Jonathan Mckinley Holt JNM 2008
Jonathan Mckinley Holt JNM 2008
Jonathan Mckinley Holt JNM 2008
com
Department of Mechanical and Materials Engineering, Queens University at Kingston, Ont., Canada K7L 1W9
Abstract
Over forty years of in-reactor testing and over thirty years of operating experience in power reactors have provided a broad under-
standing of the in-reactor deformation of cold-worked Zr2.5Nb pressure tubes, and an extensive data-base upon which to base models
for managing the life of existing reactors and for designing new ones. The eects of the major operating variables and many of the met-
allurgical variables are broadly understood. The deformation is often considered to comprise three components: thermal creep, irradi-
ation growth and irradiation creep. Of the three, irradiation growth is best understood it is thought to be driven by the diusional
anisotropy dierence (DAD). It is still not clear whether the enhancement of creep by irradiation is due to climb-plus-glide (CPG),
stress-induced preferred absorption (SIPA) or elasto-diusion (ED). The least understood area is the transition between thermal creep
and irradiation where the fast neutron ux may either suppress or enhance the creep rate. The three components are generally treated as
additive in the models, although it is recognized that this is only a crude approximation of reality. There are still signicant gaps in our
knowledge besides the thermal- to irradiation-creep transition, for example, the eect of Mo which is produced from Nb by transmu-
tation in the thermal neutron ux is not known, and on-going work is required in a number of areas. This paper reviews the current
state of knowledge of the in-reactor deformation of cold-worked Zr2.5Nb pressure tubes, and highlights areas for further research.
2007 Elsevier B.V. All rights reserved.
0022-3115/$ - see front matter 2007 Elsevier B.V. All rights reserved.
doi:10.1016/j.jnucmat.2007.02.017
R.A. Holt / Journal of Nuclear Materials 372 (2008) 182214 183
Table 1.1 damage and wear. In older CANDU units these changes
Chemical specication for Zr2.5Nb pressure tubes for CANDU reactors were not fully understood, and have required monitoring,
Element Limits (by weight) and in some cases maintenance. In newer CANDU stations
adequate allowances for them have been made for the
Niobium 2.42.8%
Oxygen 9001300 ppm design life of the reactor.
Nitrogen <65 ppm To assess their aging characteristics, pressure tubes are
Hydrogen Was <20 ppm, now <5 ppm subject to periodic non-destructive inspection, and material
Iron <1300 ppm surveillance, which, in Canada, requires a pressure tube to
be removed every three years from the unit with the highest
integrated neutron uence (lead unit), for evaluation of
the pressure is a relatively small axial component due to an fracture properties. These requirements are dened in
end-load from the out of core hardware that varies with Ref. [5]. The data that has been obtained from the periodic
time from tensile to compressive. The peak fast ux is up inspection and surveillance programs has been supple-
to 3.5 1017 n m2 s1, E > 1 MeV. The pressure tube and mented by in-service inspection programs, destructive
the annealed Zircaloy-2 calandria tube are separated by examination of tubes removed as a result of in-service
spacers and the annular gap is lled with owing CO2 to damage and irradiation of small specimens in test reactors
insulate the pressure tube from the cold moderator. The cal- [1013].
andria tube has a wall thickness of 1.4 mm and an inside
diameter of 129 mm. The pressure tubes are rolled into
403 stainless steel end-ttings at each end of the channel. 2. Deformation of pressure tubes
The end-ttings have mechanical closures to enable on-
power refueling and are connected to the heat transport sys- During reactor operation, the eects of temperature,
tem (HTS) by carbon steel feeders. stress and neutron ux change the dimensions of the pres-
The annulus gas system has been developed to detect the sure tubes. Irradiation and thermally induced deformation
presence of moisture if a leak develops in the primary pres- of fuel channel components will, in the absence of other
sure boundary inside the reactor core. The ability to detect mechanisms, eventually determine fuel channel life. The
moisture at an early stage of the formation of a sub-critical, dimensional changes in pressure tubes during normal reac-
through-wall crack in the pressure tube is an important tor operation are axial elongation, diametral expansion,
component in assuring leak-before-break of the tubes. sag and wall thinning. One can consider that there are three
mechanisms contributing to the dimensional changes: irra-
1.2. Aging mechanisms diation growth the change in shape at constant volume in
a fast neutron ux, thermal creep the change in shape due
Pressure tubes must accommodate the following aging to the eect of temperature and stress in the absence of a
mechanisms [79]: dimensional changes, material property fast neutron ux, and irradiation creep, the additional
changes, deuterium ingress due to corrosion and in-service change in shape due to stress and fast neutron ux [14].
184 R.A. Holt / Journal of Nuclear Materials 372 (2008) 182214
To a rst approximation the total in-reactor deformation assessing the microstructural and microchemical
rate is often expressed as the sum of these three terms, i.e., changes that occur during service [21];
and most recently:
e_ total
d e_ gd e_ icd e_ tc
d; 2:1
identifying the causes of variability between reactors and
where e_ is strain rate and the subscript d indicates the direc- between tubes in one reactor [22];
tion, and superscripts, g, ic and tc designate growth, irradi- creep at high stresses under multi-axial stress conditions
ation creep and in-reactor thermal creep, respectively. near aws [23,24];
To some extent, the creep and growth phenomena can the transition between thermal- and radiation-induced
be studied independently to determine their important creep near the ends of the tubes [25].
characteristics, however the real behaviour is more com-
plex than this, representing a continuum in a multi-dimen- For general reading on in-reactor deformation of zirco-
sional space of stress, fast neutron ux, temperature, fast nium alloys, see Refs. [26,27].
neutron uence and the microstructure of the material.
The changes in dimensions cause the stress state in the 2.1. Diametral expansion
pressure tube to vary with time, for example, while the
coolant pressure prole along the channel remains essen- Diametral expansion, which corresponds to an increase
tially constant with time, the internal diameter increases, in the circumference of the tube, occurs mainly by
and the wall thickness is reduced, resulting in an increase irradiation creep [14]. There is a small thermal creep com-
in the hoop stress. The change in the stress state must be ponent and the contribution of irradiation growth com-
taken into account to understand and predict the behav- ponent is actually negative, and therefore benecial. The
iour accurately. diametral strain is measured as mandated in Ref. [5].
The main trends of pressure tube deformation at normal For CANDU 6 reactors, approximately 90 diameter pro-
operating conditions were fairly well established by the les have been measured up to 123 000 full power hours
early 1980s based on various types of in-reactor testing in of operation, allowing statistical treatment of the data
the NRU Reactor at Chalk River and early diametral (examples of such data are given in Ref. [14]). A typical
and sag gauging results and elongation measurements from prole is shown in Fig. 2.1.1, and typical fast neutron ux
Pickering A [15]. In the past 20 years the emphasis has been and temperature proles are shown in Fig. 2.1.2. The
on: diametral strain is low near the ends of the tube where
the fast neutron ux is low, and peaks towards the outlet
extrapolating these results to newer reactors that oper- (hot) end.
ate at higher temperatures and with higher fast neutron An important factor aecting the shape of the diametral
uxes [16]; strain prole is the orientation of the coolant ow relative
making end-of-life predictions requiring long term irra- to the manufacturing direction of the pressure tube. Pres-
diations [12,17]; sure tubes are made using hot-extrusion, followed by
understanding sag of the pressure tube and the develop- cold-drawing and heating in a steam autoclave at 673 K
ment of contact between pressure tubes and calandria for 24 h [28]. In the hot-extrusion process the end of the
tubes [1820]; tube emerging from the extrusion press rst is referred to
106.6
106.1
MEAN DIAMETER (MM)
105.6
105.1
104.6
104.1
103.6
0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5 4.0 4.5 5.0 5.5 6.0 6.5
Axial Position Referenced to Outlet Rolled - Joint - m
Fig. 2.1.1. Typical prole of diameter from outlet to inlet along the length of a CANDU 6 pressure tube.
R.A. Holt / Journal of Nuclear Materials 372 (2008) 182214 185
300 4 60
28.6
3 48.22
280
-17
57.38
40
Strain - 10 -4
Flux 71.13
270 2
-1
30
260
-2
Temperature
1
250 20
240 0 10
0 1 2 3 4 5 6
Distance from the PT Inlet End - m
0
Fig. 2.1.2. Typical fast neutron ux and temperature proles from inlet to 0 10 20 30 40 50 60
outlet along a CANDU pressure tube. Time - kh
Fig. 2.1.4. Strain as a function of time for the fast neutron uxes shown
as the front end and the end emerging last is referred to as (in units of 1014 n m2 s1, E > 1 MeV) showing an initial transient strain
followed by a steady state rate, from Ref. [25].
the back end. The front ends of the tubes exhibit lower
yield and ultimate tensile strengths than the back ends.
