Sei sulla pagina 1di 6

Nuclear Engineering and Technology 50 (2018) 253e258

Contents lists available at ScienceDirect

Nuclear Engineering and Technology


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

Original Article

Development status of microcell UO2 pellet for accident-tolerant fuel


Dong-Joo Kim*, Keon Sik Kim, Dong Seok Kim, Jang Soo Oh, Jong Hun Kim, Jae Ho Yang,
Yang-Hyun Koo
Nuclear Fuel Safety Research Division, Korea Atomic Energy Research Institute, 111, Daedeok-daero 989Beon-gil, Yuseong-gu, Daejeon 34057, South Korea

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

Article history: A microcell UO2 pellet, as an accident-tolerant fuel pellet, is being developed to enhance the accident
Received 9 November 2017 tolerance of nuclear fuels under accident conditions as well as the fuel performance under normal
Received in revised form operation conditions.
8 December 2017
Improved capture-ability for highly radioactive and corrosive fission product (Cs and I) is the distinct
Accepted 20 December 2017
feature of a ceramic microcell UO2 pellet, and the enhanced pellet thermal conductivity is that of a
Available online 11 January 2018
metallic microcell UO2 pellet. The fuel temperature can be effectively decreased by enhanced thermal
conductivity.
Keywords:
Accident-Tolerant Fuel
In this study, the material concepts of metallic and ceramic microcell UO2 pellets were designed, and
Fission Product Retention the fabrication process of microcell UO2 pellets embodying the designed concept was developed. We
Halden Irradiation Test successfully implemented the microcell UO2 pellets and produced microcell UO2 pellets.
Microcell UO2 Pellet In addition, an assessment of the out-of-pile properties of a microcell UO2 pellet was performed, and
Thermal Conductivity the in-reactor performance and behavior of the developed microcell pellets were evaluated through a
Halden irradiation test. According to the expectations, the excellent performance of the microcell UO2
pellets was confirmed by the online measurement data of the Halden irradiation test.
© 2018 Korean Nuclear Society, Published by Elsevier Korea LLC. This is an open access article under the
CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

1. Introduction The metallic microcell UO2 pellet is a highly thermal conductive


pellet with a continuously connected metallic wall (Fig. 2). A cold
Several ATF concepts are currently being suggested and evalu- pellet reduces the fission product release by slowing down the
ated to mitigate the consequences of an accident [1e7]. At the diffusion, that is, the mobility of the fission gases is reduced by the
Korea Atomic Energy Research Institute (KAERI), a microcell UO2 lower temperature gradient in the UO2 fuel pellet. The reduced
pellet as an ATF pellet is being developed to enhance the accident temperature gradient mitigates the relocation and pellet-cladding
tolerance of nuclear fuels under accident conditions as well as the mechanical interaction during a transient operation because of the
fuel performance under normal operating conditions [8e10]. decreased thermal stress in the pellet. In addition, a microcell UO2
The microcell consists of UO2 grains or granules enveloped by pellet with high thermal conductivity significantly increases the
thin cell walls that are continuously connected. Fig. 1 shows a safety margin under design basis accidents such as a loss-of-
conceptual schematic representation of a microcell UO2 pellet. The coolant accident as well as the thermal and operational margin
main purpose of the microcell UO2 pellets is to minimize the release under normal operating conditions [11e13].
of highly radioactive and corrosive fission products (Cs and I) from The ceramic wall in ceramic microcell UO2 pellets is composed
the fuel and to reduce the pellet temperature for an enhanced fuel of an oxide phase with chemical affinity to volatile fission products
safety margin. There are two kinds of microcell UO2 pellets under (Cs and I), which acts as multiple traps to immobilize the volatile
development at the KAERI, classified according to the type of ma- fission products (Fig. 2). In this way, the ceramic microcell walls
terial composing the cell walls: metallic microcell UO2 pellets and block the migration of fission products to the pellet outside. The
ceramic microcell UO2 pellets, each with distinct features. increased retention capability of the fission products reduces the
stress corrosion cracking at the inner surface of the cladding as well
as the rod internal pressure. In addition, a soft ceramic wall facili-
* Corresponding author. tates the fast creep deformation of the pellets, thereby reducing the
E-mail address: djkim@kaeri.re.kr (D.-J. Kim). mechanical stress of the cladding under operational transients.

https://doi.org/10.1016/j.net.2017.12.008
1738-5733/© 2018 Korean Nuclear Society, Published by Elsevier Korea LLC. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/
licenses/by-nc-nd/4.0/).
254 D.-J. Kim et al. / Nuclear Engineering and Technology 50 (2018) 253e258

Fig. 1. Conceptual schematic representation of a microcell UO2 pellet.

