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http://dx.doi.org/10.5516/NET.07.2013.

713

MODELING OF INTERACTION LAYER GROWTH BETWEEN


U-Mo PARTICLES AND AN Al MATRIX
YEON SOO KIM1*, G.L. HOFMAN1, HO JIN RYU2, JONG MAN PARK3, A.B. ROBINSON4, and D.M. WACHS4
1
Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 USA
2
Dept. of Nuclear and Quantum Engineering, Korea Advanced Institute of Science and Technology
291 Daehak-ro, Yuseong-gu, Daejeon 305-701 Republic of Korea
3
Korea Atomic Energy Research Institute, 989-111 Daedeokdaero, Yuseong-gu, Daejeon 305-353 Republic of Korea
4
Idaho National Laboratory, P.O. Box 1625, Idaho Falls, ID 83415-6188 USA
*
Corresponding author. E-mail : yskim@anl.gov

Received October 31, 2013

Interaction layer growth between U-Mo alloy fuel particles and Al in a dispersion fuel is a concern due to the volume
expansion and other unfavorable irradiation behavior of the interaction product. To reduce interaction layer (IL) growth, a
small amount of Si is added to the Al. As a result, IL growth is affected by the Si content in the Al matrix. In order to predict
IL growth during fabrication and irradiation, empirical models were developed. For IL growth prediction during fabrication and
any follow-on heating process before irradiation, out-of-pile heating test data were used to develop kinetic correlations. Two
out-of-pile correlations, one for the pure Al matrix and the other for the Al matrix with Si addition, respectively, were
developed, which are Arrhenius equations that include temperature and time. For IL growth predictions during irradiation, the
out-of-pile correlations were modified to include a fission-rate term to consider fission enhanced diffusion, and multiplication
factors to incorporate the Si addition effect and the effect of the Mo content. The in-pile correlation is applicable for a pure Al
matrix and an Al matrix with the Si content up to 8 wt%, for fuel temperatures up to 200 ºC, and for Mo content in the range
of 6 – 10wt%. In order to cover these ranges, in-pile data were included in modeling from various tests, such as the US
RERTR-4, -5, -6, -7 and -9 tests and Korea’s KOMO-4 test, that were designed to systematically examine the effects of the
fission rate, temperature, Si content in Al matrix, and Mo content in U-Mo particles. A model converting the IL thickness to
the IL volume fraction in the meat was also developed.
KEYWORDS : U-Mo, U-Mo/Al, Dispersion Fuel, Interaction Layer, IL Growth, Modeling, In-pile Data

1. INTRODUCTION

U-Mo alloy fuel is a prime candidate for conversion


of high-power research and test reactors, from HEU cores
to LEU cores, thanks to its high density and advantageous
irradiation performance. Two forms of U-Mo alloy fuel
have been studied in the U.S. GTRI-CONVERT program
(formerly known as RERTR): One is U-Mo particle
dispersion in an Al matrix (U-Mo/Al dispersion fuel); the
other is direct bonding of U-Mo thin foil to Al-alloy
cladding (U-Mo monolithic fuel) (Fig. 1). In this paper,
because modeling the interaction layer growth between
the U-Mo particles and Al matrix was concerned, we
focused only on the dispersion fuel form.
One of the intrinsic characteristics of the U-Mo/Al
dispersion fuel is perhaps the interaction layer (IL) growth
between the U-Mo fuel particles and matrix Al. Interaction
layer growth is due to interdiffusion between the fuel particle
(U and Mo) and matrix (Al). Hofman and co-workers [1]
reported the first observation of IL growth in U-Mo/Al Fig. 1. Schematic Illustration of Cross Section Views of
from an irradiation test, where they also proposed a corre- Dispersion Fuel and Monolithic Fuel Forms

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KIM et al., Modeling of Interaction Layer Growth between U-Mo Particles and an Al Matrix

