Fusion Engineering and Design 109111 (2016) 14981501

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Fusion Engineering and Design

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

Gas leak tightness of SiC/SiC composites at elevated temperature

Daisuke Hayasaka a,b, , Joon-Soo. Park a , Hirotatsu Kishimoto a,b , Akira Kohyama a
a
OASIS, Muroran Institute of Technology, Muroran, Hokkaido, Japan
b
Graduate School of Engineering, Muroran Institute of Technology, Muroran, Hokkaido, Japan

h i g h l i g h t s

NITE-SiC/SiC has extremely densied microstructure compared with other SiC/SiC composite like CVI.
Excellent helium and hydrogen gas-leak tightness of SiC/SiC composites by DEMO-NITE method from prototype industrialization production line was
presented.
The excellence against stainless steel and Zircaloy at elevated temperature, together with generic excellent properties of SiC will be inevitable for
innovative blanket and divertors for DEMO- and power- fusion reactors.

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

Article history: SiC/SiC composite materials are attractive candidates for high heat ux components and blanket of fusion
Received 31 August 2015 reactor, mainly due to their high temperature properties, radiation damage tolerance and low induced
Received in revised form radioactivity. One of the challenges for SiC/SiC application in fusion reactors is to satisfy sufcient gas
20 November 2015
leak tightness of hydrogen and helium isotopes. Although many efforts have been carried-out, SiC/SiC
Accepted 27 November 2015
composites by conventional processes have not been successful to satisfy the requirements, except SiC/SiC
Available online 17 December 2015
composites by NITE-methods.
Toward the early realization of SiC/SiC components into fusion reactor systems process development of
Keywords:
DEMO-NITE process NITE-process has been continued. Followed to the brief introduction of recently developed DEMO-NITE
SiC/SiC composites process, baseline properties and hydrogen and helium gas leak tightness is presented.
Gas leak tightness SiC/SiC claddings with 10 mm in diameter and 1 mm in wall thickness are tested by gas leak tightness
High-heat ux component system developed. The leak tightness measurements are done room temperature to 400 C. Excellent gas
Blanket material leak tightness equivalent or superior to Zircaloy claddings for light water ssion reactors is conrmed.
The excellent gas leak tightness suggests nearly perfect suppression of large gas leak path in DEMO-NITE
SiC/SiC.
2015 Elsevier B.V. All rights reserved.

1. Introduction
SiC/SiC is well recognized to be an attractive material for high
heat ux components and blanket of fusion reactor, mainly due to
their high temperature properties, radiation damage tolerance and
low induced radioactivity [1]. One of the important properties for
fusion application is gas leak tightness/permeability of H, D, T and
He. This is important not only for fuel economy but also for safety
concern [2]. For the case of gas cooling blanket, helium is going to
be a candidate of coolant gas, where helium backward leakage into
fusion plasma is detrimental for fusion reaction [3].
Corresponding author at: Organization of Advanced Sustainability Initiative for
Energy System/Material, Mizumoto 27-1-Y203, Muroran, Japan. Tel.: +81 43465657.
E-mail address: hayasaka@oasis.muroran-it.ac.jp (D. Hayasaka).
SiC/SiC R & D for aerospace and nuclear fusion/ssion has been
accelerated since the Japanese invention of PCS type SiC bers, by
late Professor S. Yajima of Tohoku University. During these four
decades many fabrication processes have been developed. Among
those processes, CVD/CVI based process and NITE process have been
recognized to be the potential options for nuclear fusion/ssion
application. However, SiC/SiC by CVD/CVI process has been recog-
nized to be inherently leaky and the necessity of SiC seal coating
[4] and the new direction to move to hybrid design employing
metallic inserts or bladder are being pursued [5].
Whereas, Nano-powder Inltration and Transient Eutectoid
(NITE) processes has been intensively developed, starting at Kyoto
University [6] and now at OASIS, Muroran Institute of Technol-
ogy. Helium gas permeability of SiC/SiC composite was investigated
under the collaboration with Hokkaido University and CEA-Saclay
Laboratory, where excellent helium gas tightness was reported [7].

http://dx.doi.org/10.1016/j.fusengdes.2015.11.044
0920-3796/ 2015 Elsevier B.V. All rights reserved.
 D. Hayasaka et al. / Fusion Engineering and Design 109111 (2016) 14981501 1499