Fig. 2. Conceptual schematic representation of a metallic and ceramic microcell pellet.

These benefits are expected to enhance the robustness of a fuel severe accident, thereby reducing the release of retained radio-
rod during a severe accident as well as during normal operation. toxic fission products into the environment.
The large-sized grain and mesh-like rigid wall structures are also To implement the designed fuel concept, the KAERI has devel-
expected to prevent the massive fragmentation of pellets during a oped a fabrication process for microcell UO2 pellets that embodies
D.-J. Kim et al. / Nuclear Engineering and Technology 50 (2018) 253e258 255

Fig. 3. The microstructure of Cr metalecontaining metallic microcell UO2 pellet (a panoramic image of pellet radial direction from end to end).

the designed concept. In addition, assessments of the out-of-pile iodine [14], the chemical affinity of the wall to cesium may
properties of a microcell UO2 pellet are being performed by deeply impact the retention capability of the fission products.
various out-of-pile tests, and observations of the in-reactor per- Insolubility of the wall materials in a UO2 matrix is also an
formance and behavior of the developed pellets are in progress important requirement to maintain the microcell structure.
through Halden irradiation tests. This article describes the devel- Recent test results for AleSieO-doped UO2 suggest the chemical
opment status of the microcell UO2 pellet for ATF. trapping of volatile fission products in an SiO2-based additive
phase and a decreased possibility of the availability of aggressive
2. Fabrication of microcell UO2 pellets species in the inside cladding [15,16]. We therefore selected
several SiO2-based mixed oxides as additive candidates for
Many candidate metals for a metallic microcell wall material ceramic cell wall materials.
have been assessed and screened on the basis of their physical To fabricate the ceramic microcell UO2 pellets, we used a con-
properties such as the thermal conductivity, neutron absorption ventional liquid phase sintering technique. A powder mixture of
cross section, melting temperature, and so on. Mo and Cr were UO2 and additives was pressed into green pellets, which were then
primarily selected as metallic cell wall materials because they have sintered at an elevated temperature at which the additives for the
a relatively high melting temperature, high thermal conductivity, wall materials formed a liquid phase, penetrating through grain
and manageable neutron absorption cross section. In addition, it is boundaries and enveloping the UO2 grains to make the designed
significantly required that the Mo and Cr are compatible with a UO2 ceramic microcell.
matrix under the sintering conditions of the pellet fabrication Fig. 4 shows the microstructure of the ceramic microcell UO2
process. pellet. This pellet was obtained by mixing a 0.6 wt% SiO2eTiO2 oxide
Fig. 3 shows the microstructure of a 5 vol% Cr metal phase mixture with UO2 powder and then sintering the powder mixture at
containing metallic microcell UO2 pellets, in which the microcell 1,720 C for 4 hours in a dry hydrogen atmosphere. The sintered
concept was successfully implemented. The metallic microcell pellet density and averaged cell (grain) size were ~97.9% T.D. and
pellet was fabricated by the cosintering of metal powder over- ~80 mm, respectively. Energy dispersive spectroscopy mapping im-
coated UO2 granules through a conventional sintering process. ages revealed that the additive elements were isolated in the grain
Metal powder over-coated UO2 granules, which were prepared by boundary.
mixing metal powders and UO2 granules, were pressed into green
pellets. After that, the green pellets were sintered in a dry hydrogen 3. Out-of-pile properties of microcell UO2 pellets
atmosphere. The sintered density and averaged cell (granule) size
of the fabricated 5 vol% Cr metallic microcell UO2 pellet were ~97.0% Various out-of-pile tests were conducted to evaluate the
T.D. and ~290 mm, respectively. thermo-physical properties and fuel behaviors under the normal
The ceramic microcell wall materials require chemical affinity operating conditions and accident conditions.
to Cs to form stable compounds with incorporated Cs. Because The thermal conductivity and linear thermal expansion of the
the fission yield of Cs is roughly 10 times larger than that of metallic microcell UO2 pellets were measured. Fig. 5 shows the