lation for IL growth expressed as a function of the fission test results from the RERTR-9 and KOMO-4. The high
rate, temperature, and time. Hayes [2] later incorporated temperature test KOMO-4 showed that a Si content higher
this model in a computer model PLATE. Ryu and co- than 2 wt% had different IL growth kinetics [39],[49].
workers [3] systematically measured the kinetics of IL Therefore, a model applicable to the high temperature
growth and obtained the activation energy for IL growth regime and a Si content higher than 2 wt% was necessary.
for out-of-pile heating tests. Another objective of the present work is to unify the existing
U-Mo/Al dispersion fuel performed well in irradiation separate models for the pure Al matrix and the Al matrix
tests at lower power and burnup, so its qualification appeared with Si addition.
near [4]. However, later tests adopting higher power, i.e., An interaction layer can also grow during fabrication
higher fission rate and higher burnup, showed enhanced and the follow-on blister test when the fuel plates undergo
fuel-meat swelling, which was caused by massive IL growth, heat processes. An IL growth model in this step was also
and in some cases, by large pore formation in the fuel meat required.
[5],[6]. The pores were distinguishable from the fission gas
bubbles in the fuel particles, in that they mostly formed
outside of fuel particles, i.e., in the ILs, although both were 2. MODELS FOR OUT-OF-PILE INTERACTION
commonly filled with fission gases. The formation of IL
results in a net volume increase and a net thermal conduc-
LAYER GROWTH
tivity decrease in the meat. The low thermal conductivity
of IL provides adverse feedback for higher IL growth by 2.1 Al Matrix with no Si Addition
further increasing the fuel meat temperature. While U- IL growth during fuel fabrication and any follow-on
Mo particles and Al are crystalline, ILs formed between heating test is modeled in this section. The interaction layer
U-Mo and Al are amorphous during irradiation [7],[8]. The growth between U-Mo and Al is a typical interdiffusion
amorphous nature of the ILs is believed to be the reason process between U and Mo atoms versus Al atoms. Hence,
for large pores formed outside of fuel particles [9]. Fission in this paper, interaction and interdiffusion are used inter-
gas diffusivity in the amorphous ILs is higher than in its changeably. In addition, the rate-controlling process in
crystalline state, and viscosity is lower, both of which interaction layer growth is interdiffusion, not the reaction
promote fission-gas-pore formation in the ILs. product formation [11]. The out-of-pile IL growth takes
A remedy was needed to reduce the IL growth rate the following modified Arrhenius correlation because
and strengthen the IL to resist against pore formation and interdiffusion is due to thermal activation:
growth. Noticing the low IL growth between U3Si2/Al
dispersion that did not form pores in the IL until full LEU (1)
burnup (see [10],[11]), it was proposed at ANL that a
small amount of silicon be added to the aluminum matrix
[12],[13]. An ample number of studies, both out-of-pile where YAl is the average IL thickness (μm) in a pure Al
([14]-[25]) and in-pile ([26]-[42]), have been conducted matrix, i.e., Al matrix without any intentional Si addition,
to examine the effectiveness and better application of the T is the fuel meat temperature in K, and t is the time in s.
remedy. The common findings were that Si addition to Al The constants have been fitted using the data taken from
not only reduced IL growth, but also delayed pore formation Ryu [3] (Table 1). Only data from dispersion fuel tests
and growth in the IL. Hence, overall performance of this were used. The IL thickness was measured using optical
fuel was improved. micrographs of the cross section of a sample. From an
Since IL growth is one of the deciding performance optical micrograph, several IL thicknesses were measured,
variables for U-Mo/Al dispersion fuel, an accurate model and the average value was used as the nominal value.
is also required. The studies for interaction layer (IL) growth The method to obtain the true IL thickness is explained
modeling for in-pile applications includes two cases: one elsewhere [50]. Generally, in an optical micrograph, the
for the pure Al matrix case [1],[2],[43],[45], and the other common thinnest IL on the largest particle was taken to
for the Si-added matrix case [28],[48]. The most up-to-date represent the true IL thickness.
correlation for the pure Al matrix case was by Wachs [45], The RERTR test-plates were fabricated using the hot
which was confirmed as accurate by Kim [48]. The corre- rolling technology [51], in which the heat processes involved
lation for the Si-added matrix case, developed mostly on were much shorter, ~1 h, but at a much higher temperature,
low-temperature miniplate test data, was applied for all 500 ºC, than in-pile tests (Table 2, Table 3). For example,
Si contents larger than 2 wt%. There was no need to provide the test duration for the RERTR-4 test was 257 d, and the
a separate factor to consider the effect as a function of life-average fuel temperature was ~100 ºC.
the Si content, because in the low temperature tests the IL growth during fabrication is hard to assess, so the
addition of 2 wt% Si virtually suppresses IL growth to correlation given in Eq. (1) is for an average value. The
the lowest possible level. However, it has been noticed largest uncertainty during fabrication is due to the irregular
that the modeling under-predicts the high temperature contact pressure between particles with the matrix. For a

828 NUCLEAR ENGINEERING AND TECHNOLOGY, VOL.45 NO.7 DECEMBER 2013


KIM et al., Modeling of Interaction Layer Growth between U-Mo Particles and an Al Matrix

typical rolling process used for RERTR test plates [51], samples of the KOMO-4 test from KAERI were produced
the bonding between the U-Mo particles and matrix is poor using an extrusion process taking 0.5 hour at 400 ºC, for
during the pre-heating and first pass, so IL growth during which Eq. (1) predicts negligible IL thickness. Table 2
these steps is virtually negligible. Meaningful bonding is compares the heat processes and IL growth involved during
achieved after the second pass and subsequent IL growth fabrication of some RERTR tests and the KOMO-4 test.
occurs during the last heating ~15 min (see [51] for detailed The Mo content of the U-Mo particles is in the range
time and temperature for each step). The most IL growth of 6 – 10 wt%. However, the most common Mo contents
takes place during the subsequent blister-annealing test at are 7 wt% and 10 wt% in the RERTR irradiation tests. In
485 ºC for an hour. Using Eq. (1), we estimated an average the Mo-content 10 wt%, the thermodynamic equilibrium
of ~1.5 μm of IL growth during fabrication. The test phase of the U-Mo is the -U + -U2Mo dual phase at

Table 1. IL Growth between U-Mo a and Al from Out-of-pile Heating Tests, RERTR Tests and KOMO-4 Test during Fabrication and
Follow-on Blister Test
Heating Average IL e
Source Matrix Ref.
temp (ºC) time (h) (μm)

Ryu Al 500 1b 2.0 [3]


