Journal of Nuclear Materials 442 (2013) 133–142

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Journal of Nuclear Materials

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Mechanical characteristics of SiC coating layer in TRISO fuel particles

P. Hosemann a,⇑, J.N. Martos a, D. Frazer a, G. Vasudevamurthy b, T.S. Byun c, J.D. Hunn c, B.C. Jolly c,
K. Terrani c, M. Okuniewski d
a
University of California Berkeley, Nuclear Engineering, CA, USA
b
Virginia Commonwealth University, Mechanical and Nuclear Engineering, VA, USA
c
Oak Ridge National Laboratory, TN, USA
d
Idaho National Laboratory, ID, USA

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

Article history: Tristructural isotropic (TRISO) particles are considered as advanced fuel forms for a variety of fission plat-
Received 29 May 2013 forms. While these fuel structures have been tested and deployed in reactors, the mechanical properties
Accepted 23 August 2013 of these structures as a function of production parameters need to be investigated in order to ensure their
Available online 30 August 2013
reliability during service. Nanoindentation techniques, indentation crack testing, and half sphere crush
testing were utilized in order to evaluate the integrity of the SiC coating layer that is meant to prevent
fission product release in the coated particle fuel form. The results are complimented by scanning elec-
tron microscopy (SEM) of the grain structure that is subject to change as a function of processing param-
eters and can alter the mechanical properties such as hardness, elastic modulus, fracture toughness and
fracture strength. Through utilization of these advanced techniques, subtle differences in mechanical
properties that can be important for in-pile fuel performance can be distinguished and optimized in iter-
ation with processing science of coated fuel particle production.
Ó 2013 Elsevier B.V. All rights reserved.

1. Introduction pressure vessel to withstand internal gas pressure buildup. Finally,

TRISO fuel particles have long served as the fuel form of choice
in high temperature gas reactors (HTGRs) [1–7] and their use is
now considered to be extended into fluoride salt high temperature
reactors (FHRs) [3–6] and light water reactors (LWRs) [2]. For
HTGR applications, a large number of these TRISO fuel particles
are combined in a graphite matrix of either spheres for pebble
bed fuel or cylindrical compacts for prismatic fuels [8]. These fuel
forms have been successfully deployed in Germany in the 1960’s
[9] and are now being produced and evaluated in the US national
laboratory system [4] as well as in China and other countries.
The typical TRISO particle has five layers. In the center is the
fuel kernel, which is often uranium oxide (UO2) but can be an
oxide, carbide, or oxide/carbide mix with uranium, plutonium, tho-
rium or transuranic elements as the fuel [10]. The fuel is sur-
rounded by a low-density pyrolytic carbon buffer layer that
serves as a porous medium in order to absorb fission products
and accommodate kernel swelling. Next, there is a high-density in-
ner pyrolytic carbon (IPyC) that is impermeable to gaseous fission
products, and serves as the substrate for SiC deposition. Surround-
ing the IPyC layer, is a high density and high strength silicon car-
bide (SiC) layer providing a diffusion barrier to prevent the
release of gaseous and metallic fission products, and acts as
⇑ Corresponding author. Address: 4169 Etcheverry hall, 94720 Berkeley, CA, USA.
E-mail address: peterh@berkeley.edu (P. Hosemann).
the outermost layer consists of a high-density pyrolytic carbon
(OPyC) layer that serves to protect the SiC layer during handling
and compaction. Both IPyC and OPyC shrink during early stages
of irradiation to induce compressive stress on the ceramic pressure
vessel [9].
The silicon carbide layer of the TRISO particle is considered to
be the most important structure since it prevents fission product
release and therefore is an essential safety feature. Maintaining
the integrity of the SiC layer throughout the operating lifetime is
essential to retaining fission products within the fuel particle and
prevents contamination of the reactor and potentially the outside
atmosphere. The exact conditions of TRISO fuel manufacturing var-
ies and depends on the actual use. The TRISO fuels examined in this
project had a ZrO2 kernel directly coated with a PyC layer and an
outer SiC layer. The non-radioactive surrogate kernel was chosen
for this study in order to make the material easier to handle in a
non-radiological facility. For the purpose of characterizing the SiC
this should not have a significant effect on the properties.
A typical TRISO particle is a multilayered, <1-mm-diameter
structure making localized investigation a challenge. The spherical
shape of TRISO particles and the small diameter of the SiC layer,
usually 30–50 lm, makes determining mechanical properties
using traditional methods difficult.
Silicon carbide is a material of general interest due to its supe-
rior irradiation tolerance [3]. It is often used for high temperature
environmental applications because of its high thermal