Fig. 4. The microstructure and EDS mapping images of SieTieO-containing ceramic microcell UO2 pellet.
EDS, energy dispersive spectroscopy.
256 D.-J. Kim et al. / Nuclear Engineering and Technology 50 (2018) 253e258

1,000 C. The fuel temperature can be effectively decreased by the


enhanced thermal conductivity of the pellet. The linear thermal
expansion coefficient of the Mo metallic microcell UO2 pellet
decreased with an increasing Mo content because of the lower
thermal expansion coefficient of Mo (~4.8  10 6/K at 25 C) than
that of UO2 (~10  10 6/K). Under the transient conditions, it is
expected that the mechanical stress on the cladding due to pellet
expansion can be reduced by this feature of the metallic microcell
pellet.
Maintaining pellet-structural stability under a high-
temperature steam environment is an important property for fuel
pellets. Therefore, we investigated the steam oxidation behaviors of
Mo metallic microcell UO2 pellets. Morphology changes in the
polished surface of the sample pellets after steam oxidation tests
were observed. In the oxidation test in 500e800 C steam, even the
pellet fragmentation and pulverization due to oxidation were
retarded in the Mo metallic microcell UO2 pellets. The surface of the
pure UO2 pellets was damaged due to the oxidation along the grain
Fig. 5. The thermal conductivity measurement results of metallic microcell UO2 boundary, whereas the Mo microcell UO2 pellets maintained a
pellets [9]. sound surface morphology.
The melting temperatures of both Cr (~1,907 C) and Mo
(~2,623 C) are lower than that of UO2 (~2,865 C). Therefore, what
will happen in a metallic microcell UO2 pellet when the pellet
temperature is increased to the temperature higher than the
melting point of a metallic wall is one of the main concerns of a
metallic microcell UO2 pellet. A thermal transient annealing test
was carried out to verify the structural integrity of both Cr- and Mo-
containing metallic microcell pellets, and the results confirmed
that the microcell pellet was well preserved, even after being
annealed at higher temperature than the melting point of the wall.
For the ceramic microcell UO2 pellet, the thermal diffusivity and
thermal expansion test results showed that the thermal properties
of the ceramic microcell UO2 pellet were similar to those of a UO2
pellet. In addition, the compressive-creep deformation of ceramic
microcell pellets at high temperature was faster than that of a UO2
pellet (Fig. 6). The fast creep deformation indicates that the ceramic
microcell pellets can reduce the mechanical stress on the cladding
during a transient or accident as well as during normal operation.
The ceramic microcell wall material is an oxide phase that has
Fig. 6. Comparison of the compressive-creep deformation behavior of a UO2 pellet and inherent stability in a steam environment. The experiment results
SieTieO ceramic microcell UO2 pellet.
showed an enhanced resistance to steam oxidation in the ceramic
microcell UO2 pellet (Fig. 7). This enhancement may be related to
thermal conductivity measurement results of 5 vol% Mo and 5 vol% the large grain size of ceramic microcell UO2 pellets. A thermal
Cr metallic microcell UO2 pellets. The thermal conductivity of the transient annealing test at a higher temperature than the melting
pellets were remarkably enhanced, and the thermal conductivity of point of the ceramic wall revealed that the structural integrity of
the 5 vol% Mo metallic microcell UO2 pellet increased by 100% at pellets was well preserved after the test.

Fig. 7. Comparison of the steam oxidation behavior of a UO2 pellet and SieTieO ceramic microcell UO2 pellet.
D.-J. Kim et al. / Nuclear Engineering and Technology 50 (2018) 253e258 257

Table 1
Specifications of microcell pellet samples currently being irradiated in the Halden reactor.