In earlier reactors the pressure tubes were always experiments on small specimens [30] that the irradiation
installed in the same geographic orientation relative to creep rate changes with uence, and clear evidence that
reactor core, e.g., the back end of the tube at the west the growth rate does change [12], so reactor operators
end of the reactor. Since the coolant ow is in the reverse should remain vigilant.
direction in alternating channels, half the pressure tubes The design of the fuel channels accounts for stress rup-
then had their back ends at the outlet, and half had their ture/creep ductility and ow bypass. Based on data from
back ends at the inlet. This resulted in two types of diam- in-reactor experiments, 5% is considered to be a very
etral strain proles. Tubes with their back end at the outlet conservative limit with respect to creep rupture and creep
exhibited asymmetrical strain proles like that shown in ductility, Ells et al. [31], see Section 7. Although the mea-
Fig. 2.1.1, and tubes with their back end at the inlet exhib- sured diametral expansions are within the maximum value
ited a more symmetrical strain prole, Fig. 2.1.3. assumed in the analysis, lifetime management strategists
In later reactors tubes, were installed with their back are evaluating the need for increased inspections to pre-
ends at the outlet of all channels, to reduce the likelihood cisely quantify the variability in expansion. This will allow
of a failure mechanism called delayed hydride cracking more accurate assessments of eect of ow bypass on fuel
(DHC) at the rolled joints where the pressure tubes are cooling and the potential approach to fuel dry-out the
joined to the steel end-ttings [29]. In the most recently condition limiting the operating power of the reactor.
built reactors, this concern has been alleviated and the The variability of diametral strain is also important
tubes are installed with the back end at the inlet. because operating margin to fuel dry-out is based on the
After a small positive transient, Fig. 2.1.4, the diametral worst case. A new fuel design has been developed to ame-
strain rate at a given point along the pressure tubes appears liorate the eects of diametral creep on fuel cooling [32],
to reach a steady state, and, unlike the situation for elonga- which, if implemented, would delay any necessity to de-rate
tion, see Section 2.2, there is no evidence from power reac- reactors as a result of degraded operating margins.
tors that this rate changes with time throughout the life of
the reactor. There is some suggestion from test reactor
2.2. Axial elongation
0.012
Axial elongation is due to a combination of irradiation
Diametral strain after 117000
120 30
100 20
Elongation (mm)
80
Deflection - mm
10
60
0
40
0 150 300 450 600
20 -10
0 -20
-20
-30
0 2 4 6 8 10 12 14
25 2
Fluence (10 n/m ) -40
Distance From Inlet - m
Fig. 2.2.1. Elongation as a function of fast neutron uence (averaged
along the length of each pressure tube) for a CANDU 6 reactor. Fig. 2.3.1. Sag prole for a CANDU fuel channel after several years of
operation.
4.4
onies of misaligned a-grains, which result from the b- to
4.3 a-phase transformation during cooling after extrusion,
Fig. 3.2(b) [40]. The a-grains contain 0.61.0%Nb, a
4.2 slightly super-saturated solid solution which is thermally
stable because the transformation kinetics are sluggish [42].
4.1
Between many of the a-grains, there is a thin lm of b-
phase, perhaps 2050 nm thick, see Figs. 3.1 and 3.2. After
4
0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5 4.0 4.5 5.0 5.5 6.0 extrusion, this phase is metastable body centred cubic (bcc)
Axial Position Referenced to the Outlet End-Fitting - m b-Zr containing approximately 20%Nb, but after cold-
work and autoclaving, this phase has partially trans-
Fig. 2.4.1. Variation in wall thickness (maximum, average and minimum)
of a CANDU pressure tube with distance from the outlet end-tting. formed, through a complicated sequence, towards the equi-
librium phase distribution of a (<0.5%Nb) and bcc b-Nb
(95%Nb) and contains a combination of x (a metastable
The further development of these models and probabilistic hcp phase of intermediate Nb content) and b-Zr enriched
assessment of the likelihood of contact are now probably in Nb to 50% [43]. This partial transformation is recog-
the most important focus of on-going research. nizable by the internal structure of the b-phase observed
after autoclaving, but not immediately after extrusion,
2.4. Wall thinning Fig. 3.3.
Oxygen, which is deliberately controlled to give short
Creep and growth occur at constant volume, therefore term strength [28] is concentrated in the a-phase and
the increase in diameter and length correspond to a reduc- depleted in the b [40], although there is no technique that
tion in the wall thickness. Sag also contributes a small will give a quantitative assessment on such ne microstruc-
amount to the loss of wall thickness on the side opposite tures. The major impurity in Zr2.5Nb is Fe which is a
the centre of curvature. A typical wall thickness prole at b-stabilizer in Zr, and is primarily concentrated in the
mid-life is shown in Fig. 2.4.1. The design of the fuel chan- b-phase. Fe is also found at the aa grain boundaries [44].
nels accounts for the stress increase both due to diametral The dislocation structure in the a-phase arises mainly
expansion and due to wall thinning. Relative to the short from the cold-drawing process (27% reduction in area),
term strength, increased stresses due to diametral expan- and subsequent recovery during autoclaving [45]. It com-
sion and wall thinning are more than oset by the radiation prises both a dislocations, i.e., dislocations with a Burgers
hardening that occurs during service. The recently devel- vector lying in the basal plane of the hcp crystal, and c-
oped capability to measure wall thickness proles accu- component dislocations, i.e., dislocations with a compo-
rately, as shown in Fig. 2.4.1 allows a more accurate nent of their Burgers vector normal to the basal plane.
analysis of the diametral strain proles and elongation with The two types can be observed by transmission electron
the possibility of detecting variations in anisotropy along microscopy, Fig. 3.4 [46]. Using X-ray diraction [47] the
the length of the pressure tube. total dislocation is estimated as 34 1014 m2. and typi-
cally the c-component dislocation density is 1020% of
3. Microstructure and microchemistry of pressure tubes the total [22].
The anisotropic nature of the in-reactor deformation
The manufacturing route of Zr2.5Nb pressure tubes processes in pressure tubes results predominantly from
has varied slightly between the construction of Pickering the anisotropic hcp a-Zr crystal structure and the crystallo-
A (late 1960s) and Qinshan 1 and 2 (early 2000s), but the graphic texture developed during the extrusion process.
microstructure of the pressure tubes has remained reason- The anisotropy is mainly controlled by the orientation of
ably consistent. The basic microstructure and crystallo- the c-axis, or basal plane normal. This is the strong direc-
graphic texture arise during the extrusion process (for tion of the crystal [48]. A typical basal pole gure for a
summaries of the manufacturing route of pressure tubes pressure tube is shown in Fig. 3.5. The basal plane normals
see Refs. [28,39,40]). It comprises mainly hcp a-Zr grains are distributed in the radial/transverse plane and concen-
that are highly elongated in the axial direction of the tube, trated predominantly in the transverse direction [28]. This
as seen in the radial/axial plane, Fig. 3.1(a). In this view concentration tends to be higher at the front ends of the
they are generally between 0.2 and 0.5 lm thick and several tubes. Often there is a small concentration of basal plane
micrometer long. As seen in the radial/transverse plane normals in the axial direction of the tube at the front end
there are three types of grains [41]. Usually they are a associated with the presence of colonies of misaligned a-
few micrometer wide, and are predominantly aligned in grains [49], mentioned above. The basal plane texture is
the transverse direction but often curl around, often quantied by FR, FT and FA, the resolved fractions
Fig. 3.1(b), and a few are aligned in the radial direction, of basal plane normals in the radial, transverse and axial
188 R.A. Holt / Journal of Nuclear Materials 372 (2008) 182214
Fig. 3.1. Transmission electron micrographs from carbon replicas of a pressure tube showing: (a) elongated a-grains in the axial/radial section and
(b) curved attened a-grains in the radial/transverse section, from Ref. [41].
directions, respectively [50]. These quantities represent a tions have been established between the overall diametral
normalized average of a second-order tensor resolution strain [22] and elongation [34] of pressure tubes and micro-
into the tube directions of dilations along the c-axis for structural, chemical and manufacturing information.
all crystallographic orientations [51]. Typical values for The elongation rate of pressure tubes shows a decrease
pressure tubes are given in Table 3.1 [22]. with increasing Fe concentration, Fig. 4.1 [52]. A similar
Unless otherwise specied, the deformation characteris- correlation is seen between the rate of irradiation growth
tics described below pertain to material with the micro- and Fe concentration, Section 5.4. The elongation rate also
structural characteristics given above, and to operating appears to vary from one ingot to the next [53], Fig. 4.2,
conditions that are representative of the behaviour of pres- which could be attributable to ingot chemistry, or could
sure tubes in power reactors. be a manufacturing batch eect [34].
The diametral strain rate decreases with grain thickness,
4. Variability of pressure tube deformation Fig. 4.3, decreases as the distribution of basal plane nor-
mals becomes more pronounced in the transverse direction,
Within one reactor, the deformation rates of pressure Fig. 4.4, and decreases as the oxygen concentration (as
tubes can vary substantially once temperature, fast neutron analysed in the ingot) increases, Fig. 4.5 [22].
ux and tube orientation have been taken into account. In In all cases these correlations may be misleading because
the case of elongation, this variation is of the order of there are many potentially confounding variables.