0022-3115/$ - see front matter Ó 2013 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.jnucmat.2013.08.041
134 P. Hosemann et al. / Journal of Nuclear Materials 442 (2013) 133–142

conductivity, low thermal expansion, good thermal shock resis- 2. Experimental

tance, and good chemical inertness [3]. Important to nuclear appli-
cations, SiC has a high resistance to radiation damage due to its
small-neutron capture cross section [3]. For these reasons, SiC is of-
ten considered as a candidate for advanced nuclear reactor materi-
als even as a composite [11–13]. As described above, the TRISO
particle uses a SiC coating as the main structural layer of the fuel
particle and its properties have therefore been subject to research
over the past decade.
The mechanical properties of the SiC layer of TRISO particles
have been explored with different techniques including the ring
test method [14,15], the crush test [16–19], the micro-cantilever
test [20,21], and indentation methods [22,23]. Fracture toughness
properties have also been explored previously [24]. In this work,
effects of the manufacturing variable on Young’s modulus, hard-
ness, and fracture toughness is presented utilizing a suite of small
scale testing techniques including nanoindentation, microcantile-
ver testing, shear crush testing, and indentation fracture. Indention
techniques allow mapping the properties as a function of location
across the different layers and have been found useful on nuclear
materials in the past [25–27].
The TRISO fuel particles are manufactured using fluidized-bed
chemical vapor deposition (FB-CVD), an efficient method to coat
particles using reactant gas. Particles are typically suspended in a
deposition zone by flowing a gas upwards through a particle bed.
Pyrolytic carbon is deposited from acetylene, or a mixture of acet-
ylene/propylene, at a deposition temperature ranging from 1250 to
1450 °C, and at a concentration of acetylene/propylene of 20–40%
[28]. The ZrO2 (surrogate) or heavy metal fuel kernel is manufac-
tured using a gel precipitation process where the final step is sin-
tering in a H2 atmosphere [28]. Silicon carbide is deposited by the
decomposition of methyltrichlorosilane (MTS) in a hydrogen envi-
ronment at temperature between 1300 and 1600 °C [29]. MTS is
used for depositing silicon carbide on isotropic graphite and its
equivalent ratio of Si to C makes it easy to deposit stoichiometric
films [29]. Hydrogen is usually used as a carrier gas to transports
the MTS from the bubbler to the reactor, and also functions as a
dilution gas [30]. The ideal deposition temperature for
stoichiometric cubic SiC (b-SiC) has been found to be in the range
of 1450–1550 °C, which results in the highest strength and Young’s
modulus of SiC [31]. Grain size is primarily a function of the
deposition temperature. Higher deposition temperature results in
a larger grain size. It is important to note that using FB-CVD
technique, the grain size is not constant but instead grows
considerably with thickness [32–34]. The focus of this paper is
on demonstrating the application of these new mechanical testing
methods to TRISO fuel particles; however, some evaluation of the
different processing parameters and their effects on the
mechanical properties is included.
In this study two ZrO2 kernel sizes, with diameters of 520 lm
and 670 lm, were coated using typical AGR IPyC coating condi-
tions in the 150-mm-diameter coater at Babcock and Wilcox Nu-
clear Operations Group (B&W-NOG) [18]. These particles were
sent to Oak Ridge National Laboratory (ORNL) and SiC was chemi-
cal vapor deposited in a 50-mm-diameter coater using MTS.
Hydrogen was used as the fluidization medium and mixed with
the MTS. The processing parameters, such as SiC deposition dura-
tion, coating temperature and MTS flow rate were varied as shown
in Table 1. A roller micrometer was used to separate the two differ-
ent kernel sizes after each batch was coated. Within each batch,
particles with small kernels were separated into subsample A
and particles with large kernels were separated into subsample
C. Each subsample was then separated again by size distribution
into smaller groups and the group at the peak of the Gaussian dis-
tribution in the particle size (A2 and C2) was used for material
characterization [18]. The mean and standard deviation of each
layer’s thickness was determined using optical imaging [35]. The
larger diameter kernels (C2 batches) typically had a slightly thin-
ner IPyC layer, because coating rate is inversely related with the
particle size due to the geometrical effect on surface flux [18].
2.1. Sample preparation for nanoindentation
For each of the ten different samples, 24 individual TRISO parti-
cles were mounted in a two-part cold mount epoxy. Double sided
tape was centered and fixated to the bottom of a mounting cup and
individual TRISO particles were placed in a 5  5 matrix. One posi-
tion on the outside of the matrix was left open to allow for index-
ing. The array of particles were closely spaced and centered in the
1.25’’ diameter mount as shown in Fig. 1a. Arranging the particles
in a tightly packed matrix helped keep the cross sections flat with
sharp edges at the interfaces and also helped keep an even planar
surface for all particles.
The mounted particles were then polished to near mid-plane.
By observing the mounted particles in an optical microscope, one
can see that a shadow around the edge of the SiC layer decreases
in thickness as the mid-plane is approached. Additionally, since
the average TRISO particle diameter is known, measuring the ini-
tial thickness and then periodically measuring the amount re-
moved using a high precision micrometer, can give a good
estimate as to when a near mid-plane polish is approached. Polish-
ing very close to or past mid-plane of the TRISO particles would
cause the ZrO2 kernel to separate and fall out from the rest of
the particle, so this was avoided.
The embedded TRISO particles were manually polished in suc-
cession using Buehler SiC abrasive paper starting at coarse P600

Table 1
Samples provided by ORNL for this study. All relevant processing parameters and specimen geometries are listed.

