Nuclear Engineering and Design 263 (2013) 509–514

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Nuclear Engineering and Design

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

Computational and experimental prediction of dust production in pebble bed

reactors, Part II
Mie Hiruta a , Gannon Johnson a , Maziar Rostamian a,∗ , Gabriel P. Potirniche a , Abderrafi M. Ougouag b ,
Massimo Bertino c , Louis Franzel c , Akira Tokuhiro a
a
Department of Mechanical Engineering, University of Idaho, 1776 Science Center Drive, Idaho Falls, ID 83401, USA
b
Idaho National Laboratory, 2525 N Fremont Avenue, Idaho Falls, ID 83401, USA
c
Department of Physics, Virginia Commonwealth University, Richmond, VA 23284, USA

h i g h l i g h t s

• Custom-built high temperature, high pressure tribometer is designed.

• Two different wear phenomena at high temperatures are observed.
• Experimental wear results for graphite are presented.
• The graphite wear dust production in a typical Pebble Bed Reactor is predicted.

a b s t r a c t
a r t i c l e i n f o
This paper is the continuation of Part I, which describes the high temperature and high pressure helium
Article history:
environment wear tests of graphite–graphite in frictional contact. In the present work, it has been
Received 18 November 2012
Received in revised form 16 April 2013 attempted to simulate a Pebble Bed Reactor core environment as compared to Part I. The experimental
Accepted 19 April 2013 apparatus, which is a custom-designed tribometer, is capable of performing wear tests at PBR relevant
higher temperatures and pressures under a helium environment. This environment facilitates prediction
of wear mass loss of graphite as dust particulates from the pebble bed. The experimental results of high
temperature helium environment are used to anticipate the amount of wear mass produced in a pebble
bed nuclear reactor.
© 2013 Elsevier B.V. All rights reserved.

1. Introduction PBRs have always been considered as a potential safety concern

The Pebble Bed Reactor (PBR) is a High Temperature Gas-
Cooled Reactor (HTGR). Because of its unique online refueling
design, PBR is counted on less shut-down time for maintenance
and more efficient operation. The pebble bed in such reactors is
comprised of thousands of billiard-sized graphite-matrix spheres
as fuel elements. Each pebble contains the Tristructural-isotropic
(TRISO) nuclear fuel particles. These pebbles travel from the top
of the reactor to the bottom. They are exposed to pressurized
helium coolant and high temperatures ranging from 650 ◦ C to
950 ◦ C. As the pebbles traverse downward through the reactor,
the amount of graphite dust produced under frictional contact and
thus circulated and eligible for release under a postulated acci-
dent like depressurization and subsequent air ingress, is a design
review safety concern. Graphite dust production in previously built
∗ Corresponding author. Tel.: +1 208 310 9555.
E-mail addresses: mrostamian@asme.org, mzram 22@yahoo.com
(M. Rostamian).
(Moormann, 2009). Multiple observations are reported for the Ger-
man Arbeitsgemeinschaft Versuchsreaktor (AVR, 1960–1980) on
the accumulated dust. However, the phenomena of dust production
have never been closely examined experimentally and computa-
tionally. Computational prediction (Rostamian et al., 2010, 2011,
2012) of graphite particulate formation at room temperature has
been conducted for room temperature experiments. These works
showed a very good agreement with a review on the results by
Xiaowei et al. (2005) and by Cogliati et al. (2011). Part I of this paper
is a computational micromechanics study of graphite wear, which
introduces a nonlinear wear model for graphite (Rostamian et al.,
2013). This model predicts the experimental data from a custom-
designed tribometer. Since high temperature properties of graphite
other than its module of elasticity, are not available, high tempera-
ture finite element simulations have not been conducted to produce
a nonlinear wear law for graphite at high temperatures.
In the literature of wear of brittle materials, temperature effects
have not widely been discussed. And in those discussing the tem-
perature effects, specific cases based on the target application were
reported (e.g. Grigor’ev et al., 1983). In the present experimental