Ryu Al 525 1b 3.6 [3]
Ryu Al 550 1b 8.4 [3]
Park Al-5Si 580 1 b
8 [39]
Iltis Al-4Si 425 2c 0.5 e
[23]
Iltis Al-4Si 475 2c 0.6 e [23]
Iltis Al-6Si 425 2c 0.4 e [23]
Iltis Al-6Si 475 4 c
1.1 e
[23]
Keiser Al-2Si 450 4d 0.2 f
[24]
Keiser Al-2Si 475 4d 0.4 f [24]
Keiser Al-2Si 500 2d 1.0 f [24]
Keiser Al-4Si 450 4 d
0.6 f
[24]
Keiser Al-4Si 475 4d 0.7 f
[24]
Keiser Al-4Si 500 2d 0.7 f [24]
Keiser Al-4Si 525 1d 0.8 f [24]
Keiser Al-5Si 450 4 d
0.4 f
[24]
Keiser Al-5Si 475 4d 0.7 f
[24]
Keiser Al-5Si 500 2d 1.2 f [24]
Keiser Al-6Si 450 4d 0.7 f [24]
Keiser Al-6Si 475 4 d
0.8 f
[24]
Keiser Al-6Si 500 2d 0.9 f
[24]
Keiser Al-6Si 525 1d 0.8 f [24]
a: Fuel kernels are all U-7wt%Mo atomized particles except for Ryu’s U-10wt%Mo atomized particles
b: Fabricated at 400 ºC by co-extrusion. IL during fabrication is negligible.
c: Fabricated at 425 ºC by hot rolling. IL ~0.2 μm forms during fabrication.
d: Fabricated at 425 ºC by hot rolling. IL ~0.2 μm forms during fabrication.
e: IL growth during fabrication (0.2 μm) is subtracted.
f: IL growth during fabrication (0.2 μm) is subtracted. Only IL thickness on the -phase U-Mo is considered.

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KIM et al., Modeling of Interaction Layer Growth between U-Mo Particles and an Al Matrix

temperatures below ~550 ºC. For other Mo content in the surface and formation of a Si-barrier on the fuel surface
range of 6 – 10 wt%, the phase boundary is slightly higher to block Al diffusion. This further contributes to the formation
and another phase ( + ) exists. Therefore, during fabrication, of more irregular ILs in U-Mo/Al-Si dispersions than U-
some parts of the meta-stable -U particle transform to -U. Mo/Al dispersions after in-pile tests. Hence, considerable
The -U has a lower swelling rate during irradiation than uncertainty is inevitably involved in the IL thickness of a
the -U (see [52]-[54]for details) and has a lower IL growth plate with Si addition.
rate [17]. When the -U is partially transformed to the -U Park et al. [39] annealed a U-Mo/Al-5Si dispersion
during fabrication and the subsequent blister test, a thicker sample at 580 ºC for ~1 h and observed an average IL
IL grows on the -U while a thinner IL grows on the -U, thickness of ~8 μm (see also Ref. [49]). Because the temper-
which results in nodular type IL growth on the same U-Mo ature was much higher, but still below the -phase boundary,
particle. In this situation, expressing IL in volume is more it is probable that the decomposition of the meta-stable -
appropriate than in thickness. phase U-Mo particles was higher in Park’s test, so his datum
may be exaggerated. However, the extent of IL growth
2.2 Al Matrix with Si Addition reported by Park is lower than those of U3Si/Al and U3Si2/Al
Measured data for U-Mo/Al-Si dispersion, i.e., U-Mo dispersion fuels [11], suggesting that at the annealing
dispersion in a Si-added Al matrix, are scarce from out- temperature the U-Mo fuel surface forms an excellent
of-pile tests and scatter with considerable uncertainties. barrier that effectively blocks Al diffusion into U-Mo. This
Iltis [23] measured the IL thicknesses of Si-added plates result also implies that the effect of the presence of the
fabricated at a lower fabrication temperature than typical Mo in U-Mo/Al-Si is to synergistically reduce IL growth
RERTR plates (Table 2) and then heated for two or four as in U-Si intermetallic dispersion in Al with a small
hours. As given in Table 2, 4 wt% Si and 6 wt% Si plates addition of Mo, as reported by Ugajin [55].
show no clear correlation between the Si content and IL Some diffusion-couple test data are available in the
thickness, implying that the effect of Si content on IL growth literature [17],[18]. In a typical diffusion-couple test to
in the out-of-pile heating test is negligible. Keiser and measure interdiffusion between U-Mo and Al, a U-Mo
co-workers [24] also reported an out-of-pile heating test block is welded with an Al block, and the metal couple,
result of plates with Si addition. Using images in Ref. [24], U-Mo versus Al, is isothermally heated. In the post-test
we measured IL thicknesses as given in Table 1. The Keiser analysis, the interaction layer thickness is measured. The
data also confirm that there is no clear correlation between contact pressure between U-Mo and Al in a diffusion-
the Si content and IL thickness. This uncertainty is chiefly couple test is higher than that of a dispersion sample, so
because of the irregular IL thickness, which is caused by the IL growth rate is generally higher in the diffusion-
the decomposition of the meta-stable -phase U-Mo particles. couple test than in the out-of-pile test of dispersion fuel.
It is typical that considerable parts of the U-Mo surfaces For this reason, the diffusion-couple test data cannot be
have extremely thin ILs while some parts have thicker used with the dispersion test data.
ILs, including some nodular type ILs. As discussed in Using the data provided in Table 1, we performed a
sect. 2.1, this nodular type of IL is known to form on the data fitting to the Arrhenius equation and the IL growth
parts of the U-Mo surface transformed to + ' during the correlation is obtained as follows (R2=0.67):
heating steps. Because of the much higher IL growth rate
of the phase [17], the fuel surface with -to- + ' phase (2)
transformation shows higher IL growth. Once formed,
the thick IL on the -U precludes Si diffusion to the fuel where YAl-Si is the IL thickness (μm) in an Al with a Si
addition, T in K and t in s.