Sample Kernel diameter (lm) PyC thickness (lm) SiC thickness (lm) SiC deposition time SiC deposition temperature MTS flow
Mean St. Dev. Mean St. Dev. Mean St. Dev. (min) (°C) (cc/min)
AGRB-2T-A2 529 9 46 3 37 1 122.0 1500.0 179.0
AGRB-2T-C2 717 9 43 3 34 1 122.0 1500.0 179.0
AGRB-1W-A2 540 10 46 3 35 1 131.0 1450.0 157.0
AGRB-1W-C2 718 9 43 3 31 1 131.0 1450.0 157.0
AGRB-1V-A2 528 9 46 3 27 1 131.0 1450.0 138.0
AGRB-1V-C2 719 8 43 2 24 1 131.0 1450.0 138.0
AGRB-3R-A2 540 9 46 3 35 1 127.0 1550.0 148.0
AGRB-3R-C2 712 10 44 3 29 1 127.0 1550.0 148.0
AGRB-3S-A2 529 11 46 3 41 1 129.0 1550.0 174.0
AGRB-3S-C2 711 9 44 3 32 1 129.0 1550.0 174.0
 P. Hosemann et al. / Journal of Nuclear Materials 442 (2013) 133–142
Fig. 1. SiC Triso spheres mounted in epoxy and polished (a). Optical micrograph of the spear not polished to the sphere centerline (b). Example hardness map obtained using
cross section nanoindentation on a sample (c).
grit down to P4000 grit. Buehler diamond paste of 3 lm, 1 lm, and
4 lm in diameter on hard polishing clothes were used. Extreme
1=
care had to be taken when polishing the TRISO particles due to
the very different material properties between the layers, as well
as the mounting epoxy. Low force and fine grinding steps were
necessary in order to have intact TRISO particles. If high speeds
or high forces were used, fracture of one of the coatings could oc-
cur, which would then destroy the rest of the particles in the sam-
ple mount as coating pieces fracture off during grinding. As a last
step, the sample mounts were polished with 0.05 lm colloidal sil-
ica on a Buehler VibroMet polisher. In between each polishing step,
the sample was thoroughly cleaned with an ultrasonic cleaner with
ethanol as a cleaning medium. It was found that as the mid-plane
of the TRISO particles was approached; using the ultrasonic cleaner
would quickly separate the ZrO2 kernel from the particle. Therefore
not polishing all the way to the mid-plane was more desirable to
avoid the removal of the kernel. Having the kernel separate from
the TRISO structure can lead to easy fracture of the remaining shell
due to handling and can make the indention experiment difficult
since a deep gap will remain next to the edge.
2.2. Sample preparation for crush testing
A modified crush testing and evaluation method for hemispher-
ical shell specimens was applied to obtain the fracture stress data
for selected samples. For each sample, 24–47 hemispherical shell
specimens were selected and tested. Approximately 200 particles
were bonded to an 1.2500 diameter aluminum cylinder using
Crystalbond-509 mounting adhesive. This adhesive melts at
121 °C to allow particles to be mounted in a single layer and sets
upon cooling to a hard form suitable for grinding. Enough epoxy
was applied to cover the particles, which provided suitable edge
support during grinding. The grinding procedure was similar to
that described above for preparation of cross sections for optical
(a) (b)
Fig. 2. Optical microscopy image of a indent set into the SiC shell. The cracks used for fracture analysis are clearly visible (a). SPM scan over a cracked shell for fracture
toughness measurements (Z-scale = 8 lm a) (b). SPM image of another indent the crack originating from the indent corners is clearly visible going through the grains and not
going in the radial direction visible (z-scale 48 lm) (c).
135
imaging and indentation. Care had to be taken to avoid kernel rota-
tion during grinding, which could result in broken layers. Grinding
was stopped close to, but before passing through, the particle mid-
plane. Attempting to grind past the midplane was more likely to
result in broken coatings due to kernels becoming loose and even
falling out of the mounts. Acetone was used to dissolve the Crystal-
bond-509 and recover the ground hemispheres. Samples were then
placed in a muffle furnace and heated for 3 h at 750 °C. This was
sufficient to remove the IPyC layer, leaving the ZrO2 kernel hemi-
spheres free to fall out of the SiC hemispherical shells. Fig. 3 shows
a scanning electron image of a typical SiC hemispherical shell. A
similar approach as described above was used to manufacture C-
Rings as evaluated in the discussion section.
2.3. SEM investigation
SiC layer thickness and grain size were investigated utilizing
SEM. The resulting images can be found in the results section. A
Quanta 3D field emission gun (FEG) scanning electron microscope
with focused ion beam (SEM/FIB) at UC Berkeley was used to ob-
tain the images. FIB surface milling provided a clean surface for
better imaging of the grains in the SiC.
2.4. Nanoindentation and indentation fracture toughness
measurements
Nanoindentation measurements were performed at the Center
for Advanced Energy Studies (CAES) in Idaho Falls, ID and the
Materials Laboratory at the University of California, Berkeley. The
nanoindentation measurements at CAES were conducted on the
Hysitron Triboindenter, where the nanoindenter tip was mounted