0029-5493/$ – see front matter © 2013 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.nucengdes.2013.04.032
510 M. Hiruta et al. / Nuclear Engineering and Design 263 (2013) 509–514

study, however, wear of graphite in a wide range of temperatures Table 1

Design parameters for the testing apparatus.
(20–750 ◦ C) have been studied. In an effort to quantify the fric-
tional wear mass loss from graphite pebbles in the pebble bed, Testing parameter Description Source
a custom-designed tribometer has been developed to measure Maximum temperature 750–900 ◦ C Reactor outlet temperature
the wear of graphite pebbles in helium atmosphere at pressures (Nelson et al. (2011))
and temperatures expected in modern Graphite-Moderated Gas- Maximum pressure 6.5 MPa Primary loop pressure
Cooled Reactors (GM-GCR). This paper describes in details the (Nelson et al. (2011))
Helium environment 99.998% HTGR standards, airgas
design, deployment of the device and the experimental data of
catalog
nuclear grade graphite. The graphite dust mass produced from the Normal force 10–50 N Past Chinese studies
tribometer is then used to predict the mass produced in a PBR (Xiaowei et al. (2005))
during a full working year as discussed by Cogliati et al. (2011). Velocity <0.1 m/s Cogliati et al. (2011)
Total distance ∼500 m Xiaowei et al. (2005),
Kadak and Bazant (2004)
2. Experiment Contact geometry Sphere–sphere Pebble–pebble contact

2.1. Experimental apparatus

The majority of the test data is below the higher outlet tem-
peratures expected under normal PBR operation. Also, there is no
test data for graphite matrix or graphite at the temperatures and
pressures expected in a PBR. To conduct wear tests under such con-
ditions, a custom test apparatus was designed. In this section, the
design requirements and the experimental setup are explained in
details.
2.2. Design requirements
apparatus is essentially a small twin-disk tribometer housing in a
furnace that is completely encompassed by a pressure vessel. With
a water cooling loop removing the heat outside the furnace, the
concurrent, demanding design requirements of high pressure and
temperature were effectively decoupled. The large pressure vessel
allowed for no mechanical feedthroughs and for real-time mea-
surement of the particulate mass and the normal force applied with
only non-mechanically actuated penetrations through the pressure
boundary. The frame of the tribometer is mounted to the underside
of the top removable lid of the pressure vessel (see Fig. 1).

The tribological properties of graphite depend on several fac-
tors. Therefore, the ability to perform tests on separate effects to
simulate the real conditions of a PBR is considered important in
obtaining accurate wear rates for graphite. The design parameters
that were selected are listed in Table 1.
2.3. Tribometer design
The motion requirements for sliding between two spheri-
cal objects led to the selection of a twin disk tribometer. The
2.4. Experimental material
The main carbonaceous components in the PBR are the spher-
ical fuel elements and the core reflectors. The latter is made
from nuclear grade graphite while the fuel elements them-
selves are made from what is referred to as graphite-matrix.
This graphite matrix classically comprised of natural graphite,
synthetic-graphite, and a phenolic resin binder. This mixture is
then isomolded or quasi-isostatically molded into its final spherical
shape. It is then carbonized in heat treatment of up to 800 ◦ C, and