Ceramic microcell pellet Metallic microcell pellet

Cell wall materials 0.6 wt% SieTieO (2 vol%) 3.4 wt% Cr (5 vol%)
Averaged cell sizea (mm) ~80 ~290
Pellet density (g/cc) 10.73 ± 0.03 (~97.9% T.D.) 10.45 ± 0.03 (~97.0% T.D.)
Pellet diameterb (mm) 8.190 ± 0.002 8.196 ± 0.001
Pellet height (mm) 9.4 ± 0.2 9.12 ± 0.03
Pellet weight (g) 5.15 ± 0.10 4.93 ± 0.02
U enrichment 4.5%-U235 4.5%-U235
a
A ceramic microcell consists of one grain (~80 mm). Therefore, the cell size of a ceramic microcell pellet is equal to the grain size. On the
other hand, a metallic microcell consists of a lot of grains (~8 mm).
b
Pellet diameter after centerless grinding process.

Fig. 8. Online measurement data of fuel centerline temperature of UO2 reference pellet and Cr metallic microcell UO2 pellet as a function of the operation time. ALHR, averaged
linear heat generation rate.

4. In-reactor performance of microcell UO2 pellets These results confirmed that the metallic microcell UO2 pellet had a
beneficial effect on the fuel temperature. The online data of the fuel
In the development of microcell fuel, the irradiation behavior of temperature were in good agreement with the predicted data
the developed microcell UO2 pellet material must be investigated based on a computational simulation [17]. Until now, the temper-
based on various aspects (pellet microstructure, pellet-structural ature difference between the UO2 reference pellet and Cr metallic
integrity, cell wall soundness, cell wall material behavior and microcell UO2 pellet has been consistently maintained. This is
redistribution, soundness of interface between microcell wall and direct evidence that the metallic microcell structures were pre-
UO2, reaction between cell wall material and fission products, etc.). served well. The irradiation testing of microcell UO2 pellets is
Above all, it is important that the designed in-reactor fuel perfor- ongoing at above ~12,000 MWd/mtU according to plan and is
mances of the microcell UO2 pellet are verified. proceeding to reach a higher burnup.
Through cooperation with Thor Energy in Norway, a Halden
irradiation test of the microcell UO2 pellets is now in progress. The
KAERI is participating in the International Thorium Consortium 5. Summary
organized by Thor Energy. Two kinds (ceramic and metallic) of
microcell UO2 pellets were fabricated in accordance with the re- A microcell UO2 pellet is being developed as an ATF pellet to
quirements for the Halden irradiation test (Table 1). The number of enhance the accident tolerance of nuclear fuels under accident
samples (~60 EA each) was sufficiently provided for manufacturing conditions as well as the fuel performance under normal operating
the instrumented rigs. The irradiation test rigs with in- conditions. We designed material concepts of metallic and ceramic
strumentations were manufactured at the Institute for microcell UO2 pellets and developed a fabrication process for
Energiteknikk in Norway. microcell UO2 pellets that embodied the design concept.
Fig. 8 shows the online measurement data of the fuel centerline In addition, ongoing assessment of the out-of-pile properties of
temperature of a 5 vol% Cr metallic microcell UO2 pellet that is a microcell UO2 pellet is being performed, and observation of the
being irradiated in the Halden reactor. The 5 vol% Cr metallic in-reactor performance and behavior of the developed microcell
microcell UO2 fuel exhibited a temperature that was remarkably pellets is progressing through Halden irradiation testing. According
lower than the reference UO2 fuel, typically ~20% lower. In the to our expectations, excellent performances of the microcell UO2
preliminary calculation results, the Cs diffusion coefficient in UO2 pellets are being verified by the online measurement data of Hal-
decreased by about 1/1,000 due to the 20% lower fuel temperature. den irradiation tests.
258 D.-J. Kim et al. / Nuclear Engineering and Technology 50 (2018) 253e258