Table 2. Heat Processes during Fabrication and Follow-on Blister Test and Predicted IL Growth before Irradiation for RERTR
Tests and KOMO-4 Test
Heating a Blister annealing Predicted
Test Matrix
temp (ºC) time (h) temp (ºC) time (h) average IL (μm)

RERTR-4, -5 Al 500 ~0.5 a 485 1 1.5


RERTR-6, -7 Al-Si 500 ~0.5 a
485 1 0.7
RERTR-9 Al-Si 500 ~0.5 a 485 0.5 0.6
KOMO-4 Al-Si 400 ~0.5 a b 0.0

a: The time is estimated after bonding between U-Mo and matrix is established [51].
b: No blister test was performed.

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KIM et al., Modeling of Interaction Layer Growth between U-Mo Particles and an Al Matrix

Using Eqs. (1) and (2), the IL growth during fabrication 3. MODEL FOR INTERACTION LAYER GROWTH
and the follow-on blister test for the RERTR test plates, DURING IRRADIATION
and KOMO-4 test were calculated and given in Table 2.
Once IL growth before irradiation is assessed by using 3.1 In-pile Test Data
Eq. (1) or Eq. (2), the total IL growth accumulating during
fabrication and irradiation can be obtained by The irradiation test data used in the model development
are summarized in Table 3. While the RERTR test samples
(3) are miniplates having the meat thickness of ~0.64 mm,
KOMO-4 test samples have rod-type geometry with the
where Y is the total IL thickness, Yfab is the fabrication IL meat diameter of 6.4 mm. Because of the much greater
thickness calculated by Eq. (1) or Eq. (2), and Yi is the IL distance of heat transport and the higher heat flux, the
thickness during irradiation. The model for IL thickness KOMO-4 test samples have much higher temperatures
prediction during irradiation is described in the following than the RERTR test samples for the same power.
section. For the RERTR test plates, the fuel temperatures were

Table 3. Test Data and Comparison of IL Thicknesses between the Measured and Predicted from RERTR-4, -5, -6, -7, -9 and
KOMO-4 Tests
FD Life As-
Nominal Average Life Measured Predicted
Enrich. at meat average fabricated
Fuel/matrix Meat U Time particle average IL IL Error b
Test Plate ID U-235 center FR IL
Composition a density EFPD size Temp thickness thickness μm
% (x1021) (1014) thickness
gU/cm3 μm ºC μm μm
f/cm3 f/cm3-s μm
RERTR-4 V6001M U-10Mo/Al 6 19.5 257 65 4.51 2.03 81 15 ± 1 1.5 11.6 3.4
Miniplate V6015G U-10Mo/Al 6 19.5 257 65 5.52 2.49 106 18 ± 2.5 1.5 17.4 0.6
V6022M U-10Mo/Al 6 19.5 257 65 5.27 2.37 106 19 ± 3.5 1.5 17.2 1.8
RERTR-5 V6018G U-10Mo/Al 6 19.5 116 65 2.30 2.29 80 9±1 1.5 8.0 1.0
Miniplate
V6019G U-10Mo/Al 6 19.5 116 65 2.92 2.91 98 15 ± 3.5 1.5 10.9 4.1
V8005B U-10Mo/Al 8 19.5 116 65 2.38 2.37 109 13 ± 1.5 1.5 12.1 0.9
RERTR-6 V0R010 U-10Mo/Al 6 19.5 135 65 2.90 2.48 101 7±2 1.5 11.8 -4.8
Miniplate
R5R020 U-7Mo/Al-0.2Si 6 19.1 135 65 3.12 2.67 105 11 ± 4 1.5 11.0 0.0
R1R010 U-7Mo/Al-1Si 6 19.5 135 65 2.73 2.34 87 2.7 ± 0.5 0.7 3.3 -0.6
R2R020 U-7Mo/Al-2Si 6 19.4 135 65 3.08 2.64 93 2.6 ± 0.5 0.7 2.5 0.1
R2R010 U-7Mo/Al-2Si 6 19.4 135 65 3.21 2.75 96 2.9 ± 0.5 0.7 2.7 0.2
R3R030 U-7Mo/Al-5Si 6 19.1 135 65 2.99 2.57 95 2.2 ± 0.5 0.7 2.5 -0.3
RERTR-7 R0R010 U-7Mo/Al 6 58.1 90 140 3.89 4.61 112 9±4 1.5 14.1 -5.1
Miniplate R0R020 U-7Mo/Al 6 58.1 90 135 5.55 6.57 135 16 ± 5 1.5 20.4 -4.0
R2R040 U-7Mo/Al-2Si 6 58.2 90 75 3.84 4.94 115 3.2 ± 1.5 0.7 3.7 -0.5
R2R050 U-7Mo/Al-2Si 6 58.2 90 90 3.98 5.12 134 10.2 ± 2.5 0.7 5.4 4.8
R3R040 U-7Mo/Al-5Si 6 58.3 90 80 4.43 5.70 117 2.7 ± 1.5 0.7 3.4 -0.7
R3R050 U-7Mo/Al-5Si 6 58.2 90 135 3.98 5.12 124 3.2 ± 2.5 0.7 3.7 -0.5