Fig. 1. Tribometer (left) and its schematic (right) with pebbles in contact and the modular analytical balance.
 M. Hiruta et al. / Nuclear Engineering and Design 263 (2013) 509–514
Fig. 2. Sample geometry and orientation within the tribometer.
finally purified in a vacuum at 1950 ◦ C (Zhao et al., 2006). The car-
bonization of the binder causes it to off-gas its organic impurities,
thus lowering it mass by approximately 9%.
Graphite matrix is not currently in production in the United
States. Therefore, nuclear grade graphite was tested as a surro-
gate to the graphite matrix. The nuclear grade graphite selected for
the initial test run was Toyo Tanso’s IG-11, which is fine grained,
isomolded graphite.
2.5. Sample geometry
The basic sample design conceived for testing to mimic the
geometry of the pebble bed with the apparatus is graphite disks
machined into 2.54 cm tall disks with a 6 cm outer contour (Fig. 2).
3. Experimental results
The initial sets of experiments were conducted in air under
room temperature (Rostamian et al., 2012). These tests served as a
baseline to later run experiments in helium and under higher tem-
peratures, and pressure. The test conditions under current study are
at inter-pebble forces of 20 N, in helium environment at tempera-
tures ranging from room temperature up to 750 ◦ C, all at a pressure
of 1 MPa. An initial test with IG-11 samples was run continuously
at a relative sliding velocity of 0.08 m/s (samples spinning in the
same angular directions at 0.04 m/s) for 12,600 s (3.5 h, 1008 m).
3.1. Atmosphere gas effects
Prior to testing the graphite, the samples were out-gassed for 1 h
under nominal vacuum of 1200–1700 mTorr1 for 1 h at 200 ◦ C. The
out-gas temperature was selected to match the temperature that
was observed to de-adsorption of water from a graphitic surface by
Robert et al. (1995), as would happen to the graphite under GM-GCR
conditions.
The initial results were primarily aimed at testing the function
of helium pressure and temperature on the wear and friction of
graphite contact surfaces. This was due to the past testing that had
inclusive evidence on the effect of temperature and the total lack
of temperature testing at elevated atmospheric pressure.
It is seen that the wear mass in helium environment is almost
1⁄3 of that attributed to air environment as reported by Rostamian
et al. (2012). The atmospheric dependence of graphite friction and
wear is due to the changes in graphite surface properties. The
lamellar structure of graphite helps the establishment of smooth
surfaces between graphite segments in sliding contact. The pres-
ence of absorbed helium may further improve the smoothing of
1
Millitorr is a small pressure unit for high vacuum measurements. 1 mTorr equals
0.133322 Pa.
511
Fig. 3. Experimental wear rates (Johnson, 2012) for various temperatures in com-
parison with prior results (Stansfield, 1969).
graphite surface in frictional contact (Rollins, 1961). The low fric-
tion of graphite is attributed to the fact that the crystallite basal
planes are low-energy surfaces (Roselman and Tabor, 1976). When
frictional contact initiates, the basal planes become damaged, lead-
ing to the production of ‘edge sites’, which leads to wear. This is
because the shear strength associated with edge site interactions
has been estimated to be 10–100 times greater than that between
basal planes (Roselman and Tabor, 1976). Lancaster and Pritchard
(1981) attributes the adsorption of gases and vapors to the reduc-
tion in adhesion between these sites. It is reported by Cannon
(1964) that freshly exposed edge sites generated during wear can
be neutralized by adsorption; directly from the gaseous environ-
ment or by migration of pre-adsorbed molecules already present
on basal planes. Therefore, it is seen that the difference between the
experimental data of atmospheric pressure tests and that of high
pressure helium environment is consistent with the gas adsorption
effects discussed in the literature.
3.2. Temperature effects
In the literature of wear of brittle materials, temperature effects
have not widely been discussed (Blau, 1992; Bhushan, 2000). And
in those discussing the temperature effects, specific temperature
ranges based on the target application were reported (Grigor’ev
et al., 1983). In the present experimental study, however, wear of
graphite in a wide range of temperatures have been studies. There
are two phenomena observed in the wear rate variations with tem-
perature (Fig. 3). At room temperature, wear occurs along a narrow
ring around the pebbles (Fig. 4) with a small amount of dust accu-
mulated (approximately 1 mg) for 1000 m of wear length. When
the temperature reaches 200 ◦ C, the wear mass increases to 400 mg
for the same wear length. This increase in wear rate is attributed
to the changes in the graphite surface. As mentioned in Section
3.1, edge sites are the main cause of large wear mass formation.
At higher temperatures, the edge sites are more prone to damage
especially due to the fact that the samples are out-gassed before
the experiments. The out-gassing effect is exactly opposite of the
gas adsorption effect explained in Section 3.1. This effect is seen to
be dominant up to 750 ◦ C.
It has been observed that the wear formation process at high
temperatures is different from that at room temperature. To dis-
cuss this difference, graphite surfaces at different temperatures
were characterized by Scanning Electron Microscopy (SEM) (JOEL
USA Inc. JSM-6610LV) at 20 kV. The surface of graphite from the
test at room temperature shows a scar width of about 1500 ␮m, as
seen in Fig. 4a. This is while the surface of graphite from the test at
512 M. Hiruta et al. / Nuclear Engineering and Design 263 (2013) 509–514

Fig. 4. SEM images of graphite surface at room temperature in helium after proper out-gassing (a) 35× and (b) 500×, and at 400 ◦ C (c) 35× and (d) 500×.