on a transducer allowing lateral scanning of the sample, as well as
precise motion using the piezoelectric and capacitor actuators. The
nanoindentation measurements at UC Berkeley were conducted on
(c)
136 P. Hosemann et al. / Journal of Nuclear Materials 442 (2013) 133–142
SiC
specimen
(a)
Fig. 3. SEM image of a SiC hemispherical shell (AGRBW-1W) prepared for crush testing (a). Schematic sketch of the crush test as developed by ORNL (b).
the Micro Materials NanoTest™. The NanoTest is a horizontal tip-
sample arrangement in contrast to the vertical arrangement of
the Hysitron device [36]. This system allows higher loads of up
to 500 mN without changing the transducer. In addition the Micro
Materials system is capable of heating the sample and tip up to
750 °C and performing high temperature tests. However, the effect
of temperature was not part of this study. The reason for utilizing
two different indenters was machine availability. Both systems
were always calibrated against fused silica before each indentation
run in order to allow cross comparison between samples and ind-
enters. The indents were typically 200 nm deep and 4 lm apart
from each other. A cross comparison on selected TRISO particles
was conducted ensuring that the same data was measured using
both systems. The indentation size effect was not part of this study
therefore the values measured should be compared to indents of
similar depth.
A nanoindenter was also used to measure the fracture tough-
ness of a given material. For these measurements, a Berkovich dia-
mond indenter tip was used to perform fracture toughness
measurements. Fracture toughness was calculated based on the
crack length starting from the corners of the imprint using the
widely known the following equation:
 12
E P
Kc ¼ a ð1Þ
H c3=2
where Kc is the fracture toughness of the material, P is the maxi-
mum load, c is the crack length measured as shown in Fig. 2, E is
the elastic modulus, H is the hardness, and A is an empirical con-
stant corresponding to the indenter shape, a = 0.016 for a Berkovich
tip [37]. In the literature extensive discussions on indention fracture
toughness methods are published [51,52] including a comprehen-
sive review of the technique and the calculations utilized today.
In our work we utilize Eq. (1) since it is the equation given in the
textbook on nanoindentation [53] and is rather simple to use. In
addition this equation does not utilize the distance from the inden-
tation center to the edge of the imprint but rather uses the distance
from the crack tip to the center of the indent. While being an older
approach it does have the advantage that a sometimes difficult to
determine edge of the imprint is not needed and the question of
where exactly the imprint starts becomes irrelevant. It has to be
pointed out to the reader, not familiar with indentation fracture
toughness, that several different approaches exists as outlined in
[52] where most equations are based on empirical data generation.
Loading
Plunger
Insert material
(Soft metal)
Testing Bed
(b)
This implies that the values obtained here might not be directly
comparable to are not bulk values but are in reasonable good agree-
ment with what is found elsewhere and discussed in the later sec-
tion of this paper.
The radial cracks, initiated by indenting, were measured with
the in situ scanning probe microscopy (SPM) imaging capability
of the Hysitron TriboIndenter as well as an optical microscope.
The SPM allowed for immediate post-test observation of the indent
produced on the sample and eliminated the need to locate the in-
dent with its associated cracks with a different instrument such as
an SEM.
3. Crush test measurements
In a study performed in 2008 by ORNL [19], a modified crush
testing technique for hemispherical shell SiC specimens was devel-
oped. As described by the ORNL study [19], the modified crush test
used a soft metal (either copper or brass) at the specimen–plunger
contact to generate a uniformly stressed area at the inner surface of
the shell specimens. A schematic testing diagram shown in Fig. 3
shows the hemispherical shell specimen diametrically loaded be-
tween a bottom base and a loading plunger with a blanket metal
inserted in between. The hemispherical shell specimens were
tested in a 40 kN capacity Tinius-Olsen static testing machine
using the plunger-jig assembly. While the detailed theoretical
approach of how the measured load is related to fracture stress
is given in [19], a summary is also given here.
The maximum membrane stress and bending stress in a partial
spherical thin shell loaded by a load, F is calculated using
pffiffiffiffiffiffiffiffiffiffiffiffiffiffi
F 1  t2
rmembrane ¼ C 1 ð2Þ
t2
Fð1 þ tÞ
rbending ¼ C 2 ð3Þ
t2
where m is the Poisson’s ratio, t is the thickness of the shell, and
coefficients, R is the outer radius of the shell, C1 and C2, are obtained
using below,
C 1 ¼ 0:2205  0:04l  0:0115l2 ð4Þ
C 2 ¼ 1:2044 expð1:2703lÞ ð5Þ
With
 P. Hosemann et al. / Journal of Nuclear Materials 442 (2013) 133–142 137