Encouraged by these attractive features, SiC/SiC cladding R & D

for GFR was carried out from 2001 to 2005, where 200 mm length
SiC/SiC cladding with 10 mm inner diameter and 1 mm wall thick-
ness was developed and two years later 0.8 mm wall thickness tube
with An excellent helium gas leak tightness cladding was fabricated
and supplied to CEA-Saclay Laboratory[8]. Since the establishment
of OASIS at Muroran Institute of Technology, March 2009, the orig-
inal NITE process has been drastically changed from wet aqua
slurry system to polymer-based slurry for making green sheets
and prepreg sheets as intermediate materials [9]. Process named
DEMO-NITE is a mass-production for fabrication of the preform and
currently continuous cladding fabrication process modication is
underway and the excellent helium and hydrogen gas leak tight-
ness at room temperature has been reported, where, helium gas
leak tightness presented is better than 1 1012 Pa m3 /s [10].
The objective of this work is to investigate helium and hydrogen
gas leak tightness at elevated temperature, as a preliminary eval-
uation of hydrogen and helium isotopes permeability for fusion
Fig. 2. Conceptual drawing of gas leak tightness test equipment.
reactor design.

2. Experimental procedure
SiC/SiC tube with 200 mm in length, 10 mm in inner diameter
and 1 mm in wall thickness was evaluated in this work, as shown in
Fig. 1. SiC/SiC bers were aligned to 60 along tube axis in multi-
layers. As reference materials, stainless steel tubes (SUS304) and
Zircaloy tubes (Zircaloy-2) were also measured.
Helium and hydrogen gas leak rate was measured by con-
ventional gas spray method to evacuated sample tube [11]. The
schematic illustration of the method is shown in Fig. 2. The fur-
nace used was cylindrical furnace with 15 mm inner diameter and
100 mm in length with Kanthal heaters, the maximum heating tem-
perature was 800 C and the uniform heating length is 30 mm at the
center of the furnace. The specimen temperature was measured
at the center surface of the test tube by K type TC attached. The
coupling apparatus was used to connect the tube to the measuring
system utilizing O-ring and uorinated grease (Z-300 by Ulvac co.).
The inner pressure of the tube was below 0.01 MPa and there was
no detectable differences for the cases of SiC/SiC.
The leak rate test apparatus detects and analyze the leak rate of
helium and hydrogen gases those were sprayed to the outer surface
of the sample, diffused through to the inner surface and released
into the inner cavity evacuated. There is a gas supply hole at the
center of the furnace. Outgassing of the test samples were done
at 400 C for 30 min. in vacuum chamber and the test was done
immediately take out the samples from the chamber. Gas tem-
perature was below 25 C at the mass-spectrometer. The very low
level of helium and hydrogen signal was detected before starting
the test and this was accounted as the background. The gas leak
rate measured includes many source of noises and in this study
valid detection limit was set to 2 1012 Pa m3 /s in helium and
1 108 Pa m3 /s in hydrogen.
3. Experimental results

Temperature dependence of helium gas leak rate is shown in

Fig. 3. As was mentioned, all test samples have better leak rate than
1 1012 Pa m3 /s at room temperature, thus, all data for SiC/SiC are
on bottom axis. For the case of stainless steel and Zircaloy tubes,
leak rate clearly increased around 250 C.
Temperature dependence of hydrogen gas leak rate is shown in
Fig. 4. The temperature dependence is quite similar for hydrogen
leak and for helium leak, but leak rate increase for hydrogen started
slightly higher temperature with rather steep increase behavior.