1520% [33] and in the case of diametral strain the varia- The eect of grain size might be expected from the the-
tion can be of the order of 30% [22]. Further variations are oretical predictions of the eect of grain size on irradiation
seen from reactor to reactor, but these might be attributable growth in the transverse direction [54], see Section 5.6. The
to dierences in operating conditions. A number of correla- eect of texture is expected from its eect on both creep
R.A. Holt / Journal of Nuclear Materials 372 (2008) 182214 189
Fig. 3.2. Transmission electron micrographs from thin foils of a pressure tube showing: (a) transversely oriented a-grains in the radial/transverse section
and (b) a radially oriented a-grain in the radial/transverse section. Both micrographs show some Widmanstatten a-grains (centre in (a) and upper right in
(b)), from Ref. [41].
Irradiation growth is a shape change induced by any The growth behaviour of Zr2.5Nb pressure tube
energetic radiation that causes displacement damage dis- material in the axial and transverse directions at 550 K is
190 R.A. Holt / Journal of Nuclear Materials 372 (2008) 182214
Fig. 3.3. Transmission electron micrographs from thin foils of a pressure tube showing: (a) undecomposed b-phase before autoclaving and (b) partially
decomposed b-phase after autoclaving for 24 h at 673 K, both in radial/axial section, from Ref. [43].
Fig. 3.4. Transmission electron micrographs from thin foils of a pressure tube showing: (a) a-dislocations b 1=3h1 1 2 0i and (b) c-component
dislocations b 1=3h1 1
2 3i, both in radial/transverse section, from Ref. [46].
R.A. Holt / Journal of Nuclear Materials 372 (2008) 182214 191
A 1.6
Wolsong PT
1.2
0.8
11
1 2 3 45 7 9 0.6
R + T
0.4
0.1 0.2 0.3 0.4 0.5 0.6
Mean Grain Width - m
Fig. 4.3. Correlation between peak diametral strain rate of pressure tubes
in operating reactors and grain thickness, from Ref. [22].
Maximum 12
2
Fig. 3.5. Typical basal pole gure of a cold-worked Zr2.5Nb pressure 1.8
1
14
0.8
12
0.6
10 0.4
8 0.2
0
6
0 0.1 0.2 0.3 0.4 0.5
4 F T - FR
2
Fig. 4.4. Correlation between peak diametral strain rate of pressure tubes
0 in operating reactors and the dierence between texture parameters
0 500 1000 1500 2000 2500 3000
FT FR, from Ref. [22].
Iron Content - ppm
120 1.5
Total elongation (mm)
399149
100
398757 1
80 399012
60 0.5
40
20
0
800 1000 1200 1400 1600
0 Oxygen Concentration - ppm
0 2 4 6 8 10 12 14
Fig. 4.5. Correlation between peak diametral strain rate of pressure tubes
Fluence (x10 25 n/m 2 ) in operating reactors and the ingot oxygen analysis for two reactor types,
from Ref. [22].
Fig. 4.2. Elongation as a function of fast neutron uence (averaged along
the length of each pressure tube) for tubes made from three dierent ingots
in a CANDU 6 reactor.
transverse direction of about 0.02%. Subsequently, the
growth is relatively at, or slightly negative in the axial
illustrated for low and high fast neutron uence in Figs. direction for a fast uence of 11.5 1025 n m2,
5.1.1 [57,58] and 5.1.2 [12]. There is an initial rapid increase E > 1 MeV, and establishes a relatively steady negative rate
in length in the axial direction and decrease in length in the in the transverse direction after about 0.5 1025 n m2,
192 R.A. Holt / Journal of Nuclear Materials 372 (2008) 182214
0.15 1.5
Axial
0.1 1 Radial
Growth Strain - %
Growth Strain - %
Transverse
Volume
0.05 0.5
0
0
-0.05
-0.5
-0.1
-1
-0.15
0 1 2 3 4 5 -1.5
-25 -2 0 5 10 15 20
Neutron Fluence x 10 - n.m , E>1MeV
-25 -2
Neutron Fluence x 10 n.m , E>1MeV
Fig. 5.1.1. Growth strain as a function of fast neutron uence for cold-
worked Zr2.5Nb in DIDO at a fast neutron ux of 6 1017 n m2 s1, Fig. 5.1.3. Growth strains in three dimensions as a function of fast
E > 1 MeV, from Ref. [58]. neutron uence for Zr2.5Nb pressure tube material irradiated at 520 K in
Osiris at 2 1018 n m2 s1, E > 1 MeV, from Ref. [59]. Note several
points in the range 913 1025 n m2 are thought to be erroneous.
1
0.8 553 K the strain rates in all three directions evolve with fast u-
0.6
ence, Fig. 5.1.3 [59], and the strain in the thickness direc-
Growth Strain - %
Axial 583 K tion can be inferred to be the negative sum of the strains
0.4 in the axial and transverse directions.
0.2
0.12 0.8
Osiris
Bruce A
0.1 DIDO 0.6
NRU
Growth Strain %
Growth Strain - %
0.08
0.4
0.06
0.2
0.04 Medium Fe
0 Low Fe
0.02 High Fe
-0.2
0 520 540 560 580 600
0 0.2 0.4 0.6 0.8 1 1.2 1.4 Temperature - K
-25 -2
Neutron Fluence x10 , n.m , E>1MeV
Fig. 5.3.2. Growth strain in the axial direction of cold-worked Zr2.5Nb
Fig. 5.2.1. Growth strain in the axial direction of cold-worked Zircaloy-2 pressure tube material at a fast neutron uence of 1 1026 n m2,
pressure tube material at 553 K in DIDO at 6 1017 n m2 s1, E > 1 MeV, as a function of temperature, from Ref. [12].
E > 1 MeV; 553 K in Osiris at 2 1018 n m2 s1, E > 1 MeV, and in a
carrier bundle in a CANDU reactor at 2 1017 n m2 s1, E > 1 MeV,
from Ref. [60].
0
Medium Fe
Typical irradiation growth curves for pressure tube -0.2
Low Fe
materials at 553 and 583 K are shown in Fig. 5.1.2, in High Fe
which the magnitudes of the positive axial and negative -0.25
transverse growth strains both decrease with increasing 540 560 580 600
temperature. Over a temperature range of 330623 K, the Temperature - K
growth rate of Zr2.5Nb pressure tube material in the axial
Fig. 5.3.3. Growth strain in the transverse direction of cold-worked Zr
direction decreases with temperature, Fig. 5.3.1 [58,61,62]. 2.5Nb pressure tube material at a fast neutron uence of 1 1026 n m2,
Over the temperature range of pressure tube operation, the E > 1 MeV, as a function of temperature, from Ref. [12].
same behaviour is seen for a variety of dierent pressure
tube materials, Fig. 5.3.3, the curves being displaced for
materials with dierent Fe concentrations (see Section 0.15
5.4). The (negative) magnitude of the transverse growth
553 K
rate also decreases with temperature, for a range of tubes, 0.1
Growth Strain - %
623 K
0.05
10
Strain Rate x 10 29 m 2n-1 (E>1 MeV)
5 -0.05
-0.1
0 1 2 3 4 5
-25 -2
0 Neutron Fluence x 10 , n.m , E>1MeV
Fig. 5.3.1. Eect of temperature on the growth rate of cold-worked Zr Fig. 5.3.4. When the parameters of quadratic equations t-
2.5Nb pressure tube material, from Ref. [61]. ted individual growth curves are plotted as a function of
194 R.A. Holt / Journal of Nuclear Materials 372 (2008) 182214
temperature, it appears that the temperature aects primar- provide recombination sites for vacancies and interstitials.
ily the initial growth rate, but has less eect on the rate of Also, its presence at aa grain boundaries [44] could inu-
acceleration. ence their role as sinks. Finally, Fe changes the volume
When the temperature is changed during a growth test, fractions of a and b during extrusion, and could thus have
there are signicant transients, Fig. 5.3.4, and the growth an indirect inuence through the texture.
rate does not immediately re-establish itself at the expected
rate for the new temperature [58]. Analysis of the anisot- 5.5. Eect of crytallographic texture
ropy of these transients suggested that there may be a long
lasting eect of the dislocation microstructure developed at Based on the growth behaviour of a typical pressure
the earlier irradiation temperature. This could be impor- tube material, Section 5.1, it can easily be inferred that,
tant in future reactors that are designed to load follow with on the crystalline level, growth comprises, to some degree,
signicant changes in temperature over the power range. shrinkage along the c-axis and expansion along the a-axis
of the hcp crystal. Growth tests on small diameter tubes
with two dierent crystallographic textures irradiated to
5.4. Eect of Fe concentration
high fast neutron uence in the Osiris reactor in France
clearly illustrate this [17]. Fig. 5.5.1 shows the crystallo-
Based on the fact that Fe has a signicant eect on the
graphic textures of the two types of tubes referred to as
diusional characteristics of vacancies in Zr [63,64], and
FS (fuel sheathing) and MPT (micro-pressure tube), and
the observation that the elongation rates of pressure tubes
Table 5.5.1 gives the microstructural parameters.