1=4
l ¼ r0 ½12ð1  t2 Þ=ðR2 t2 Þ ð6Þ 4. Results

The maximum tensile stress is given in Eq. (26), which occurs at the Images of the SEM analysis are displayed in Figs. 4–8. A low
inner surface of the shell [19]. magnification and a higher magnification image are presented for
each specimen investigated. The images obtained were used to
rmax ¼ rmembrane þ rbending ð7Þ characterize the grain structure on each sample. Some samples
show a more uniform grain structure while others show a radially
Since the ratio between mean fracture strengths of two specimens oriented grain texture. Using the intercept method in ImageJ soft-
having different sizes can be correlated with the ratio of the effec- ware on the SEM images, the grain sizes were quantified for the
tive surface area [38,39], the mean fracture stress for a full-size TRISO variants at three different locations across the SiC layer in
spherical particle can be determined using Eq. (7) [31]. two directions and the average of each location was calculated
!1=m !1=m with the appropriate error as listed in Table 2 – at the IPyC/SiC
SLE pr20 interface, the middle of the SiC layer, and at the outer edge of
rFf ¼ rLf ¼ rLf ð8Þ
SFE 4pðR  tÞ2 the SiC layer. A summary of these results is shown in Table 2 be-
low. All the TRISO variants have very similar small grain structure
where rLf and rFf are the fracture stresses for partially loaded and at the IPyC/SiC interface. Progressing towards the outside of the SiC
full spherical shell specimens, SLE and SFE are the effective surfaces, layer, the grain size was found to increase in all the samples, and
m the Weibull modulus, and r0 is the radius of effective area which the grains were radial oriented starting at the IPyC/SiC interface.
is given by the measured radius of indentation impression. The At a deposition temperature of 1450 °C there was a finer grain
modified crush test technique was performed multiple times on structure throughout the layer. With the increase of the deposition
each variant to determine statistical results. temperature to 1500 °C and 1550 °C, there was a more pronounced

Fig. 4. SEM image of SiC grain structure for AGRBW-1W TRISO batches with SiC deposition duration = 131 min, MTS flow = 157 cc/min, and SiC deposition
temperature = 1450 °C. (a and b) small kernel’s (c and d) large kernels.

Fig. 5. SEM image of SiC grain structure for AGRBW-1V TRISO batches with SiC deposition duration = 131 min, MTS flow = 138 cc/min, and SiC deposition
temperature = 1450 °C. (a and b) small kernel’s (c and d) large kernels.
138 P. Hosemann et al. / Journal of Nuclear Materials 442 (2013) 133–142

Fig. 6. SEM images of SiC grain structure for AGRBW-2T TRISO batches with SiC deposition duration = 122 min, MTS flow = 179 cc/min, and SiC deposition
temperature = 1500 °C. (a and b) small kernel’s (c and d) large kernels.

Fig. 7. SEM images of SiC grain structure for AGRBW-3R TRISO batches with SiC deposition duration = 127 min, MTS flow = 148 cc/min, and SiC deposition
temperature = 1550 °C. (a and b) small kernel’s (c and d) large kernels.

Fig. 8. SEM pictures of SiC grain structure for AGRBW-3S TRISO batches with SiC deposition duration = 129.2 min, MTS flow = 174 cc/min, and SiC deposition
temperature = 1550 °C. (a and b) small kernel’s (c and d) large kernels.
 P. Hosemann et al. / Journal of Nuclear Materials 442 (2013) 133–142 139

Table 2
Summary table of the results obtained from nanoindentation and grains structure analysis including the basic production parameters.

Sample SiC SiC MTS Average H. ± Average H. ± Average H. ± SiC outer SiC H SiC grain size Average red ±
dep. dep. flow outer edge outer edge SiC/IPyC edge grain gradient diameter (lm) modulus
time temp. SiC SiC interface structure across SiC
(min) (°C) (cc/ (GPa) (GPa) (GPa) (GPa) (GPa) (GPa) IPyC/ Middle Outer (GPa) (GPa)
min) SiC edge
AGRB-2T-A2 122.0 1500.0 179.0 30 2 34 2 28 3 Medium Slight 2.0 2.1 3.0 220.0 11.0
AGRB-2T-C2 122.0 1500.0 179.0 31 2 33 4 30 3 Medium Slgiht 1.5 1.8 2.3 195.0 8.0
AGRB-1W-A2 131.0 1450.0 157.0 39 1 38 1 40 1 Fine None <1 <1 <1 335.0 5.0
AGRB-1W-C2 131.0 1450.0 157.0 40 2 41 2 38 3 Fine None <1 <1 <1 328.0 13.0
AGRB-1V-A2 131.0 1450.0 138.0 41 3 42 3 41 3 Fine None <1 <1 <1 318.0 8.0
AGRB-1V-C2 131.0 1450.0 138.0 38 4 39 4 36 3 Fine Slight 1.1 1.3 1.8 322.0 16.0
AGRB-3R-A2 127.0 1550.0 148.0 36 2 39 1 32 3 Large Large 2.2 2.7 3.3 304.0 10.0
AGRB-3R-C2 127.0 1550.0 148.0 36 3 38 2 34 3 Large Large 1.2 2.4 2.7 298.0 14.0
AGRB-3S-A2 129.0 1550.0 174.0 42 3 41 4 42 3 Large None 1.7 3.2 4.6 340.0 13.0
AGRB-3S-C2 129.0 1550.0 174.0 39 2 41 1 36 2 Large Slight 1.4 2.4 2.7 314.0 10.0