Fig. 1. DEMO-NITE SiC/SiC Tube studied. Fig. 3. Temperature dependence of helium leak rate.
1500 D. Hayasaka et al. / Fusion Engineering and Design 109111 (2016) 14981501
Fig. 4. Temperature dependence of hydrogen leak rate.
4. Discussion
4.1. Excellent gas leak tightness
As was mentioned the above, SiC/SiC by CVI/CVD method, in
general, includes larger than 15% porosity and resulted in poor
gas leak tightness. As an exceptional example, SiC/SiC by advanced
CVD/CVI method presented lower porosity than 10% [12]. The typ-
ical example of macro-structure difference in SiC/SiC composite by
CVD/CVI method and DEMO-NITE method is presented in Fig. 5.
Matrix densication in CVD/CVI method is based on chemical
vapor reaction, which required sufcient gas supply and matrix
densication disturbs the reaction gas supply to completely reduce
pores. As shown in Fig. 5, SiC/SiC CVI presented about 100 m pores
inter- ber bundles and about 10 m pores intra- ber bundles.
However, SiC/SiC by DEMO-NITE method presented no clear poros-
ity. The similar excellent gas leak tightness with CVI monolithic SiC
may indicate suppression of potential gas leak passes, such as cracks
or mist along SiC bers and matrix micro-cracks. This may be also
the reason of excellent thermal shock resistance [13].
Fig. 5. Macro-structure by CVD/CVI method and DEMO-NITE method.
Fig. 6. Arrhenius plot of helium leak rate.
4.2. Temperature dependence of gas leak tightness
The current gas leak rate data do not allow to extend quanti-
tative analysis based on gas diffusion mechanism. However, the
excellent gas leak tightness both for hydrogen and helium up to
500 C in this study can be interpreted the gas leak mechanism to
be bulk diffusion process through SiC dense matrix, grain bound-
ary diffusion and F/M interfacial diffusion, but no open channel gas
diffusion was observed, as was frequently observed in SiC/SiC by
different method.
Fig. 6 is Arrhenius plot of the helium gas leak rate, L. Under this
data detection limit, diffusion behavior of helium in SiC/SiC can-
not be analyzed, for helium diffusion coefcient is too small to be
analyzed in this level. As shown in this gure, the leak rate for the
case of CVD-SiC/SiC shows about ve order of magnitude higher
than NITE-SiC/SiC [14]. For the case of stainless steel and Zircaloy,
nominal helium leak rate equation can be obtained from the gure;
For stainless steel : L = 1.0 108 e4/RT
For Zircaloy : L = 1.3 103 e12/RT
where is constant reecting test condition, R is gas constant and
T is absolute temperature.
Fig. 7 is Arrhenius plot of the hydrogen gas leak rate. Under
this data detection limit, diffusion behavior of hydrogen in SiC/SiC
can hardly be analyzed, for hydrogen diffusion coefcient is too
small to be analyzed in this level. For the case of stainless steel
and Zircaloy, nominal hydrogen leak rate equation can be obtained
from the gure;
For stainless steel : L = 1.6 10e12/RT
For Zircaloy : L = 3.0 106 e20/RT
The furnace used in this experiment did not have sufcient
length of uniform high temperature region for test. Thus alpha
should be unity when the length is sufcient, however, as shown
 D. Hayasaka et al. / Fusion Engineering and Design 109111 (2016) 14981501
Fig. 7. Arrhenius plot of hydrogen leak rate.
in Fig. 7, from the data tting line gradient suggests that alpha vale
is 2. This value is consistent with the alpha value indicated in Refs.
[15,16].
Higher hydrogen leak rate in Zircaloy at lower temperature com-
paring with stainless steel looks questionable, but in consideration
of zirconium hydride formation, there will be a possibility. This will
be clearly analyzed and mechanistically claried under the much
higher sensitivity test in the furnace with sufcient uniform high
temperature region.
The preliminary data presented in this study is encouraging to
investigate further toward fusion reactor design from energy econ-
omy and safety concerns. From this preliminary work, excellence
of DEMO-NITE SiC/SiC against stainless steel and Zircaloy at ele-
vated temperature, even for the case of water cooling blanket and
this advantage will be overwhelmingly expanded for high temper-
ature blanket systems and high performance diverters for DEMO-
and power- fusion reactors.
Monolithic SiC coating on SiC/SiC composites as gas leak bar-
rier coating and environmental barrier coating has been carried