correlate with Fe concentration (see Section 4), pressure
Fig. 5.5.2 illustrates the growth behaviour in two directions
tubes with dierent Fe concentrations were chosen for a
for both types of tubes at 553 K. Both FS and MPT mate-
long term growth experiment in the Osiris reactor in
rial grow a similar amount in the axial direction, in which
France [12,52]. These showed a clear trend, with the mag-
there are very few basal plane normals. The MPT material
nitude of the irradiation growth rate in either direction
exhibits a much greater shrinkage in the transverse direc-
decreasing with increasing Fe concentration. Fig. 5.4.1
tion than FS material, corresponding to the much higher
shows growth curves for pressure tube materials at a nom-
concentration of basal plane normals in the transverse
inal temperature of 553 K with two dierent Fe concentra-
direction in MPT material than in FS material.
tions. Fig. 5.3.3 shows the eect of Fe on the axial growth
At the single crystal level, this behaviour corresponds to
rate as a function of temperature, and Fig. 5.3.4 the eect
a net accumulation of vacancies at defects (dislocations,
of Fe on the transverse growth rate as a function of temper-
dislocation loops) lying on the basal plane and an accumu-
ature. As in the case of temperature, the initial rate is more
lation of self-interstitial atoms (SIAs) at defects perpendic-
sensitive to Fe concentration than the acceleration in the
ular to the basal plane, as originally proposed by Buckley
growth rate with increased uence, Fig. 5.3.4. The eect
[65]. As seen in the next section, however, there are other
of Fe has not yet been satisfactorily explained. During irra-
components to the behaviour which is clearly modied by
diation it is dispersed into the a-phase [44], but whether it
very ne elongated grain structures. In addition, we now
remains in solution or exists as sub-microscopic precipi-
know that the dislocation structures in dierent crystal ori-
tates is not known. As a solute, it may aect the vacancy
entations is dierent [12] and this will no doubt aect the
diusion characteristics [63], while as a precipitate, it might
growth anisotropy [66].
1.2
5.6. Eect of dislocation density and grain size
1 Low Fe (<500ppm)
High Fe (~1000ppm)
There are no growth data for Zr2.5Nb pressure tube
0.8 material in which the initial dislocation density2 has been
Longitudinal
Growth Strain - %
A A
Micro PT Fuel Sheathing
1 1
3 2
3 4
2 3 4 5 6 7 8 R + T
R + T
Table 5.6.1
Microstructural details and long term irradiation growth rates at 553 K of Zr2.5 Nb pressure tube materials modied to vary grain size, grain shape and
dislocation density [61]
Material Dislocation density FR FT FA Grain aspect Grain Axial growth Transverse
designation ( 1014 m2) ratioa thicknessa (lm) rateb growth rateb
AR 4.2 0.36 0.61 0.03 1520 0.32 3.2
SR 1.8 0.36 0.61 0.03 1520 0.32 0.8
CW 4.7 0.28 0.64 0.08 2.3 1.5 3.7
R1 2.4 0.40 0.56 0.03 1520 0.25 2.1 0.7
R2 4.8 0.37 0.59 0.03 510 0.34 3.2 1.4
R3 2.7 0.36 0.61 0.03 510 0.37 2.3 1.5
D1 4.5 0.35 0.62 0.04 1520 0.31 2.7 2.2
a
Grain length in the axial direction/grain thickness in the radial direction.
b
Averaged in units of 1029 m2 n1 between 2 and 8 1025 n m2, E > 1 MeV.
4 6
-1
3
-1
2
2
29
3
29
2
Growth Rate x10
1
1
0
0 0.5 1 1.5 2
-1
0
0 1 2 3 4 5 6
-2
-14 -2
Dislocation Density x 10 -m Grain Thickness - m
Fig. 5.6.1. Eect of dislocation density on growth rate for cold-worked Fig. 5.6.3. Eect of grain thickness on the growth rate for cold-worked
Zr2.5Nb with a grain thickness of 0.310.37 lm. Zr2.5Nb corrected to a dislocation density of 4 1014 m2, to a grain
aspect ratio of 15:1 and an FA of 0.03.
Curiously, there is no discernable eect of pre-extrusion Irradiation creep is more dicult to study than irradia-
b-quenching of the material [52], an operation expected to tion growth because any shape change that occurs under an
rene the grain size. No microstructural data were applied stress incorporates some components of the shape
reported, and possibly the tubes studied had grain sizes change that occurs without stress or due to thermal creep.
R.A. Holt / Journal of Nuclear Materials 372 (2008) 182214 197
For practical purposes, the irradiation growth strain is sim- ponent of growth which also has a linear dependence on
ply subtracted from the total strain, the dierence being fast ux (Section 5.2) and also includes thermal creep. Note
dened as creep. However, on a microscopic level, the that if thermal creep were a signicant contributor to the
processes associated with the growth strain may be dier- total strain rate (e.g., as the temperature increases) the total
ent with and without stress depending upon the mechanism strain rate would exhibit a ux exponent, n < 1 even when
(see Section 10). The issue of the thermal creep is even more the ux dependence of irradiation creep was linear.
complicated because the creep rate without a fast neutron
ux is not relevant to the in-ux behaviour, since it is sup- 6.2. Eect of fast neutron uence
pressed by radiation damage [14,15,25] as will be discussed
in Section 7.2. Frequently, it is found that the latter is small Typically, if diametral strain is plotted against time
relative to the radiation-induced component of creep and or fast neutron uence for a pressure tube irradiated at fast
in many cases, to a rst approximation, can be ignored. neutron uxes typical of power reactors (2
1017 n m2 s1, E > 1 MeV) with an internal pressure, there
6.1. Eect of fast ux is a small positive intercept at the abscissa, Fig. 6.2.1
[15,25], suggesting a transient or primary creep strain.
The dependence of irradiation creep of Zr alloys on fast The transverse irradiation growth strain is negative and
neutron ux (displacement damage rate) is often expressed exhibits only a small transient over the rst 1 1025 n/m2,
as a power law, i.e., E > 1 MeV [56], Fig. 5.1.1, so this transient must be attrib-
uted mainly to creep. A similar transient is also observed at
e_ ic / /n ; 6:1:1
the edge of the reactor core where the irradiation creep is
where / is the fast neutron ux and n is the ux exponent. negligible [25]. Pressurized micro-pressure tube specimens
For pressure tubes at reactor operating temperatures the irradiated at very high ux (2 1018 n m2 s1, E >
fast ux dependence is generally accepted to be approxi- 1 MeV) do not exhibit this intercept [17], presumably
mately linear, i.e., n 1 [15]. because the irradiation creep strain is relatively much lar-
Although no similar experiments exist for Zr2.5Nb, the ger, and hence this initial transient is likely attributable
linear sensitivity of irradiation creep to displacement dam- to thermal creep.
age has been clearly demonstrated by proton irradiation in We have recently shown, however, that over the long
hot-rolled and annealed Zircaloy-2 plate at 553 K [72], term (16 1025 n/m2, E > 1 MeV) the creep rate can vary
Fig. 6.1.1. slowly [30], as shown for example in Fig. 6.2.2. The change
The eect of fast ux is most graphically demonstrated in strain rate may be positive or negative and its sign and
for Zr2.5Nb pressure tubes by the diametral strain proles magnitude depend upon temperature, stress and direction
of pressure tubes in power or test reactors, and examples of and probably relates to long term evolution of the micro-
which are shown in Fig. 2.1.3. Here the strain follows the structure, see Section 9.
prole of the fast ux through the core (although these
may be skewed because of the temperature gradient and/ 6.3. Eect of temperature
or end-to-end eect). The diametral strain includes a com-
From uniaxial in-reactor creep tests at high temperature
10 (>600 K), stress relaxation tests at low and intermediate
5
Axial MPT
4 Transverse MP
-
Creep Rate x10 h
Axial FS
6
Creep Strain %
3 Axial MPT
1
2
0
0 5 10 15 20
0.1 -1
0.1 1 10 -25 2
Neutron Fluence x 10 - n/m , E>1MeV
7 -1
Dose Rate x10 dpa.s
Fig. 6.2.1. Creep strain (total strain minus growth strain) as a function of
Fig. 6.1.1. Creep rate as a function of damage rate for cold-worked neutron uence for small pressurized tubes (Section 5.5) irradiated at
Zircaloy-2 pressure tube material irradiated with 4 MeV protons, from 553 K in Osiris with a nominal stress of 160 MPa at a neutron ux of
Ref. [72]. 2 1018 n m2 s1, E > 1 MeV, from Ref. [17].