Conflict of interest [7] J.G. Stone, R. Schleicher, C.P. Deck, G.M. Jacobsen, H.E. Khalifa, C.A. Back, Stress
analysis and probabilistic assessment of multi-layer SiC-based accident
tolerant nuclear fuel cladding, J. Nucl. Mater. 466 (2015) 682e697.
No conflict of interest. [8] Y.H. Koo, J.H. Yang, J.Y. Park, K.S. Kim, H.G. Kim, D.J. Kim, Y.I. Jung, K.W. Song,
KAERI's development of LWR accident-tolerant fuel, Nucl. Technol. 186 (2014)
Acknowledgments 295e304.
[9] H.G. Kim, J.H. Yang, W.J. Kim, Y.H. Koo, Development status of accident-
tolerant fuel for light water reactors in Korea, Nucl. Eng. Technol. 48 (1)
This work was supported by the National Research Foundation (2016) 1e15.
of Korea (NRF) grant funded by the Korea government (MSIT: [10] D.J. Kim, Y.W. Rhee, J.H. Kim, K.S. Kim, J.S. Oh, J.H. Yang, Y.H. Koo, K.W. Song,
Fabrication of microcell UO2-Mo pellet with enhanced thermal conductivity,
Ministry of Science and ICT) (No. 2017M2A8A5015056). J. Nucl. Mater. 462 (2015) 289e295.
[11] K.A. Terrani, D. Wang, L.J. Ott, R.O. Montgomery, The effect of fuel thermal
References conductivity on the behavior of LWR cores during loss-of-coolant accidents,
J. Nucl. Mater. 448 (2014) 512e519.
[12] N.R. Brown, A.J. Wysocki, K.A. Terrani, K.G. Xu, D.M. Wachs, The potential
[1] I. Younker, M. Fratoni, Neutronic evaluation of coating and cladding materials
impact of enhanced accident tolerant cladding materials on reactivity initi-
for accident tolerant fuels, Prog. Nucl. Energy 88 (2016) 10e18.
ated accidents in light water reactors, Ann. Nucl. Energy 99 (2017) 353e365.
[2] M.Q. Awan, L. Cao, H. Wu, Neutronic design and evaluation of a PWR fuel
[13] X. Wu, W. Li, Y. Wang, Y. Zhang, W. Tian, G. Su, S. Qiu, T. Liu, Y. Deng,
assembly with accident tolerant-fully ceramic micro-encapsulated (AT-FCM)
H. Huang, Preliminary safety analysis of the PWR with accident-tolerant fuels
fuel, Nucl. Eng. Des. 319 (2017) 126e139.
during severe accident conditions, Ann. Nucl. Energy 80 (2015) 1e13.
[3] K.D. Johnson, A.M. Raftery, D.A. Lopes, J. Wallenius, Fabrication and micro-
[14] G. Brillant, F. Gupta, A. Pasturel, Fission products stability in uranium dioxide,
structural analysis of UN-U3Si2 composites for accident tolerant fuel applica-
J. Nucl. Mater. 412 (2011) 170e176.
tions, J. Nucl. Mater. 477 (2016) 18e23.
[15] J. Matsunaga, Y. Takagawa, K. Kusagaya, K. Une, R. Yuda, M. Hirai, Funda-
[4] C.P. Deck, G.M. Jacobsen, J. Sheeder, O. Gutierrez, J. Zhang, J. Stone, H.E. Khalifa,
mentals of GNF Al-Si-O additive fuel, TopFuel 2009, Paris, France, September
C.A. Back, Characterization of SiC-SiC composites for accident tolerant fuel
6e10, American Nuclear Society, 2009.
cladding, J. Nucl. Mater. 466 (2015) 667e681.
[16] D. Jadernas, F. Corleoni, A. Puranen, P. Tejland, M. Granfors, PCI mitigation
[5] X. Wu, T. Kozlowski, J.D. Hales, Neutronics and fuel performance evaluation of
using fuel additives, TopFuel 2015, Zurich, Switzerland, September 13e17,
accident tolerant FeCrAl cladding under normal operation conditions, Ann.
American Nuclear Society, 2015.
Nucl. Energy 85 (2015) 763e775.
[17] H.S. Lee, D.J. Kim, S.W. Kim, J.H. Yang, Y.H. Koo, D.R. Kim, Numerical charac-
[6] J.H. Park, H.G. Kim, J.Y. Park, Y.I. Jung, D.J. Park, Y.H. Koo, High temperature
terization of microcell UO2-Mo pellet for enhanced thermal performance,
steam-oxidation behavior of arc ion plated Cr coatings for accident tolerant
J. Nucl. Mater. 477 (2016) 88e94.
fuel claddings, Surf. Coat. Technol. 280 (2015) 256e259.

Potrebbero piacerti anche