out and many excellent gas leak tightness results have been pub-
lished [17], simple and stable structure of DEMO-NITE SiC/SiC may
be recognized to be prime candidate concept for the future.
5. Summary
The very preliminary evaluation results of helium and hydro-
gen gas leak tightness for advanced SiC/SiC composite were
presented. The attractive potentiality of the advanced SiC/SiC
may require accelerated and international collaborative work
on SiC/SiC application for post-ITER, DEMO- and power fusion
reactors.
1501
Acknowledgements
Present study is partly supported by the Ministry of Educa-
tion, Culture, Sports, Science and Technology of Japan (MEXT)
on Innovative Nuclear Research and Development program. For
the SCARLET project. The supporting activities for making NITE-
SiC/SiC materials and basic property evaluation done through OASIS
with including utilization of FEEMA Facility. The members of OASIS,
Muroran Institute of Technology are also acknowledged for their
continuing supports for this study.
References
[1] S. Sharafat, R.H. Jones, A. Kohyama, P. Fenici, Status and prospects for SiCSiC
composite materials development for fusion applications, Fusion Eng. Des. 29
(1995).
[2] Y. Hatano, et al., Permeation of tritium and radioactive contamination and
decontamination, J. Plasma Fusion Res. 85 (2009) 726735.
[3] T. Nishio, S. Ueda, I. Aoki, R. Kurihara, T. Kuroda, H. Miura, T. Kunugi, Y. Seki, T.
Nagashima, M. Ohta, J. Adachi, S. Yamazaki, I. Kawaguchi, T. Hashimoto, K.
Shinya, Y. Murakami, H. Takase, T. Nakamura, Improved tokamak concept
focusing on easy maintenance, Fusion Eng. Des. 41 (1998) 357.
[4] R.H. Jones, Gas leak rate estimates for ceramic matrix composites, Fusion
Reactor Materials Semimanual Progress Report for Period Ending September
30, 1991, DOE/ER-0313/11, 1991, pp. 304308.
[5] Yang D Jae Ho, International presentation on SiC, in: Second Meeting of the
Expert Group on Accident Tolerant Fuels for Light Water Reactors, 2325
Sept., 2014, OECD/NEA HQ, 2014.
[6] A. Kohyama, K. Kotani, Y. Katoh, T. Nakayasu, M. Sato, Y. Yamamura, K.
Okamura, J. Nucl. Mater. 283287 (2000) 565.
[7] T. Hino, E. Hayashishita, Y. Yamauchi, M. Hashiba, Y. Hirohata, A. Kohyama,
Helium gas permeability of SiC/SiC composite used for in-vessel components
of nuclear fusion reactor, Fusion Eng. Des. 73 (April (1)) (2005) 5156.
[8] A. Kohyama, T. Hinoki, T. Mizuno, T. Kunugi, M. Sato, Y. Katoh, J.S. Park, R & D
of Advanced Material Systems for Reactor Core Component of Gas Cooled Fast
Reactor, in: Proceedings of ICAPP 05, Seoul, Korea, Paper 5282, 2005.
[9] A. Kohyama, Y. Kohno, H. Kishimoto, J.S. Park, H.C. Jung, Industrialization of
advanced SiC/SiC composites and SiC based composites; intensive activities at
Muroran Institute of Technology under OASIS, in: Proceedings of ICC3, 2010.
[10] J.S. Park, N. Nakazato, H. Nishimura, D. Hayasaka, H. Kishimoto, A. Kohyama,
To Be Published as Proceedings of NUMAT 2014, 2015.
[11] Japanese Industrial Standards, JIS Z2331, Method for helium leak testing,
2006.
[12] T. Goto, High Speed Deposition of SiC Coating by Laser Chemical Vapor
Deposition, in: To Be Published as Proceedings of CMCEE-11, 2015.
[13] A. Kohyama, D. Hayasaka, H. Kishimoto, J.S. Park, High Performance SiC/SiC
Component by NITE-method and its application to energy and environment,
in: To Be Published as Proceedings of CMCEE-11, 2015.
[14] C. Sauder, C. Lorrette, F. Audubert, A. Michaux, C. Colin, P. David, A. Coup, L.
Ph Berne, J.L. Briottet, L. Sran, Chaffron, Innovative SiCf /SiC composite
materials for fast reactor applications, in: Colloque MECAMAT 2011Aussois,
2011.
[15] H. Hagi, T. Yanagawa, Hydrogen Penetration into SUS304 Stainless Steel and
Hydrogen Embrittlement Caused by Cathodic Polarization, Memoirs of the
Fukui Institute of Technology, Fukui, 2008, pp. 38.
[16] H. Ogawa, T. Saburi, K. Kiuchi, Basic Evaluation on Metal-Hydrogen
Interaction for Selecting Cladding Material, JAERI-Research 2000-055, JAERI,
2000, http://jolissrch-inter.tokai-sc.jaea.go.jp/abstracts/seika/jp/reports
2005/reports JAERI-Research.html. http://jolissrch-inter.tokai-sc.jaea.go.jp/
pdfdata/JAERI-Research-2000-055.pdf.
[17] H.E. Khalifa, C.P. Deck, O. Gutierrez, G.M. Jacobsen, C.A. Back, Fabrication and
characterization of joined silicon carbide cylindrical components for nuclear
applications, J. Nucl. Mater. 457 (2015) 227240.