198 R.A. Holt / Journal of Nuclear Materials 372 (2008) 182214
160 MPa
0.12 For the temperature range 555 K to 588 K this expres-
0.1 sion predicts an increase in strain rate of 56%, very close
122 MPa
0.08
to the variation of creep compliances later observed in
the axial and transverse directions of pressurized capsules
0.06 82 MPa
of cold-worked Zr2.5Nb irradiated in a fast neutron ux
0.04 of 2 1018 n m2 s1, E > 1 MeV, i.e., 53% and 49%,
43 MPa
0.02 respectively [75], Table 6.3.1 and Fig. 6.3.2. As the temper-
0 ature is reduced, Eq. (6.3.2) becomes at at about 450 K.
0 5 10 15 20
-25 -2
Neutron Fluence x 10 - n.m , E>1MeV 6.4. Eect of stress
Fig. 6.2.2. Variation in steady state creep rate with neutron uence
for small pressurized tubes irradiated at 553 K in Osiris at 2 At pressure tube operating temperatures, the stress
1018 n m2 s1, E > 1 MeV, from Ref. [30]. dependence of irradiation creep of pressure tube materials
is approximately linear, for stresses up to about 200 MPa,
i.e.,
temperature (310570 K) and from the asymmetry of the
diametral strain proles caused by the coolant temperature e_ ic / rn ; 6:4:1
changes in pressure tubes, we have previously inferred a
where r is stress and n 1. The early evidence for this came
general temperature dependence of the in-reactor creep
from full size pressure tubes irradiated in the NRU Reactor
rate. This is at at low temperatures with a transition in
at Chalk River Laboratories with zones of dierent stress
the operating temperature range of pressure tubes in power
created by machining to dierent wall thicknesses [76],
reactors (520580 K) to a relatively steep temperature
Fig. 6.4.1. These tests typically ran for a relatively short
dependence at higher temperatures (P600 K) [15],
time, typically 10 000 h at uxes of about 2 1017 n
Fig. 6.3.1. In the high temperature range the temperature
m2 s1, E > 1 MeV, or a fast uence of 1 1025 n m2,
dependence can be expressed approximately by [14]
E > 1 MeV. Hence the contribution of growth was small
e_ total / expT act =T ; 6:3:1 compared to the total strain (see Fig. 5.1.1), and was not
detected. Subsequently, stress relaxation of bent beams
where e_ is the strain rate, T the absolute temperature and [77,78] supported the observation of linear stress depen-
Tact is the activation temperature and has a value of
around 17 000 K. This is about the value for thermal creep Table 6.3.1
in this temperature range, variously reported as 15 000 Creep compliances as a function of temperature for micro-pressure tube
specimens irradiated in Osiris at 2 1018 n m2 s1, E > 1 MeV
25 000 K [73]. Possibly in-reactor creep is entirely thermal
at these temperatures. Temperature Axial creep Transverse creep
(K) compliance compliance
In the low to intermediate temperature range (310 (m2 n1 MPa1) (m2 n1 MPa1)
580 K) we have inferred a temperature dependence of irra-
555 0.55 1030 0.88 1030
diation creep given by [74] 588 0.84 1030 1.16 1030
Temperature - C 20
2
583K Transverse
--1
15 583K Axial
Log Strain Rate - h
553K Transverse
-6.00
553K Axial
10
-1
2
5
-29
60C
-7.00
Strain Rate x 10
-5
-8.00 -10
1.4 1.6 1.8 2 2.2 0 20 40 60 80 100 120 140 160 180
3 -1
Inverse Temperature x 10 K Hoop Stress - MPa
Fig. 6.3.1. Temperature dependence of the transverse strain rate of cold- Fig. 6.3.2. Variation of strain rate in the transverse and axial directions
worked Zr2.5Nb pressure tubes and pressure tube material, from Ref. with stress for Zr2.5Nb micro-pressure tube material irradiated at 553 K
[15]. and 583 K in Osiris at 2 1018 n m2 s1, E > 1 MeV, from Ref. [75].
R.A. Holt / Journal of Nuclear Materials 372 (2008) 182214 199
1000
100
Stress Exponent - n
10
Fig. 6.4.1. Variation in accumulated strain with elevation for a Zr2.5Nb 0.1
pressure tube in the core of NRU. The wall thickness is varied to give the 0 200 400 600 800
stress indicated and the peak neutron ux is 2 1017 n m2 s1, Applied Stress - MPa
E > 1 MeV, from Ref. [76].
Fig. 6.4.3. Stress exponent of in-reactor creep of cold-worked Zr2.5Nb
pressure tube material as a function of applied stress, from Ref. [79].
dence. After a small transient the logarithm of stress de-
cayed linearly with fast uence or time indicating linear
stress dependence of both the axial and diametral creep 3
rates, Fig. 6.4.2.
Tests on pressurized capsules irradiated to very high fast 2.5
uences (1.6 1026 n m2, E > 1 MeV) continue to show out of flux
Stress Exponent, n
Transverse
passed through the shielding of the reactor (thermal creep
only).
-1
- m .n .MPa
developed a methodology for separating irradiation creep
and growth in pressure tube deformation based on calcula-
-1
2
tions of the expected anisotropy from the texture and on
the elongation and diametral strain rates of pressure tubes
30
Creep coefficient x 10
in power reactors. This showed that creep made a substan-
tial contribution to the elongation of pressure tubes and
0.20
that growth reduced the diametral strain rate. We now
know that about 33% of the elongation rate is due to irra-
diation growth and 67% due to irradiation creep while the
contribution to diametral strain rate of creep is reduced
1
about 25% by growth [61].
1 10
The eect of texture on the biaxial deformation behav- -14 -2
Dislocation Density x 10 -m
iour has since been clearly demonstrated in tests on inter-
nally pressurized tubes of two dierent textures Fig. 6.6.1. Irradiation creep rate measured by stress relaxation as a
[17,52,75]. Some results are shown in Fig. 6.2.1. Here the function of pre-irradiation dislocation density. Irradiation in NRU at
irradiation growth has been subtracted from the total 2 1017 n m2 s1, E > 1 MeV and 573 K, from Ref. [83].
strain rate and only the irradiation creep is shown. The cor-
responding pole gures are shown in Fig. 5.5.1 and the tex- 50% over a grain size range of 0.370 lm, but there are
ture parameters are given in Table 5.5.1. many potentially compounding factors. There are no stud-
Here it is clear that a material with a strong transverse ies in which the creep rate has been measured as a function
texture, similar to that of a pressure tube, exhibits a rela- of grain size alone. The creep rate has been shown, how-
tively low transverse creep rate and a high axial creep rate, ever, to increase from front to back of pressure tubes, coin-
whereas a material with a more radial texture exhibits a rel- ciding with a reduction of grain size from about 0.4 to
atively high transverse creep rate and a small negative axial 0.3 lm and also with an increase in dislocation density
creep rate. Note that the axial component of texture is and less transverse texture [22], see Section 3. Also the
small in both cases, and the axial creep rate depends upon diametral strain rate of pressure tubes increases with
the distribution of basal plane normals in the radial/trans- decreasing grain size, Fig. 4.3, an observation which might
verse plane. Factors other than texture are believed to also be attributed to a decrease in the absolute irradiation
inuence the anisotropy however, in particular a correla- growth rate in that direction [54].
tion of the dislocation substructure with crystal orientation
[12,66] and possibly the interaction of the hcp a-phase with
the bcc b-phase [82]. 7. Thermal creep
6.6. Eect of dislocation density Thermal creep contributes little to the peak diametral
strain of a pressure tube or to elongation [14]. However
Causey et al. [77,83] showed, using stress relaxation thermal creep contributes the majority of the deformation
tests, that the irradiation creep rate is weakly sensitive to at the ends of the channel where the fast neutron ux is
the initial (as-manufactured) dislocation density, i.e., low, but the bending moment in the pressure tube is high.
e_ ic / qp , where q is the dislocation density and p has a value It may thus contribute signicantly to controlling the sag
of 0.23, Fig. 6.6.1. Within the experimental variations prole of the pressure tube and the potential for pressure
this is comparable to the value (q 0.16) found for Zirca- tube-to-calandria tube contact. Also thermal creep may
loy-2 pressure tubes by extraction of creep and growth contribute signicantly to the strain at high stresses, for
components from elongation and diametral strain data example in the vicinity of a crack tip, and hence assist
[67]. Like the growth, the creep rate and anisotropy prob- the relaxation of stresses that can potentially cause failure
ably depend on the mixture of dislocation types and their by the process of delayed hydride cracking [84,85].
distribution amongst the dierent crystal orientations as The thermal creep of Zr alloys at about 570 K is compli-
well as the overall density [66]. cated by the existence of strain aging [26,27], which can
produce transient increases in strain rate during steady
6.7. Eect of grain size state creep and anomalous stress sensitivity in certain tem-
perature and strain rate ranges. Strain aging in Zr is
The eect of grain size (the thickness of the attened, believed to be associated with solute eects.
elongated a-grains in pressure tubes) on irradiation creep
has not been clearly established. Causey et al. [77] showed 7.1. Thermal creep at aws
a very weak grain size dependence of the in-reactor creep
rate for a variety of Zr alloys over a very wide grain size The stress concentrations at aw tips in pressure tubes
range, the creep rate increasing with grain size by about can initiate delayed hydride cracking under certain
R.A. Holt / Journal of Nuclear Materials 372 (2008) 182214 201
-1
Transverse Strain Rate x 10 - h
tope concentration. Often the aws will be present for many
8
operating hours before the conditions exist which could ini- 20
tiate cracking. In this situation the peak stress at the aw tip
can relax by creep. The creep rate is fastest at the tip of the 15
500
400 unknowns in the area of pressure tube deformation.