was found from sample to sample. The summarized hardness data

in Table 2 includes two columns, where the average hardness is
listed as a function of location in the SiC layer (near the IPyC/SiC
interface and near the outer edge). The nanoindentation results
for all variants show that some of the fuel particles had a hardness
gradient in the SiC layer, where a higher hardness value at the out-
er edge of the SiC was found. This gradient is qualitatively summa-
rized in Table 2.
The indentation fracture toughness data are displayed in Table 3
for selected samples. Most samples experienced an anisotropic
fracture behavior. The cracks propagated significantly further in
the azimuthal direction than in the radial direction, as can be seen
in the AFM image in Fig. 2. This is particular interesting since the
Fig. 9. Compiled hardness values across the three layers for all TRISO variants. columnar grains tend to be oriented in the radial direction. It
was also observed that the cracks are of a transgranular rather than
intergranular nature. The difference in crack length resulted in dif-
Table 3 ferent fracture toughness values in the two directions (Table 3),
Results obtained from indentation fracture toughness measurements. with a significantly higher fracture toughness in the radial direc-
Sample Tangential average fracture Radial average fracture tion. It is also interesting that the azimuthal cracks were not
toughness (MPa m1/2) stress (MPa m1/2) straight, but rather followed the circumferential path of the
AGRBW 1W-A2 1.5 ± 0.6 1.7 ± 0.3
particle.
AGRBW 1W-C2 1.1 ± 0.8 2.1 ± 0.8 The crush test results are reported in Table 4. For samples 2T-A2
AGRBW 2T-A2 1.1 ± 0.6 1.6 ± 0.3 and 2T-C2, a significant difference in the fracture stress was found,
AGRBW 2T-C2 1.2 ± 1.5 3.6 ± 3.6 while the production parameters were the same but not the kernel
AGRBW 3S-C2 1.0 ± 0.5 1.8 ± 0.8
diameter. This observation is discussed in more detail in the dis-
cussion section of this paper.
increase in the grain structure size progressing towards the outer
part of the SiC layer. This is reflected by the three columns in
Table 2 showing the average grain size measured near the IPyC/ 5. Discussion
SiC interface, the middle of the SiC layer and the outer edge.
The nanoindentation results for all the samples are plotted in This study on the mechanical properties of TRISO fuel particles
Fig. 9. There, the complete hardness profiles for the SiC layer, IPyC delivers a range of different parameters as a function of processing
layer, and kernel are displayed. As expected the SiC is the hardest condition which are discussed in this section. The data suggests a
structure while the IPyC is the softest; however, sample to sample strong influence of the kernel diameter and SiC growth condition
variations were found. It can be seen that the IPyC layer has a on the grain structure, and, therefore, possibly some influence on
rather homogeneous hardness profile, indicating that the measure- the mechanical properties.
ments are reasonably reliable since the hardness numbers show Most specimens investigated showed the often reported grain
minimum sample to sample variation. The same is true for the structure of fine grains at the IPyC/SiC interface and larger grains
surrogate fuel kernel, where no significant hardness variation at the outer areas [40]. As expected, due to their low energy of for-

Table 4
Crush test fracture stress results.

