the detritiation of soft housekeepings under
mild conditions, i.e. without housekeeping combustion. After 18 h-
experiments, the 120 C-initial reference temperature is too mild to
declassify soft housekeeping waste weakly contaminated but also
to establish a hierarchy concerning the most efcient carrier gases,
even if the oxidative gases give higher detritiation yields. Thus, the
reference temperature was to be slightly increased up to 150 C.
The rst results of experiments carried out at this new refer-
ence temperature reveal that this temperature increasing leads to
a vefold detritiation yield increasing, leading to the possibility to
declassify waste treated with Ar2%O2 .
Further experiments currently carried out may conrm the sur-
face contamination of the waste by tritium as well as the inuence
of the feed ow on the detritiation yield.
The most appropriate carrier gas to be employed for housekeep-
ing detritiation and gaseous tritium recovery by the membrane
reactor designed by ENEA is Ar2%O2 , which will be used at 150 C.
This gas will allow to obtain reasonable detritiation efciency and
to have the advantage to be hazard-free toward hydrogen. The feed
ow rate needs to be optimized by a compromise between waste
detritiation and membrane permeability efciencies.
Acknowledgments
This work was supported by EURATOM and carried out within
the framework of the European Fusion Development Agreement
(EFDA JET Fusion Technology Program). The views and opinions
expressed herein do not necessarily reect those of the European
Commission.
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