300
200
100
0 8. Creep ductility
-100
-200 The statement by Ells et al. [31] that an operating limit
-300
-400
of 5% circumferential expansion seems to be very conserva-
0 2 4 6 8 10 tive is based on the argument, rst put forward by Wood-
Distance (mm) ford [87,88] that the total elongation of materials that fail
Fig. 7.1.1. Finite element calculation showing the relaxation of peak stress in a ductile manner under tension is inversely related to
at a aw in cold-worked Zr2.5Nb pressure tube material after 60 h at the stress sensitivity of the strain rate (the inverse of the
573 K, from Ref. [23]. exponent n in Eq. (6.4.1)), Fig. 8.1. Superplastic materials
202 R.A. Holt / Journal of Nuclear Materials 372 (2008) 182214
10000 quoted above is based on the fact that these tests are likely
to be very conservative. One might debate this conclusion:
Fig. 9.1. Electron micrographs showing the a dislocation structure of Zr2.5Nb pressure tube material, (a) before and (b) after irradiation at 543 K to a
neutron uence of 1.1 1026 n m2, E > 1 MeV. Note the high density of loops in (b), from Ref. [12].
10
causing an initial apparent reduction (based on X-ray line
7
Fig. 9.3. Electron micrographs showing the c-type dislocation structure of Zr2.5Nb pressure tube material, (a) before and (b) after irradiation at 543 K to
a neutron uence of 1.1 1026 n m2, E > 1 MeV. Note loop nucleated on a screw dislocation at arrow in (b), from Ref. [12].
204 R.A. Holt / Journal of Nuclear Materials 372 (2008) 182214
state condition depends upon temperature and fast ux rium is reversed and the b has about 40%Nb. At the inlet
[93]. At the high ux region towards the inlet end and in end there is a very slow progression towards the equilib-
the middle of the core, the transformation towards equilib- rium state and at the outlet end this progression is more
rapid. Fig. 9.6 shows a compilation of data for uences
of >2 1025 n m2, E > 1 MeV.
The Fe which is initially concentrated in the b-phase is
dispersed by irradiation and can no longer be detected
within the b or in the a-grains because its average concen-
tration is below the limit of detection (0.15%) [44]. Fe is
still found at the aa sub-boundaries however at approxi-
mately the same level as before irradiation.
-1
contraction or dilation in the direction of the boundary
-s
1 microns
normal. 6 0.3 microns
11
Axial Growth Rate x 10
0.15 microns
Two conditions are necessary for a macroscopic strain
4
to occur from the disposition of point defects at sinks.
First, the sinks must experience net uxes of point defects, 2
i.e., the ux of one species of point defect must, over time
0
exceed the ux of the species of the opposite sign. Obvi- 0 1 2 3 4 5 6
ously, if a particular sink experiences at net ux of one spe- -2
cies, some other sink must experience a net ux of the other
-4
species. Second, the orientation distribution of the sinks
that experience net uxes of the dierent species of point -6
defect must be dierent. Network Dislocation Densityx10
-14
-m
-2
0.5 6 microns
exhibit anisotropic diusion in Zr a natural consequence 0
of the hcp crystal structure, and that the diusional aniso-
-0.50 1 2 3 4 5 6
tropies of the two species of defects are dierent, a natural
-1
consequence of the dierent relationship of the two defects
to the hcp lattice. This provides a very powerful driving -1.5
and the applied stress elevates the stress in crystals of a cer- Detailed mathematical treatments of the models for
tain orientation above the yield stress causing them to creep are given in the Refs. [98110].
yield. Continued growth causes continued yielding in a
direction that is biased by the applied stress. This model 11. Modelling pressure tube deformation
has generally been ignored in recent times, but has not been
discounted by experimental facts. 11.1. The need for models
The climb-plus-glide model [103] is an extension of the
dislocation creep model [104] of thermal creep in which dis- Models are required to predict the deformation of mod-
locations are able to bypass obstacles by climb due to the ied pressure tubes operating in new reactor designs under
absorption of thermally generated vacancies. The strain conditions dierent from those that have been experienced
producing step is glide. Under irradiation, a net ux of previously or to predict the future deformation of pressure
either vacancies or interstitials to a given dislocation will tubes in existing power reactors for the purposes of plant
allow it to bypass obstacles and glide. In the late 1970s this life management (PLiM).
model was supported by an experiment in which the neu- In the case of new reactor designs the operating condi-
tron ux to a creeping specimen was turned on and o tions, ux, temperature, coolant pressure, may be more
by moving the creep rig in and out of reactor [105]. A posi- severe so that the thickness of the tube must be adjusted.
tive strain transient was seen in both cases, even though on Also, one may want to take advantage of the knowledge
initiating irradiation, the dislocations in the specimen of the eects on deformation of microstructural, chemical
would experience a net ux of SIAs corresponding to the and manufacturing variables to improve the deformation
build up of a vacancy super-saturation, while on terminat- behaviour in order to achieve a satisfactory pressure tube
ing the irradiation a net ux of vacancies would be life in the new design. An example of such a new design
expected as the super-saturation decayed. This result has is the 1000 MWe class Advanced CANDU Reactor
never been explained by another mechanism. A modica- (ACR 1000 [16]) which has higher coolant temperatures
tion of this model is Gittis I-creep model [106], in which and pressures for improved thermodynamic eciency,
there is coordinated movement of arrays of dislocations and higher channel powers for increased average power
by glide after climb. density of the core.
More recently Semenov and Woo [107] have developed In the case of PLiM, a general algorithm for managing
an analysis of the stochastic nature of displacement cascade the life of the pressure tubes in a CANDU reactor is as fol-
damage in both time and space, show that a net ux of lows [7]:
point defects to dislocations may not even be necessary
for them to surpass obstacles and glide, given that the uc- plan maintenance based on predictions using models
tuations in the defect uxes of the two species are large based on R&D and surveillance data;
enough. monitor on-going changes to verify predictions/modify
SIPA [106,108110] assumes a bias of the ux of point models;
defects to dislocations as a function of the orientation of disposition out-of-design conditions, e.g., aws and
the Burgers vector with respect to the applied stress. Dislo- contact of PT with CT (this could involve removal of
cations whose Burgers vectors are aligned with the tensile tubes);
stress experience a net ux of SIAs. By default, those continued R&D including end-of-life testing to improve
aligned with a compressive stress experience a net ux of models;
vacancies. Any deviatoric stress tensor will induce a bias. modify maintenance plans accordingly.
This bias was initially attributed to the elastic interac-
tions of the point defects with and the strain elds of the In many cases, it may be sucient simply to extrapolate
dislocations in a stress eld [100]. The point defects are data from previous inspection campaigns, for example, the
considered as inclusions with elastic properties dierent elongation of each pressure tube in a CANDU 6 reactor
from the matrix. The key feature for SIPA to be viable is can be measured every time that the fuelling machine refu-
that the SIA must to exhibit an eective shear modulus less els that channel. Here a linear extrapolation of the data to
than that of the matrix while the vacancy exhibits a shear the next maintenance outage may be sucient, and for
modulus similar to that of the matrix. This might not longer term planning it may be simply a matter of know-
always be the case. Another possibility is that the disloca- ing how to extrapolate the data (e.g., a quadratic
tions are not perfect sinks (as is often assumed in calcula- equation).
tions of creep and growth) but that there is a barrier to In other cases, there is no alternative but to use a model.
absorption. This barrier may then be a function of stress This is the case for spacer location and repositioning
and dierent for interstitials and vacancies [100]. Finally (SLAR)[37], the objective is to prevent contact of the hot
there is the concept that the anisotropy of point defect pressure tube with the cold calandria tube late in life when
migration is stress dependent [98], so the applied stress the deuterium concentration of the pressure tubes has
modies the DAD eect. This is referred to as SIPA_DAD increased to reach a critical level. In earlier CANDU reac-
or elasto-diusion (ED). tors the spacers, helical springs circling the pressure tube to
R.A. Holt / Journal of Nuclear Materials 372 (2008) 182214 207
centre it in the calandria tube, Fig. 1.1.1, were loose and aspect of such a model is the dependence of the anisotropic
were found to move during service [38]. This caused the deformation behaviour on the multi-axial stress tensor.
