2013 International Nuclear Atlantic Conference – INAC 2013

Recife, PE, Brazil, November 24-29, 2013

ASSOCIAÇÃO BRASILEIRA DE ENERGIA NUCLEAR – ABEN
ISBN: 978-85-99141-05-2

STUDY OF TRANSVERSE CRACK FORMATION ON SURFACE

AREA OF UO2 PELLET CIRCUMFERENCE.

Dionísia S. Oliveira1, Lélia F. P. C. Paneto1 and Patrícia O. de Souza1

1
Gerência de Análise Técnica do Combustível Nuclear
Indústrias Nucleares do Brasil S. A.
Rodovia Presidente Dutra, km 330 Engenheiro Passos
27555-000 Resende, RJ
dionísia@inb.gov.br
lelia@inb.gov.br
patriciasouza@inb.gov.br

ABSTRACT

Microstructure of a polycrystalline material has a considerable influence on particular properties, such as

mechanical strength, electrical conductivity, optical transmission and magnetic susceptibility. The uranium
dioxide (UO2) is used in water-cooled nuclear reactors, due to its desirable ceramics characteristics as a nuclear
fuel. The UO2 is used in the form of pellets manufactured by wet route by INB, where they are loaded into fuel
rods to build the fuel assemblies used in pressurized water reactors of Angra 1, Angra 2 and future Angra 3
nuclear power plants, for electric energy generated from nuclear power in Brazil. The geometric and structural
integrity of these pellets cause direct influence on their performance during the reactor core operating cycle ,so
pellets presenting surface cracks leading to the phenomenon of pellet cladding interaction-PCI, resulting in
failures in the fuel rod and subsequently release of fission products in the reactor coolant. Transverse cracks on
surface area of pellet circumference are detected by visual inspection during the manufacturing process. This
paper presents the study of these cracks formation by content analysis conducted with the support of electron
microscopy. These results here are analyzed from the point of view of materials science through observation of
the microstructure, and the pressing process where the defect was probably generated.

1. INTRODUCTION

The fuel pellets of uranium dioxide are produced in Brazil through a sequence of
manufacturing steps with control measures designed to ensure that the product complies with
the design requirements [1]. In the manufacturing process, after mixing the UO2 powder with
U3O8 originating from recycled material and lubricant, the blended mixture is transported to
the automatic rotary press, where a metal matrix by pressure applied by the upper and lower
punches in order to form products called green pellets, since they aren’t still sintered. The
green pellets are then inserted into a sintering furnace and heated around to 1750°C to
increase hardness and acquire the necessary resistance to operating conditions that they are
submitted within the reactor of the nuclear power plants Angra 1 and Angra 2 [2].
 Figure 1: Manufacturing process of fuel pellets UO2 [2].

After the processes of pressing, sintering and grinding (figure 1), the visual inspection step
allows to verify whether cracks occurred on the surface of UO2 fuel pellets, as shown in
figure 2, where it’s presented two transverse cracks in surface area UO2 pellet
circumferences. So this current paper aims to study the formation of these cracks through
metallographic examinations by optical and scanning microscopies, and further presenting
analysis of the parameters that influence the pressing process.

Figure 2: UO2 design pellets presenting transverse crack in the surface area of its circumference.

2. MATERIALS AND METHODS

UO2 fuel pellet manufactured by wet route with nominal density of 10.40 g/cm3 and 4.25%
enriched uranium-235 having transverse crack in the circumference area was used for
microscopy analysis. The cross section of the UO2 fuel pellet sample was obtained in a
manner that it clearly observes the extent of cracking, from surface until interior of the pellet.
For this purpose, the pellet was embedded in cold resin, followed of thermal attack at 1400°C
for 4 hours. The metallographic analyses were obtained by optical and scanning microscopies
with 100X and 400X magnification, respectively
The homogenization and pressing process parameters appropriated to the pellet design are
shown in table 1 and then compared with the press process parameters generated in the
production of the pellets that presented cracks. Analyses were done by consulting the data of
the control program of the press as shown in table 2: lower pressure and higher pressure of
the punch, lubrification pressure, green density, filling depth and pressing speed.

Table 1: Process parameters of homogenization and pressing.

Target value
Nominal operating values Limits Unit
(set-point)
Homogenization time mín ≥ 120 120 minutes
Green density limits value 5.55 a 5.75 5.65 g/cm3
Pressing pressure limits limit 1.5 a 5.0 - t/cm2
Speed press limit 101 a 152 101 pellets/minute
Source: Data process of INB.

Table 2: Parameters of production press

Presure (bar) To target density of 5.75 g/cm3 (1)

Filling

height
Table
depth
Run

Number punch Pellet density

Upper Bottom Lubrication pellet which is above the
above the tolerance tolerance
1 8.8 8.8 1.8 34.5 17.1 - -
3 8.7 8.7 1.8 34.5 17.1 13 5.83
5 8.7 8.7 1.8 34.8 17.1 - -
7 8.8 8.8 1.0 34.5 17.1 15 5.83
9 8.8 8.8 1.8 33.6 17.1 13 5.85
11 8.78 8.78 1.0 33.8 17.1 - -
13 5.84
13 8.77 8.77 1.8 34.2 17.2
15 5.86
15 8.9 8.9 1.8 34.3 17.2 - -
Source: Control system of the press.
(1) Green density 5.75 g/cm3 ± 0.05g/cm3.