RERTR-9 R2R088 U-7Mo/Al-2Si 8.5 58.1 115 50 5.60 5.64 153 9.1 ± 3.5 0.6 9.4 -0.3
Miniplate R6R018 U-7Mo/Al-3.5Si 8.5 58.1 115 50 5.45 5.49 154 7.1 ± 3 0.6 7.0 0.1
KOMO-4 557MD3 U-7Mo/Al C 4.5 19.5 132 260 4.02 3.52 181 32 ± 3 0.0 34.0 -2.0
Rod
U-7Mo/Al MR 4.5 19.5 132 260 4.02 3.52 165 28 ± 3 0.0 29.1 -1.1
6762S1 U-7Mo/Al-2Si C 5 19.5 132 260 3.70 3.24 194 17 ± 2 0.0 23.7 -4.7
U-7Mo/Al-2Si MR 5 19.5 132 260 3.70 3.24 182 15 ± 2 0.0 17.9 -0.9
6765S1 U-7Mo/Al-5Si C 5 19.5 132 260 3.56 3.12 187 11 ± 1.5 0.0 10.6 0.4
U-7Mo/Al-5Si MR 5 19.5 132 260 3.56 3.12 171 8 ± 1.5 0.0 7.6 0.4
6768S2 U-7Mo/Al-8Si C 5 19.5 132 260 3.49 3.06 181 7±1 0.0 7.6 -0.6
U-7Mo/Al-8Si MR 5 19.5 132 260 3.49 3.06 167 6±1 0.0 6.5 -0.5

a: Numbers before Mo and Si mean the Mo content in fuel particles and the Si content in matrix in wt%, respectively.
b: error = measured – predicted
C: meat center
MR: meat mid-radius

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KIM et al., Modeling of Interaction Layer Growth between U-Mo Particles and an Al Matrix

calculated at BOL and EOL, and arithmetic averages of pores forming in the matrix, and fuel creep occurring
were taken to represent the test samples (Table 3). For in the fuel meat loaded closer to the ATR core center, a
the KOMO-4 test, the time-dependent fuel temperatures phenomenon reported previously [56],[57]. For the KOMO-
were calculated and life-average values were obtained. 4 test, measurements were made at the meat center and
The test-sample power, and hence the fission rate, decreases meat mid-radius regions, by which two IL thicknesses at
due to depletion of fissile atoms in the sample. On the different temperatures with the same fission rate were
other hand, fuel temperatures tend to increase as the meat obtained (Table 3).
thermal conductivity degrades due to IL growth and the The measurement errors, given in Table 3, stem largely
formation of fission gas pores. These two factors somewhat from the irregular IL thicknesses. The errors tend to be
compensate for each other, and as a result, the change in larger for the samples with a Si-added matrix than the
fuel temperature over test life is insignificant. In the RERTR
miniplate tests, although the temperature and fission rate
(i.e., power) are each independent variables to each other,
they are still coupled. In this regard, the KOMO-4 test
data are valuable because they have higher temperatures
than the RERTR test data while the fission rates are similar.
IL thicknesses were measured at several locations in an
optical micrograph and the average value was used as the
nominal value. The method to obtain the representative
IL thickness is illustrated in Fig. 2. Two cross sections
are shown for illustration. The cut surface A is off of the
equator B. Therefore, the IL thickness L1 measured in
the cut surface A is thicker than L2 measured in the equator.
Generally, on a metallographic picture, the common thinnest
IL is more likely to be the true IL thickness, because it is
more likely to be on a plane close to the equator of the fuel
particle.
In Fig. 3 and Fig. 4, posttest micrographs of RERTR-
6 and KOMO-4 samples are shown, respectively. The
RERTR-6 is a test having relatively low temperatures and Fig. 3. Post Irradiation Micrographs Showing Microstructures
low fission rates. Although temperatures vary by ~18 ºC, of RERTR-6 plates. The Burnup is in Percent Fission Per
all test plates consistently show that IL thickness decreases Initial Heavy Metal Atom (FIHMA).
as the Si content increases. This trend is more noticeable
in the KOMO-4 test, which has less temperature variability.
The ILs of the RERTR samples were measured at the
plate transverse (width) center to exclude possible influence

Fig. 2. Schematic Illustration of the Measurement Method of Fig. 4. Post Irradiation Micrographs Showing Microstructures
Interaction Layer Thickness. A and B are Cross Section of KOMO-4 Samples. The Burnup is in Percent Fission Per
Planes. Initial Heavy Metal Atom (FIHMA).