Sample SiC dep. MTS flow SiC dep. Local fracture Mean fracture Avg. hardenss ± (GPa) Avg. hardenss ± (GPa) Avg. red ± (GPa)
temp. (°C) (cc/min) duration (min) stress (MPa) stress (MPa) across SiC (GPa) SiC/IPyC modulus (GPa)
interface (GPa)
AGRB-1 W-A2 1450 157 131 1182 356 39 1 40 1 335 5
AGRB-2T-A2 1500 179 122 1074 196 30 2 28 3 200 11
AGRB-2T-C2 1500 179 122 1481 109 32 2 30 3 196 8
AGRB-3R-A2 1550 148 127 1047 203 36 2 32 3 304 10
AGRB-3S-A2 1550 174 129 1560 461 42 3 42 3 341 13
140 P. Hosemann et al. / Journal of Nuclear Materials 442 (2013) 133–142
mation stacking faults were observed similar to what was reported
in [41]. The data also suggests that higher deposition temperature
results in larger grains and causes a larger grain size gradient
throughout the sample, while lower deposition temperature pro-
duces a finer and more homogeneous distribution of grain size. It
appears that samples with longer deposition times (indicating low-
er deposition rate) can be seen as having a finer grain structure
than the samples with a shorter deposition time. No clear trend
can be seen from the variation in the MTS flow. Samples with lar-
ger grains on the outside of the TRISO fuel particle still maintain a
fine grain structure near the IPyC interface, leading to a gradient in
average grain size and a radial arrangement of the grains. Similar
results have been reported in [42,27] where even a 1300 °C depo-
sition temperature was reported. A detailed study outlining the
grain structure and type of grain boundaries has recently been
published by [41]. The results found here agree well with the grain
sizes found in that study.
The nanoindentation results obtained draw a similar picture. A
hardness of 36–42 GPa and an E-modulus between 304 and
341 GPa was found on most samples, except the specimen
AGRBW-2T-A2 and AGRBW-2T-C2, which showed a lower hard-
ness and a modulus around 200 GPa. The most significant differ-
ence on these samples was that they had the shortest deposition
time of 122 min and the highest MTS flow rate (179 cc/min).
The indentation results presented here are similar to what was
found elsewhere [43]. In [23] it was found that different moduli
can be found as a function of grain structure in respect to the
indentation direction, so that indents in grain axis showed a mod-
uli of 440 GPa, while grains tilted 15° towards the indenter showed
a moduli of 400 GPa. This was not reproduced here, since the sam-
ple was always cut near a 90° axis (cross section) in this case.
The hardness of the IPyC was consistently between 4 and 6 GPa,
and the reduced modulus between 20 and 30 GPa, which is in good
agreement with data reported in [44].
Fig. 10. SiC Average hardness and average reduced modulus vs. SiC deposition temperature (a). Average hardness and average reduced modulus vs. SiC Deposition duration
(b). Average hardness and average reduced modulus vs. MTS gas flow (c). Average hardness vs. mean fracture stress obtained from crush testing (d).
A small but measurable gradient can be found from the IPyC/SiC
interface to the outer surface. The SiC near the IPyC/SiC interface
shows higher hardness values than the indents placed at the out-
side area especially on specimens which also experience a larger
microstructural gradient throughout the SiC layer. On the very fine
grained material this was not observed. It appears that the grain
structure is directly linked to the hardness within the same mate-
rial and that the finer grain structure leads to higher hardness
within the same SiC layer. Investigations of pore densities might
be of value as a function of layer thickness, but were not conducted
here. However, considering the rather different production param-
eters it was found that the hardness is rather similar across all
samples.
A significant observation from the fracture toughness measure-
ments was that the cracks induced with the Berkovich tip had an
anisotropic nature. The cracks found in the radial direction were al-
ways shorter than the cracks in the azimuthal direction, and the
cracks in the this direction followed the curvature of the SiC shell.
This means that the fracture toughness was higher in the radial
direction than in the azimuthal direction. Utilizing the calculations
mentioned in the experimental section of this paper it was found
that the fracture toughness was nearly twice as high in the radial
direction (Table 3). In order to avoid any effect of the 3 sided pyr-
amid, up to 10 indents were placed on a SiC shell, changing the an-
gle of the three sided pyramid to the outer edge as the three sided
pyramid (indenter) was moved around the circumferential direc-
tion. This did not impact the anisotropic cracking. It appears that
the cracks go through the grains and do not follow any particular
grain structure, which is in contrast to [23] but can be seen in
Fig. 2. However, since no TEM was conducted, it is not known if
there are finer nano-cracks underneath the indents. The question
remains, why did the cracks in the azimuthal direction propagated
further than in the radial direction. The idea of having remaining
stress in the sample from processing might be viable, however,
 P. Hosemann et al. / Journal of Nuclear Materials 442 (2013) 133–142 141

Table 5
results from microcantilever experiments.

Sample Bend bar a (m) b (m) w (m) L (m) P (N) Fracture toughness (MPa m1/2)
IV-C2 2 1.22E-06 7.13E-06 6.07E-06 1.20E-05 1.85E-02 7.99
1V-C2 4 5.00E-07 5.53E-06 7.89E-06 9.20E-06 2.04E-02 5.24
1V-C2 7 1.31E-06 8.05E-06 5.44E-06 1.30E-05 8.41E-03 3.79
1W-A2 1 1.50E-06 6.45E-06 4.13E-06 1.30E-05 4.76E-03 4.47
1W-A2 2 1.50E-06 6.82E-06 3.46E-06 1.30E-05 4.70E-03 5.03