3. RESULTS

As can be observed from optical metallography at a 100X magnification (figure 3a), the
grains show straight edges and glossy surface. There is the presence of a crack with
appearance predominantly intergranular in the grain boundaries. As can also be shown from
metallography scanning at a 400X magnification (figure 3b) the microstructure confirms
microvoids located in grain boundaries and the presence of a crack with characteristic
intergranular in certain regions and transgranular, through the grain, in other. No
metallographic analysis realizes the presence of second phase precipitates in the grain
boundaries [3].
 a) b)

Figure 3a: Optical metallography with 100X magnification showing the crack propagation in grain boundaries;
Figure 3b: Scanning metallography with 400X magnification showing the crack propagation and pores.

Alignment of pores and stress line on pellets surface is shown in figures 4a and 4b through
optical micrographs with 50X magnification, respectively. Probably the causative agent
evidenced at the pellets is owing to these defects.

a) b)

Figure 4a: Optical metallography with 50X magnification showing an alignment of pores;
Figure 4b: Optical metallography with 50X magnification showing a stress line.

The press machine is programmed in accordance with the suitable parameters to achieve an
acceptable product (table 1). However due the aging of the machine, adjustments were made
during the process to ensure the desired density values (table 2). The process target density is
5.75 g/cm3 with tolerance of ± 0.05 g/cm3, a value above the predicted would result in a
diversion of waist in pellet (figure 6) during the sintering process, this situation also occurs
with density values below the minimum tolerance. According to table 2, pellets from
punctures 13 and 15 showed density above the allowable tolerance, however its influence was
not observed in the crack formation.
The deficiency of the lubricant in lower punch was detected with evidence of enhanced
brightness on lateral surface pellet. The lack of lubricant has been corrected by adjusting
valves and regulating micrometric adjusting the lubrication pressure, regulating the amount of
lubricant to each matrix [4].
Taking into account that in the pressing process in analysis, the enrichment uranium 235
information is recorded at the pellet top by the top punch printing, was found easily that the
pellet analyzed showed crack in the top to the surface center of the circle (figure 2) giving its
proximity to the upper punch.

4. DISCUSSION

The phase diagram of the uranium-oxygen system (figure 5) shows that in the equilibrium
condition and stoichiometric 2.01 for oxygen/uranium ratio at temperatures up to about
337ºC, two phases are present UO2+X and U4O9-y [5], but according to figure 3a and 3b is not
observed inclusions and precipitates along the grain boundaries or second phase particles
retained in microstructure as a result of abrupt cooling after the sintering process causing
weakening. The grains are cohesive and impurities are not presented in the grain boundaries
[6].

Figure 5: Uranium-oxygen system phase diagram [5].

In the analysis of microstructure represented in figures 3a and 3b it is noted that the crack
originated in the grain boundary by microvoid nucleation and the formation of the cavity
(figure 3b) occurred in stress-rupture condition at high temperature. Figures 4a and 4b
respectively show micrographs showing stress-line and aligned pores. The presence of these
defects is derived, in most cases, of anomalies in the pressing process causing the appearance
of cracks and in many cases leading to fracture the pellet.
Regarding the type of crack, some considerations are made: the presence of intergranular
cracks in the grain boundaries, is an indication that the crack may have propagated in the
early sintering as a cause of the density gradient and, by the presence of transgranular crack,
cracks passing through the grain, its propagation may have occurred during cooling
influenced by the temperature gradient or phase changing.
In the pressing, stage of the manufacturing process, the friction force between the powder
particles and the matrix may reduce the applied pressure causing uniform density gradients as
shown in figure 6 [7], so the appearance of transverse cracks in the area of the pellet
circumference can happen due to inhomogeneity in the green pellets influenced by the
difference in pressing force of the upper and the lower punches often arises from the lack
lubrication, whose function is to reduce the frictional force between the powder and the
matrix wall during the compression and to avoid retention force during the green pellet output
of the matrix to the flat-boat [8]. Compression occurs by simultaneous displacement of the
upper and lower punches, if there is difference of these forces can occur displacement of the
“neutral zone” which is the region where the powders particles suffer less influence of
mechanical compression, i.e., lower strength compression which will generate final pellet
heterogeneous zones with different properties (figure 6). Around the neutral zone there is a
degree of compaction incompatible with the part of the other regions and cracks may occur
on the pellet surface. An increase in the pressing pressure influences positively increasing
density, but otherwise appear cracks at the pellets ends faces [9].
However, the pressing machine does not issue report with the actual values, it is not possible
to show the actual pressure values of the upper and lower punches, i.e., the difference in
compression was not measurable. In the data analysis pressing machine (table 2) revealed that
the values of lubricant, upper and lower pressure parameters have been introduced by the
operator and adjusted as happened target value deviations in the density. The green pellets
density is highly heterogeneous and depends on the pressing parameters: applied pressure,
residence time, lubrication of matrix wall, as well as the pellets geometry: diameter,
length/diameter ratio. If all parameters are not specified, it will happen in the density
distribution of green pellets different than expected.

Figure 6: Distribution of the density green pellets after the pressing process.
 5. CONCLUSION

Evidences of metallographic analysis indicates the cause of the crack formation, the
combination of porosities alignment and the appearance of internal stresses at high
temperature caused by inhomogeneity of the Green pellets by atypical density gradient at
sintering. These abnormalities were consequences of the difference in strength between the
upper and lower punches by lack of lubrication through the lower punch in the pressing step.
The difference in compression force between the punches shifted the neutral zone
immediately to above the center of the pellet causing a asymmetric distribution density of the
green pellet and providing opening of the crack by difference in density between the regions.

Acknowledgements

We thank the pellets expert Georg Maier for having shared their valuable knowledge that
contributed greatly to this work, our manager Márcio Adriano Coelho da Silva for his
encouragement and guidance in our activities and laboratory technical Ticiana Aparecida
Vieira Gomes and Luiz Arnaldo Rodrigues Olegário by their talent and dedication in sample
preparation and processing of the images.

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