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KIM et al., Modeling of Interaction Layer Growth between U-Mo Particles and an Al Matrix

pure Al matrix samples. PIE images also showed locally depends on temperature. For the RERTR-6 test, the Si effect
thick, nodular type, ILs, the cause for which originated is virtually saturated at 2 wt% Si (Fig. 5). However, the
from the + ' transformation during fabrication and the KOMO-4 test shows that the IL reduction effect continues
following blister test. On the other extreme, PIE images up to 8 wt% Si without saturation. Fitting the IL reduction
showed that ILs on some U-Mo particles were still thinner versus the Si content for two different temperatures given
than the average IL thickness during fabrication. This in Fig. 5, we obtained the IL reduction factor by Si addition
indicates either that some parts of the fuel surface had in Al as
poor contact from fabrication to the end of irradiation, or
that large Si particles contacting the fuel particle effectively
(7)
blocked Al diffusion. The as-fabricated IL thickness was
subtracted from the post-irradiation IL, which means the
predicted results by the new correlations are for those where T is the fuel meat temperature in K (” 473 K) and
during irradiation. WSi is the Si content in the matrix in wt% (” 8 wt%). fsi is
in the range 0.002 ” fSi ” 1. The minimum occurs at the
3.2 Correlation Development for Irradiation Si content of 8 wt%, whereas the maximum occurs for
3.2.1 Basic Correlation the pure Al.
The IL growth correlation during irradiation is a modified 3.2.3 Factor for Mo Content Effect, fMo
Arrhenius equation from Eq. (1), and an additional term
with the fission rate is multiplied to account for fission- It is known that as the Mo content increases, the IL
enhanced-diffusion (FED): growth rate decreases [2],[54],[14], so cases with a Mo
content other than 7 wt% need to be considered. The current
(4) understanding is that the metastable -phase U-Mo more
readily decomposes to the + ' if the Mo content in the
where fÚ is the fission rate, and A and q are empirical con- alloy is reduced. Although the -phase transforms back to
stants. The power, p, to the fission rate was empirically the -phase soon after irradiation starts [59],[60],[61],
determined as p=0.5 [11],[44]. once formed, the -phase produces a thicker IL during
There have been several other correlations that take a fabrication and the subsequent blister test. The thicker IL
similar form to Eq. (4) but with different constants [44], formed on the a phase weakens the Si addition effect, and
[45],[48],[58]. In order to fit both the RERTR and KOMO the result is an increase in the overall IL growth rate during
data, the fitting constants here were revised from those of irradiation. In the thick IL, as the Si concentration decreases,
Refs. [44] and [45]. The best fit was obtained with A= so does its activity [43]. Mirandou [19] also found a weak-
2.6x10-8 and q=3850 K for plates with U-7Mo in a pure ened Si effect in the thick IL from an elevated-temperature
Al matrix. In Table 3, the predicted and measured IL out-of-pile test and argued that it was owing to the formation
thicknesses are compared. Therefore, the correlation for
the samples with a pure Al matrix is:

(5)

where Y is in μm, fÚ in f/cm3-s, T in K, and t in s.


The effects of Si addition and Mo content are considered
by multiplying additional factors to Eq. (5) as follows:

(6)

where fSi is the reduction factor by Si addition in the Al


matrix and fMo is the factor to assess the Mo content other
than 7 wt% in the U-Mo alloy particles. The modeling of
these factors is described in the following subsections.

3.2.2 Factor for Si-addition Effect, fSi


The addition of Si in the Al matrix results in an expo- Fig. 5. Comparison of IL Reduction Factors Obtained for the
nential reduction of IL thickness that varies with the Si Low-temperature RERTR-6 Test (at Life-avErage T ~100 ºC)
and the High-temperature KOMO-4 Test (at Life-average T
content. Comparing the results from the lower temperature ~180 ºC), where the IL Reduction Factor is Defined as the
test RERTR-6 and the higher temperature test KOMO-4, Square of IL Thickness Divided by the Square of IL Thickness
it is noticeable that the Si addition effect on IL growth also for a Pure Al Matrix at the Same Irradiation Condition.

NUCLEAR ENGINEERING AND TECHNOLOGY, VOL.45 NO.7 DECEMBER 2013 833


KIM et al., Modeling of Interaction Layer Growth between U-Mo Particles and an Al Matrix