rupture of a Zircaloy-2 pressure tube in the Pickering Unit
2 reactor in 1983 as a result of pressure tube sagging into 11.2. Models for anisotropic creep and growth
contact with the calandria tube and the formation of zirco-
nium hydride blisters on the outside of the pressure tube at To describe the deformation behaviour of pressure tubes
the line of contact [29]. under a multi-axial stress state, an anisotropic deforma-
At that time, there were 20 reactors constructed or in- tion equation is required for anisotropic creep and growth
service with the loose spacer design. Fortunately 18 of these of the material. Combined with an equivalent equation for
units had Zr2.5Nb pressure tubes which exhibit a much the calandria tube, such an equation can then be used as
lower deuterium pick-up rate than Zircaloy-2. The two input to a nite element model to predict the deformation
reactors with Zircaloy-2 tubes were immediately shut down of the fuel channel, and in particular the sag and the poten-
for retubing, the spacers for new reactors were changed to tial for pressure tube-to-calandria tube contact. The sim-
a tight-tting design [38], and a maintenance procedure plest anisotropic formulation for creep is that derived by
called SLAR was developed for the 18 reactors with loose Ross-Ross et al. [76] from Hill [111]. Such an equation con-
spacers and Zr2.5Nb tubes. tains three independent anisotropy parameters, and thus
The response of the horizontal pressure tube-calandria requires the measurement of three independent deforma-
tube assembly to the weight of the fuel and coolant is an tion rates under at least two dierent stress states. The
elastic deection several millimeter as a result of the bend- parameters for such a model cannot, therefore, be derived
ing moment. During operation a permanent sag is devel- solely from the elongation and diametral strain data from a
oped due to irradiation creep of both the calandria tube pressure tube. Because the stress exponent n 1 in Eq.
and the pressure tube a process referred to as creep-sag. (6.4.1), the expressions derived by Ross-Ross et al. are con-
The annealed Zircaloy-2 calandria tube exhibits a much sistent with the polycrystalline approaches described
higher resistance to creep-sag than the pressure tube so in below. However, the polycrystalline models allow assump-
the rst few years of operation the pressure tube sags to tions about the deformation mechanisms to be substituted
transfer most of the load of fuel and coolant to the calan- for measurements.
dria tube through the spacers [18]. Thereafter the gross sag The rst anisotropic deformation model for pressure
of the assembly is controlled by the calandria tube and the tubes [75] did not separate irradiation growth, which had
pressure tube properties determine the rate at which the not yet been observed, from the total deformation rate
pressure tube approaches contact with the calandria tube which was treated entirely as creep. The rst deformation
between the spacers [19]. If the spacers are displaced, this equations separating creep and growth were developed in
may happen before the end of the design life and there is the late 1970s [51,67,74]. The anisotropic eects of texture
a potential for blister formation. were taken into account by averaging the behaviour of
In the SLAR process, an instrumented tool is inserted individual crystals, assuming certain strain-producing
into each pressure tube which can detect the spacers, apply mechanisms at the single crystal level in what is referred
an upward bending moment to the inside of the tube to to as a polycrystalline model. This was a lower bound
lift it so that the spacers are free to move and apply an polycrystalline model, which ignores the fact that dierent
electromagnetic pulse to move the spacers with a linear orientations of crystals have dierent strain tensors. The
induction motor [37]. This process has proven very success- anisotropy of the polycrystal (the pressure tube) depends
ful at all the reactors with the loose spacer design. The upon the relative contributions of the strain mechanisms
question arises, Where should the SLAR operator leave at the single crystal level. This was derived from bent beam
the spacers? Since the pressure tube and calandria tube uniaxial stress relaxation tests in which the growth
have already undergone plastic deformation, each assembly component does not contribute to the measured strain
is now unique. A deformation model is used to answer the [7779,83,112] and allowed the prediction of the creep
question [19,20]. anisotropy of a pressure tube under biaxial loading. The
The model comprises three elements, a two dimensional growth anisotropy was derived again using a lower bound
nite element representation of the fuel channel, CDEPTH polycrystalline model, by assuming, that at the single crys-
[19], a calandria tube deformation equation and a pressure tal level, dislocations were the sinks for SIAs, and grain
tube deformation equation. The deformation equation for boundaries were the sinks for vacancies. Once the anisot-
the pressure tube must predict its response to bending ropy of creep and growth were dened, their contributions
moments essentially a uniaxial loading in the axial direc- to elongation and diametral strain in a given power reactor
tion of the tube. Because the calandria tube controls the could be derived from the elongation and diametral strain
gross sag (which can be easily measured) there is no reactor data for that reactor, and the response of a pressure tube to
measurement of this response. A model is required to pre- a multi-axial stress state, including sag [113], could be
dict this response, based upon the measurable deformation predicted.
responses of the pressure tube to a biaxial stress state, i.e., In the mid 1980s, an upper bound approach was used
elongation and diametral strain. The most important (in which all crystals are assumed to exhibit the same strain
208 R.A. Holt / Journal of Nuclear Materials 372 (2008) 182214
tensor) to study the eects of interactions between the crys- the ends of the pressure tube and for high stresses relevant
tals [68,69]. The approach was developed mainly to explain to the relaxation of stresses at aws [23,24].
the irradiation growth response of calandria tube materials
[35,69]. The parameters of the model were derived by the 11.3. Model for pressure tube deformation
same methodology as those for the earlier lower bound
model, but including data for creep in shear as well as stress Although the means to predict polycrystalline behaviour
relaxation [83]. At the same time nite element methods from the behaviour of individual crystals now exist as
were used to calculate the sag more accurately [19,114]. described above, the basic physical parameters that would
Both the upper and lower bound approaches can lead to be needed to construct reliable mechanistic models to pre-
systematic errors in predictions for stress tensors dierent dict the deformation of even a pure Zr single crystal are not
from those for which the data are obtained to normalize known (e.g., mobility and anisotropy, conguration, elastic
the model. As concerns about the accuracy of sag predic- properties of point defects, structures of dislocation
tions for the SLAR application developed in the early cores, and the inuence of impurity atoms on these charac-
1990s (see previous section), a self-consistent polycrystal- teristics). We therefore still rely a phenomenological
line model, SELFPOLY, was developed which allowed for approach.
individual crystals to deform dierently, but under con- The complex interaction between the eects of tempera-
straints imposed by the surrounding matrix of crystals with ture and fast neutron ux on the deformation has led to the
dierent orientations [115]. The single crystal creep and development of analyses that assume that long term steady
growth are deconvoluted from in-reactor data for polycrys- state deformation consists of separable, additive compo-
talline pressure-tube and pressure-tube like materials tested nents from thermal creep, irradiation creep and irradiation
with a range of stress tensors including uniaxial tension, growth as given in Eq. (2.1) [14]. All three components are
biaxial tension and shear [116,117]. The single crystal anisotropic and contribute to length as well as diameter
growth parameters could for the rst time be based on changes. They are given by
growth data coming from tests in high ux reactors [12,61].
This model, currently in use, represents the behaviour of e_ tc d d 2
d K 1 C 1 r1 K 2 C 2 r2 expQ1 =T
the tubes quite well over a narrow range of textures close to
those of pressure tubes, but there are inconsistencies in the K 3 C d1 r1 expQ3 =T ; 11:3:1a
predicted creep anisotropy when the texture is changed sig- e_ icd K c K 4 xC d4 xrx/expQ4 =T K 5 ; 11:3:1b
nicantly [118], Fig. 11.2.1. This is likely due to secondary
contributing factors to the anisotropy, including aniso- e_ ig
d K g K 6 x; /tC d6 x/ expQ6 =T : 11:3:1c
tropic grain shape, anisotropic dislocation distributions
introduced during manufacturing, and the presence of an The in-reactor thermal creep component has two terms [14]
isotropic second phase. A variation of the self-consistent that dominate at temperatures above and below 570 K,
polycrystalline model, applicable for the case when the respectively. The last two terms describe ux-dependent
stress exponent n 5 1 in Eq. (6.4.1), SELFPOLY-N has creep and irradiation growth, respectively. The stress expo-
also been developed [119] for the case of thermal creep near nent for thermal creep varies with stress: for stresses below
120 MPa, the stress exponent is 1, while for stresses be-
tween 120 and 200 MPa, the stress exponent increases to
2 [78]. The parameters in Eq. (11.3.1) are dened as
1.5 follows:
Anisotropy ratio - CBL/CBT
1
e_ d strain rate in a direction d (i.e., radial, transverse,
SELFPOLY axial), h1;
0.5
e_ K 1 ; K 2 constants for high temperature in-reactor thermal
creep;
K3 constant for low temperature in-reactor thermal
0
creep;
K4(x) function describing the variation of irradiation
-0.5
creep due to variations of microstructure along
the length of the tube;
-1
-0.4 -0.2 0 0.2 0.4 x distance from the back end of the tube;
Texture Parameter - FT - FR K6(x, /t) function describing the variation of irradiation
growth due to variations of microstructure along
Fig. 11.2.1. Comparison of measured and calculated (from texture)
the length of the tube as a function of uence;
anisotropy ratios (axial strain rate:transverse strain rate) for internally
pressurized tubes under irradiation creep conditions, from Ref. [118]. The C d1 ; C d2 anisotropy factors due to texture for in-reactor
open square represents CANDU pressure tubes. FT and FR are dened in thermal creep in a given direction d and for stress
Section 3. exponents, n, of 1 and 2, respectively;
R.A. Holt / Journal of Nuclear Materials 372 (2008) 182214 209
10 10
-1
-
Diametral StrainRate x 10 - h
8
8 8
6 6
4 4
2 2
0 0
0 1 2 3 4 5 6 0 1 2 3 4 5 6
Distance from Inlet - m Distance from Inlet - m
10 10
-1
-1
Diametral Strain Rate x 10 - h
8
8 8
6 6
4 4
2 2
0 0
0 1 2 3 4 5 6 0 1 2 3 4 5 6
Distance from Inlet - m Distance from Inlet - m
Fig. 11.3.1. Comparison of predicted and measured strain rate proles for Zr2.5Nb pressure tubes in a Pickering A reactor: (a,b) back end at outlet and
(c,d) back end at inlet, from Ref. [14].