400 ◦ C shows a scar width of about 7500 ␮m, as partially illustrated
in Fig. 4c. The close-up image of the wear scar at room tempera-
ture shows a smooth surface (Fig. 4b), which indicates that graphite
wears with proper lubricant properties at this temperature. This
is why a small wear mass is reported for room temperature test.
This indicates that the edge sites that are created under the fric-
tional contact are overlaid evenly at the same time. By contrast,
the close-up image of the wear scar at 400 ◦ C shows a rough sur-
face with scale-like surface structure (Fig. 4d). This indicates that at
higher temperatures, the lubricant property of graphite is reduced
due to large edge site formation, which helps produce more dust
than at room temperature.
3.3. Wear mechanisms at high temperatures and high pressure
As mentioned in Section 3.2, the graphite wear rate reaches its
peak at 200 ◦ C and starts to decrease thereafter (Fig. 3). To investi-
gate a second mechanism contributing to the decreasing trend, SEM
and X-ray diffraction (XRD) analyses on the accumulated graphite
dust at different temperatures were performed. The SEM images of
the dust particles show a wide variety of grain sizes and flake types.
As seen in Fig. 5b and c, the large-sized flakes are observed at 400 ◦ C
and 750 ◦ C, respectively. This is consistent with our observations
in Fig. 4d, where at higher temperatures such as 400 ◦ C, graphite
shows a scale-like surface structure that helps produce flakes. The
change from powder formation at 200 ◦ C to powder and flake for-
mation at 400 ◦ C is observed by comparing the SEM images of dust
particles Fig. 5a and b. The size of the flakes at 400 ◦ C in Fig. 5b
approximately matches with the size of scales observed in Fig. 4d.
The flakes are of a much larger area-to-weight ratio in comparison
to powder dust. Therefore, flakes adhere to the surface of graphite
pebbles. This will then result in a decreasing trend in the wear rate
for temperatures higher than 200 ◦ C up to 750 ◦ C.
The XRD analysis of wear dusts at 200 ◦ C and 400 ◦ C are per-
formed to further study the wear mechanism at temperatures
higher than room temperature.
The surface forces that cause the thin flakes to adhere to the
surface can be of dispersion forces (Burnham and Kulik, 1997). The