of the -phase, on which U4Mo6Al43+UAl3 phases form, adding Si to the matrix. One is adding Si to the Al as an
excluding Si. alloying element, and the other is directly adding the Si
In the RERTR experiment modeling [2], we observed powder to the Al powder during fuel fabrication. The
that the IL growth rate decreased linearly with the Mo former was considered the better method to provide finer
content in the range of 6 – 10 wt%. This effect was similarly Si particles in the matrix.
formulated as follows: In order to have more accurate modeling, consideration
of the parameters discussed above (U-loading, homogeneity
(8) in fuel-particle spatial distribution and Si precipitate size in
the matrix) may also be necessary. In the present modeling,
where WMo is the Mo content in fuel particles in wt%. fMo however, these parameters are not explicitly considered.
varies between 0.85 (at 10 wt% Mo) and 1.05 (6 wt% Mo). The Si concentration in the IL tends to decrease during
A Mo-content beyond 10 wt% is not considered in the irradiation. As the Si concentration decreases, the Si’s
US RERTR program. strength to reduce the IL growth rate also decreases. How-
ever, the change in the Si effect during irradiation is not
included in the present model.
4. DISCUSSION The comparison between the measured data and pre-
dicted IL thicknesses are given in Table 3. Considering
uncertainties in temperatures and measurement errors, a
One of the objectives of the development of the present
fair agreement was generally achieved, except for some cases.
model was to unify the two independent IL growth correla-
The uncertainty in the meat temperatures is believed to be
tions applicable either to a pure Al matrix, or to an Al
caused by the uncertainty in the meat thermal conductivity
matrix with up to 8wt% Si and temperatures up to 200 ºC.
at high burnup. Measurement errors were primarily due to
In addition, IL formation before irradiation is included,
the irregular IL thickness.
so the model can be used for fuels produced by various
fabrication methods.
The observations from the KOMO-4 test [39] showed
that Si tends to accumulate mostly at the IL-matrix interface 5. CONVERSION OF IL THICKNESS TO IL VOLUME
due to Si diffusion from the matrix. It is known that Si
contained only in the fission-fragment recoil zone produces IL growth data given in thickness are often more
Si diffusion flux. As the IL grows, the overlapping volume convenient than those given in IL volume, because they
fraction of the recoil zones increases and, hence, there is a do not need supplemental data such as U-loading and U-
decrease in the effective amount of Si per unit-fuel-surface Mo particle size. However, for high IL growth cases, the
area available for diffusion. thickness is not only difficult to measure, but it is also less
For the RERTR-9 test, the fuel plates were made with meaningful. For these circumstances, data on IL volume
smaller fuel particles and higher U-loading, which yielded fraction is a better metric. Consequently, a conversion
more recoil-zone overlapping during the test, and in turn model from IL thickness to IL volume was developed,
reduced the effective Si amount available per unit-fuel- assuming that fuel particles had a uniform size and were
surface area. Contrarily, the KOMO-4 test samples had distributed in an FCC array.
larger fuel particles sizes and relatively lower U-loading Fig. 6 illustrates the configuration of two neighboring
in the meat (see Table 3). As a result, smaller recoil-zone fuel particles and the IL formed around them. The distance,
overlapping was made, so the effective Si amount per
unit-fuel-surface area was higher. As U-loading increases,
not only the matrix volume decreases and the depletion of
the matrix occurs earlier, but homogeneity in fuel particle
spatial distribution also tends to decrease. Regions with
higher U-Mo particle densities occur, where the effective
Si amount per unit-fuel-surface area decreases. Hence,
even for the same Si content in the matrix, the IL growth
rate can be different.
In the meat, the homogeneity of fuel-particle spatial
distribution may also affect the effective Si availability.
For example, a higher homogeneity in fuel-particle spatial
distribution improves the effect of Si addition.
An additional consideration in the efficacy of Si is how
Si is added to the matrix Al. The finer the Si precipitates,
the more effective is the Si addition: Hence, a lower IL Fig. 6. Schematic Showing Configuration of Two Neighboring
growth rate. At present, there are two viable methods of Particles with IL Formed on the Surfaces and IL Overlapping.

834 NUCLEAR ENGINEERING AND TECHNOLOGY, VOL.45 NO.7 DECEMBER 2013


KIM et al., Modeling of Interaction Layer Growth between U-Mo Particles and an Al Matrix

d, between the surfaces of two neighboring particles is

(9)

where a is the FCC unit cell edge length, and r is the fuel
particle radius. The fuel volume fraction in the meat is
defined as

(10)

where Vm is the meat volume and Vf is the fuel volume in


the unit cell, respectively. Because there are four fuel
particles in the unit cell, Vf is given by

(11)
Fig. 7. Prediction of IL Volume Fraction as a Function of IL
Thickness for 6 gU/cm3 and 8 gU/cm3 U-density in the Meat
where r is the average fuel particle radius known from (Average Fuel Particle size = 70 μm) and for 5 gU/cm3 U-
the fabrication data. From Eqs. (9) – (11), d can be found Density in the Meat (Average Fuel Particle Size = 150 μm).
by

(12) (16)

where the applicable range of vf is less than 0.74, which is where VILis given by Eq. (15) and Vf given in Eq. (11).
the FCC packing fraction. The fuel volume fraction vf is Fig. 7 shows the model predictions for IL volume
usually calculated with known fabrication data (U-loading), fraction versus IL thickness for 6 gU/cm3 and 8 gU/cm3
because vf =wU/ U where wU is U-loading, and U is U- U-loading cases with a fuel particle size of 70 μm. Also
density in the fuel particle. For example, vf for 8 gU/cm3 included is a case for the KOMO-4 test, for which fuel
of U-7Mo is calculated by vf= wU/ U = 8/16.3=0.49 where loading is 5 gU/cm3 with fuel particle size of 150 μm. Fuel
U = 17.5 * (1 – 0.07). The physical density of U-7Mo swelling and fuel consumption by the interdiffusion layer
alloy is 17.5 g/cm3. growth are not considered. However, these two factors
In Fig. 6, the overlapping part of the IL volume of the somewhat tend to compensate for each other to give
right-hand-side fuel particle, by the neighbor particle, is a reasonably acceptable model predictions. A more detailed
partial sphere with height, h, of which the volume is model is necessary for an accurate result, but the model
described here is suitable for approximate estimates.
(13)

where h = Y – d/2 and R= r + Y. Here Y is the IL thickness. 6. CONCLUSIONS


When the IL overlaps with neighboring fuel particles, i.e.,
Y is greater than d, as marked by the darker gray region in
In the US GTRI-convert program (formerly known as
Fig. 6, and this volume must be subtracted from the large
RERTR), U-Mo alloy particle dispersion in Al is a primary
cap volume given in Eq. (13). Because there are two symmetric
fuel form being studied for use in converting HEU-fueled
caps, two of these small caps must be considered.
research and test reactors to LEU-fueled ones. In order to
achieve sufficient total uranium densities, high fuel-volume
(14)
loading is pursued. One of the largest obstacles to good
fuel performance is interaction layer (IL) growth between
where g = (Y– d)/2.
the U-Mo particles and matrix Al, which needs to be
The IL volume can be calculated considering only one minimized.
fuel particle surrounded by 12 neighboring ones by For an accurate fuel performance analysis, a prediction
model for IL growth is therefore necessary. Two empirical
(15) IL growth correlations were developed for out-of-pile
fabrication and possible subsequent testing: One is for
the pure Al matrix, and the other for the matrix with Si
The IL volume fraction vIL in the fuel meat can be addition. The IL growth correlations are Arrhenius
calculated by equations.