20 50
-1
Measured Diametral Strain Rate x 10 - h
CANDU 6
8
Bruce A 40
Elongation - mm
15 Pickering A
30
10
20
10
5
0
0 1 2 3 4 5 6
0 -25 -2
Neutron Fluence x 10 - n.m , E>1MeV
0 5 10 15 20
8 -1
Predicted Diametral Strain Rate x 10 - h Fig. 11.3.3. Comparison of the model predictions with elongation data for
pressure tubes in a Bruce A reactor, from Ref. [14].
Fig. 11.3.2. Comparison of measured and predicted diametral strain rates
of Zr2.5Nb pressure tube in CANDU reactors, from Ref. [14].
tends to under-predict peak diametral strain rates for
the proles are derived from other information. The model CANDU 6 pressure tubes with outlet temperatures above
is a reasonably good predictor of the diametral strain rates, 570 K, Fig. 11.3.2. This tendency, which at the time was
Fig. 11.3.2, and elongation rates, Fig. 11.3.3 of Zr2.5Nb thought to be within the predictive uncertainty of the
pressure tubes in Bruce A and Pickering A, operating tem- model, has since proven to be even greater [120].
peratures up to 570 K. It also predicts well the axial and
diametral strain rates for small tubes with textures similar 12. Outstanding issues and future work
to pressure tubes irradiated at high fast neutron ux at
553 and 583 K [12], Fig. 11.3.4, and diametral strain rates Over 40 years of in-reactor testing and over 30 years of
for pressure tubes operating at temperatures of up to operating experience in power reactors have provided a
670 K at low stress (<80 MPa), Fig. 11.3.5. However, it broad understanding of the in-reactor deformation of
R.A. Holt / Journal of Nuclear Materials 372 (2008) 182214 211
-50
12.2. More severe reactor operating conditions
-50 0 50 100 150 200
8
Calculated Strain Rate x 10 , h
-1 The model described in Section 11.3 was normalized to
data from the Pickering A Nuclear Generating Station and
Fig. 11.3.4. Comparison of measured and predicted axial and transverse tested against data from the Bruce A Station and early data
strain rates for micro-pressure tubes irradiated at 2 1018 n m2 s1,
from CANDU 6 units which operate at higher tempera-
E > 1 MeV, in Osiris at 553 and 583 K, from Ref. [75].
tures and fast uxes than exist in the Pickering A units.
Already one could see a tendency to under-predict the
CANDU 6 data, Fig. 11.3.2. Although, in 1996, this dis-
70
crepancy was deemed to be within the predictive error of
60 the model, we now know that there is a systematic under-
-1
12.1. Polycrystalline modelling The principle that creep can relax stresses at aws has
been clearly demonstrated experimentally. The susceptibil-
As stated in Section 11.2, models for anisotropy of creep ity of notched specimens of pressure tube material is signif-
and growth that are based solely on crystallographic tex- icantly less if the notched specimen is held at temperature,
ture suer from some deciency when one attempts to under load, to allow creep to relax the notch-tip stress prior
extrapolate over a wide range of textures. Other micro- to testing for DHC susceptibility [125].
212 R.A. Holt / Journal of Nuclear Materials 372 (2008) 182214
The model for localized creep at the high stress regions 12.8. Creep at the pressure tube ends
near aws is based on a very limited data set and this cer-
tainly needs to be augmented. The least understood aspect of in-reactor deformation
of pressure tubes is the transition region between thermal
12.5. Temperature cycling eects creep and irradiation creep, i.e., the fast ux range of
0.16 1016 n m2 s1, E > 1 MeV. This corresponds to a
Because they have a high capital cost and a low oper- region about 0.3 m long, adjacent to the end-ttings at each
ating cost, most existing nuclear generating stations end of the reactor, where the bending moment is high. The
operate as base-load electricity suppliers. Future nuclear current representation of the creep behaviour in this region
plants may operate in a load-following mode, particular is crude, and is not a good match to the data. It is very
if, as seems likely, nuclear power occupies a larger share likely that a more accurate model will change the results
of the electricity supply in some markets. Operating reac- of sag and contact predictions, and it is therefore most
tors in load-following mode may involve signicant tem- important that eorts to address the deformation rates in
perature changes. The large transients in growth strain this fast ux range [25] should continue.
observed after temperature changes, see Section 5, suggest
that temperature cycling may contribute a component to Acknowledgements
the strain, dierent from that predicted by the models
presented in Section 11. This area requires further I would like to acknowledge John Slade of New Bruns-
investigation. wick Power for permission to use previously unpublished
data from the Point Lepreau Nuclear Generating Station,
12.6. Creep rupture and Grant Bickel, Pam Simons and Eric Nadeau of AECL
for providing the gures showing that data. I would also
The case for operating pressure tubes to creep strains of like to thank Navid Badie, Grant Bickel and Stephen
the order of 5% is based on the supposition that pressure Douglas of AECL for permission to refer to their unpub-
tubes will exhibit quasi-superplastic behaviour under irra- lished data, Malcolm Griths of AECL for providing
diation creep conditions because of the low stress sensitiv- micrographs and Nick Christodoulou of AECL for provid-
ity of the strain rate, see Section 8. As pressure tubes in ing digital versions of some of the gures. The preparation
current reactors are approaching this level of peak diame- of this review was sponsored by the Natural Sciences and
tral strain (some tubes in the older CANDU 6 reactors Engineering Research Council of Canada, Ontario Power
have strains >4%), it is important to assess the microstruc- Generation Inc., the CANDU Owners Group Inc., and
ture at the peak-strain location to verify that there is no Nu-Tech Precision Metals Inc., under the Industrial Re-
evidence of impending failure due to an as-yet unidentied search Chair program in Nuclear Materials at Queens
mechanism associated with the high levels of radiation- University.
induced mass transport. This is especially important in Figs. 2.1.3, 2.1.4, 3.2, 4.1, 4.34.5, 5.1.1, 5.1.2, 5.3.1
view of the microchemical changes induced by the thermal 5.3.4, 5.4.1, 5.6.1, 5.6.2, 6.2.1, 6.6.1, 7.2.1, 9.19.6, 11.2.1,
ux, see Section 12.7. 11.3.111.3.5 were adapted, with permission, from pro-
ceedings of the 6th, 8th, 9th, 10th, 11th, 12th, 13th, 14th
12.7. Transmutation eects and 15th International Symposia on Zirconium in the
Nuclear Industry, ASTM STPs 824, 1023, 1132, 1245,
A little recognized fact is that Nb transmutes to Mo as 1295, 1354, 1423, 1457 and the Journal of ASTM Interna-
a result of irradiation by thermal neutrons. It is estimated tional Vol. 2 copyright ASTM International, 100 Barr Har-
that about 25% of the Nb is transmuted to Mo at the bor Drive, West Conshohocken, PA 19428.
mid-core location after 30 years of operation [126]. The Figs. 3.4, 3.5, 5.1.3, 5.5.1, 5.5.2, 6.2.1, 6.3.2, 6.4.1, 6.4.2,
alloy content will be changed from 2.52.8 wt%Nb to 6.4.6, Figs. 8.2, 10.1.1, 10.1.2 and 11.3.4 were adapted with
1.92.1 wt%Nb and 0.60.7%Mo. There is very little permission from the Journal of Nuclear Materials, Vol-
information on irradiation behaviour of alloys containing umes 60, 98, 149, 159, 317 and 335, copyright Elsevier B.V.
Mo except for Excel (Zr3.5 wt%Sn0.8 wt%Nb
0.8 wt%Mo) which behaves similarly to Zr2.5Nb, but
References
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