Fig. 5. SEM image of graphite particles from wear test at (a) 200 ◦ C, (b) 400 ◦ C and (c) 750 ◦ C.
 M. Hiruta et al. / Nuclear Engineering and Design 263 (2013) 509–514
Fig. 6. XRD pattern of IG-11 crystallite at 200 ◦ C and 400 ◦ C in comparison to refer-
ence.
position of an electron about the nucleus of an atom is not fixed
with time; it oscillates, generating a fluctuating dipole field. The
field interacts with nearby atoms, inducing the appropriate instan-
taneous dipole moments in them that are always attractive. This
is known as the dispersion force because the frequencies corre-
spond to those of visible and ultraviolet light, which the fluctuations
disperse. The powder-to-flake ratio needs be addressed in future
studies.
The XRD results are shown in Fig. 6. The profile of reference
shows a well-ordered graphitized carbon crystal structure. The pro-
files of dust for 200 ◦ C and 400 ◦ C tests show weaker but broader
peaks. IG-11 is a highly-graphitized carbon. Therefore, (1 0 0) and
(1 0 1) peaks are originally separated as the reference indicates.
However, it is seen that the two peaks are merged into one broader
peak at higher temperatures. This suggests that the graphite parti-
cles have lost their well-graphitized structure, which results in high
wear rates at high temperatures. Even though the crystal structure
for graphite dusts of 200 ◦ C and 400 ◦ C are not different, it is seen
that the wear rate is higher at 200 ◦ C than at 400 ◦ C. SEM images
of the graphite dust particles indicate that the large-sized flakes
formed at 400 ◦ C can lower the wear rate. However, as explained
earlier, it is seen that the wear rate is higher at 200 ◦ C than at
400 ◦ C due to the difference in the type of wear formations and
wear particulates.
3.4. Dust estimate for a PBR
The wear experiments were performed using a custom-
designed tribometer capable of operating at temperatures ranging
from room temperature up to 750 ◦ C, all at a pressure of 1 MPa. The
accumulated wear mass is plotted with respect to the wear length
as illustrated in Fig. 7. The uncertainty associated with the wear
mass ±1 ␮g for one pebble under study. This is the uncertainty of
the scale used to record mass accumulation.
The accumulated wear from one pebble is used to predict the
amount of wear mass for a PBR of an actual size such as HTR-10.
Performing the type of calculation as conducted by Cogliati and
Ougouag (2010), for HTR-10 with an inventory of 27,000 pebbles
and a pebble flow rate of 125 pebbles per day, the wear mass is
predicted to be 2318.05 g/yr. The change from 5.36 g/yr at room
temperature to 2318.05 g/yr at elevated temperature of a PBR indi-
cates that the wear behavior of graphite significantly changes. This
behavior is explained as the increased brittleness of this material
at elevated temperatures due to an increase in the Young’s mod-
ulus as shown by Albers (2009). At elevated temperatures, edge
sites of a now more brittle material cannot stand the high stress
concentrations and fail. In this way a much higher amount of wear
mass is accumulated for HTR-10. This amount is in the order of
513
Fig. 7. Experimental high temperature, high pressure wear mass loss for IG-11.
magnitude of the 3 kg/yr dust estimate for AVR (Moormann, 2009).
This is a very good agreement, although it was a much larger reactor
as compared to the HTR-10.
It should be noted that the explosion tests performed by Poulsen,
University of Idaho, has determined a minimum dust concentra-
tion of 0.26 g/cm3 (Poulsen, 2011). Considering the dimensions of
HTR as reported by Wu (2002), the core volume is approximately
5m3 . Having a core porosity of 0.39 (Jun, 2008), the volume is
approximated at 1.95m3 . A crude approximation of the dust mass
inventory required for explosion will then be 508,322 g/yr. This
is approximately 220 times the amount of dust mass predicted
in the present study. Therefore, the possibility of explosions in
HTR as predicted by Poulsen (2011) is confirmed to be extremely
low.
It is known that helium gas environment in a typical PBR has
pressures up to 6.5 MPa (Johnson, 2012). Therefore, experiments
on high pressures are being performed at University of Idaho at the
Center for Advanced Energy Studies.
4. Conclusions
In this work a tribometer has been designed based on the
PBR temperature and pressure requirements. Wear tests at high
temperatures up to 750 ◦ C at a pressure of 1 MPa have been per-
formed in helium gas environment. It has been observed that at
higher temperatures the wear formation process is quite differ-
ent from that at room temperature. At temperatures higher than
room temperature a general increase of wear mass is observed. The
XRD analysis of graphite particulates has revealed that graphite
surface loses its well-graphitized crystal structure during wear
test. The loss of its original graphitized crystal structure increases
the likelihood of edge site formation, which increases wear. This
observation is confirmed by analyzing the SEM images of the
worn surface of the graphite pebble samples at various temper-
atures.
At temperatures higher than 200 ◦ C, the SEM analysis of graphite
particulates has revealed that particulates start to change from tiny
powder particulates to a combination of powder and flakes. In com-
parison with powder, flakes have a higher area to weight ratio.
Therefore, these flakes do not easily fall off from the graphite sur-
face due the adhesion forces with the surface of graphite samples. It
can be concluded that both of these phenomena exist at all temper-
ature ranges. However, at room temperature, the phenomenon of
flake formation is insignificant; instead powder formation is dom-
inant. On the contrary, at temperatures higher than 200 ◦ C, the
514 M. Hiruta et al. / Nuclear Engineering and Design 263 (2013) 509–514
phenomenon of surface adhesion affects the overall trend of wear
increase.
The predicted wear mass for a PBR with an inventory of 27,000
pebbles and a pebble flow rate of 125 pebbles per day, the wear
mass is predicted to be 2318.05 g/yr. However, at higher pressures,
the gas adsorption effects are anticipated to decrease the wear
mass. This is the work under study as part of this DOE NEUP project.
Acknowledgement
We express our gratitude to DOE, under NEUP09-151, “The
Experimental Study and Computational Simulations of Key Pebble
Bed Thermomechanics Issues for Design and Safety” for providing
financial support for this study.
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