[41,45] recently showed that it appears there is no significant
strain in the lattice on a TRISO particle cross section. High resolu-
tion microbeam XRD or Raman might be able to investigate this
question in more detail in future studies to come.
Considering the fact that the TRISO shell has higher fracture
toughness in radial direction than in circumferential direction
can be discussed in the light of in reactor service. In actual opera-
tion this anisotropic property can be desirable. A radial fracture pe-
netrating from the IPyC to the outside of the particle can lead to
immediate fission gas release while a circumferential crack will
still prevents this. In fact a circumferential crack might help releas-
ing stress in the SiC particle and therefore makes radial cracks less
likely which improves the properties. Also radial cracks potentially
generated during operation can hit a preexisting circumferential
crack and get deflected which also helps to prevent fission gas
release.
The crush tests conducted on these coating batches lead to the
data reported in Table 4. Five specimens were selected. The mean
fracture stress obtained by crush tests correlated well with the
average hardness data, and formed a linear correlation (Fig. 10).
The relationship between hardness and mean fracture stress can
be calculated to be 0.0316 + 27.376. Comparing the local and
the mean fracture stress, it is found that sample 2T-A2 and 2T-C2
experience a lower mean fracture stress which correlates well with
the lower hardness numbers found. While the data between mean
fracture stress and hardness is consistent to each other as dis-
played in Fig. 10d it is not entirely clear what causes the softer
and weaker properties (see Figure 11d)
In the past, it was reported that fracture toughness can be mea-
sured via a microcantilever bend bar testing technique [46,21,48],
[50] where one manufactures a microbend bar utilizing a FIB and
performs the associated test utilizing a nanoindenter. In this work,
initial efforts were made to perform similar tests. The FIB quanta
3D FEG was used to manufacture bend bars, and initial tests were
made. Since this research is in its early stage we report these re-
sults under discussion in order to give a comprehensive view of
the techniques and measurements but not to fully document the
results at this time. Fig. 11 shows images from the microcantilever
bend bar test and an initial dataset; the results of first tests are re-
ported in Table 5 utilizing the equation proposed in [21]. It was
found that these initial datasets show a 2–3 times higher fracture
toughness than measured using the indentation technique and as
reported in the literature. It appears that this is due to the fact that
it is not a simple task to manufacture a sharp notch on the speci-
men using the FIB and the notches manufactured in this first at-
tempt were too dull. A pre-notching and fatigue cracking
technique like that proposed in [49] might be a more desirable ap-
proach. However, with the development of high temperatures ind-
enters this technique when improved so sharper notches are made
can be also conducted at higher temperatures.
Initial attempts were also made to simplify the crush testing. In-
stead of a half sphere, a C-Ring was manufactured and tested. The

Fig. 11. Microcantilevers manufactured in the 1V-C2 specimen (a). Fractured cantilever in cross section (fracture surface) (b). Load displacement curve obtained from
microcantilever experiments (c). Experimental setup of in situ ring push testing (d).
142 P. Hosemann et al. / Journal of Nuclear Materials 442 (2013) 133–142
tests were performed in situ in collaboration with LANL on a cus-
tom-built mesoscale mechanical testing stage. While the sample
handling is significantly more delicate, the benefit of such in situ
testing is clearly visible, since one can observe the failure directly.
However, great care has to be taken to not damage or pre-crack the
100 lm wide C-bend specimens. In addition, the outer layer of the
SiC is in tension and the inner layer in compression, which is not
the same loading condition as in service. Nevertheless, as a quan-
titative measurement and quality control method, these types of
tests might still be useful.
6. Conclusions
Mechanical and microstructural characteristics of SiC and PyC
shells in TRISO particles were characterized in this study utilizing
a range of different small scale mechanical testing techniques. It
was found that the grain structure gradient correlates with the
nanohardness across the SiC layer, where the IPyC/SiC interface
was harder (smaller grains) and the outside rim was softer (larger
grains). Columnar grains were found on the samples manufactured
with higher deposition temperature while the lower temperature
samples showed smaller grains and more homogeneous
properties.
Indentation hardness and crush test strength correlated well. It
was found that a linear correlation between these two techniques
existed. Fracture toughness measurements were also conducted
and it was found that the samples had an anisotropic fracture
behavior leading to higher fracture toughness in the radial direc-
tion, compared to the azimuthal direction. Also the cracks in azi-
muthal direction follow the SiC curvature. It is important to note
that the cracks propagated perpendicular to the grain structure
rather than with the grain structure, and the cracking was trans-
crystalline. Recent approaches and ideas for in situ C-bend testing
and microcantilever testing were also introduced.
Acknowledgements
The authors want to thank the NRC for providing funding for
this work, through NRC faculty development grant number NRC-
38-09-948. In addition, we want to thank the DOE/AGR program
at ORNL and the NRC safeguards program for student support.
Instrument access at CAES was supported by the ATR-NSUF user
program at Idaho National Laboratory, which is supported by the
US Department of Energy, Office of Nuclear Energy under DOE Ida-
ho Operations Office Contract DE-AC07-051D14517.
We also want to thank N. Mara and W.M. Mook for performing
an initial ring crush feasibility test utilizing the in situ loading
stage in the SEM at Los Alamos National at the Centre for Inte-
grated Nanotechnologies, a US Department of Energy.
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