NUCLEAR ENGINEERING AND TECHNOLOGY, VOL.45 NO.7 DECEMBER 2013 835


KIM et al., Modeling of Interaction Layer Growth between U-Mo Particles and an Al Matrix

The in-pile growth correlation, developed using the and Test Reactors (RERTR), Las Vegas, Nevada, USA,
RERTR-4, -5, -6, -7 and -9 data, as well as KOMO-4 data, October 1-6, 2000. <http://www.rertr.anl.gov>
takes a form similar to the out-of-pile correlations. For the [ 5 ] G. L. Hofman, Yeon Soo Kim, M.R. Finlay, J.L. Snelgrove,
in-pile correlation, the out-of-pile IL growth was augmented S.L. Hayes, M.K. Meyer, C.R. Clark, “Recent Observations
at the Postirradiation Examination of Low-Enriched U-Mo
by fission-enhanced diffusion (FED). The FED effect was
Miniplates Irradiated to High Burnup,” Proc. Int. Meeting
modeled by the square-root of the fuel-particle fission rate. on Reduced Enrichment for Research and Test Reactors
The in-pile correlation was further enhanced to include (RERTR), Chicago, Illinois, October 5-10, 2003.
the effect of Si addition in the Al and the effect of the Mo <http://www.rertr.anl.gov>
content. The model is applicable for Si contents in the [ 6 ] P. Lemoine, J. L. Snelgrove, N. Arkangelsky and L. Alvarez,
matrix up to 8 wt%, for fuel temperatures up to 200 ºC, and “UMo dispersion fuel results and status of qualification
for Mo content in fuel particles in the range of 6 – 10 wt%. programs,” Trans. RRFM 2004, Munich, Germany, March
An approximate analytical method to convert IL thick- 21-24, 2004.
ness to IL volume fraction in the fuel meat was proposed. http://www.euronuclear.org0meetings/rrfm2004/index.htm
For a more accurate conversion, the volume changes in fuel [ 7 ] H.J. Ryu, Yeon Soo Kim, G.L. Hofman, “Amorphization of
and matrix caused by their consumption by IL growth the interaction products in U-Mo/Al dispersion fuel during
irradiation,” J. Nucl. Mater., vol. 385, pp. 623-628 (2009).
must be considered together with the volume expansion
[ 8 ] S. Van den Berghe, W. Van Renterghem, A. Leenaers,
by fission-product-induced fuel swelling, which was not “Transmission electron microscopy investigation of irradiated
considered in the present work. U-7 wt%Mo dispersion fuel,” J. Nucl. Mater. vol. 375, pp.
340-346 (2008).
ACKNOWLEDGMENTS [ 9 ] Yeon Soo Kim and G.L. Hofman, “Irradiation behavior of
This paper contains information obtained from the the interaction product of U-Mo fuel particle dispersion in
reduced-size plate tests ~RERTR-6, -7, and -9 irradiated an Al matrix,” J. Nucl. Mater., vol. 425, pp. 181-187 (2012).
in the ATR, in the Global Threat Reduction Initiative- [ 10 ] G.L. Hofman, J. Rest, J.L. Snelgrove, T. Wiencek, S.K.V.
Conversion program ~formerly known as the RERTR Groos, “Aluminum-U3Si2 Interdiffusion and Its Implications
for the Performance of Fuel Operating at Higher Temper-
program. For design and fabrication of the test samples,
atures and Fission Rates,” Proc. Int. Meeting on Reduced
Mrs. T. Wiencek, C. Clark, and G. Moore are acknowledged. Enrichment for Research and Test Reactor (RERTR), Seoul,
The physics data were made available by Dr. G. Chang Korea, 1996. <http://www.rertr.anl.gov>.
and Ms. M. Lillo at INL. The operation staff at ATR is [ 11 ] Yeon Soo Kim and G.L. Hofman, “Interdiffusion in U3Si-Al,
also acknowledged for the RERTR irradiation tests. The U3Si2-Al, and USi-Al dispersion fuels during irradiation,” J.
authors appreciate the hands-on PIEs performed at the Nucl. Mater., vol. 410, p. 1-9 (2011).
Materials and Fuels Complex of INL. The authors also [ 12 ] G. L. Hofman, M. R. Finlay and Yeon Soo Kim, “Post-
thank Dr. J. S. Cheon of KAERI for providing the drawing Irradiation Analysis of Low Enriched U-Mo/Al Dispersion
shown in Fig. 2. This work was supported by the U.S. Fuel Miniplate Tests, RERTR 4 and 5,” Proc. Int. Meeting
Department of Energy, Office of Global Threat Reduction on Reduced Enrichment for Research and Test Reactors
(NA-21), National Nuclear Security Administration, under (RERTR), Vienna, Austria, November 7-12, 2004.
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Contract No. DE -AC-02-06CH11357 between UChicago
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