A translation from
Atomit: Energy of Canada
by
C. PETERSEN
Kernforschungszentrum
translated by
R. Gerarts and L.G. Bell
translated from
Gesellschaft fur Kernforschung m.b.H., Karlsruhe,
report KFK-Ext. 6/73-6, March 1973
Power Projects
Sheridan Park Research Conrtinunity
Mississauga, Ontario
March 1975 ASCL-5101
LITEPATURE SEARCH ON SOME PROPERTIES OFZIRCA1OY-4 AT HIGH TEMPERATURES*
by
C. PetersenKernf orschungszentruni
(Nuclear Research Centra)Karlsruhe, Germany
Translation by R. Gerarts and L.G. Bell
Power ProjectsSheiidan Park Research Community
Mississauga, OntarioMarch, 1975
^Translated from the Germair for Atomic Energy of AECL-5101CariaM%imite"a from Gesellschaft fur Kertiforschangisvb.H., Karlsruhe^ report KFK-̂ Ext. 6/73-6, March, 1973
Données g l a n é e s dans l e s p u b l i c a t i o n s c o n c e r n a n t
c e r t a i n e s p r o p r i é t é s du Z i r c a l o y - 4 aux h a u t e s t e m p é r a t u r e s *
par
C. P e t e r s e n
Kern fo r schungszen t rum( C e n t r e d ' é t u d e s n u c l é a i r e s )
K a r l s r u h e , Allemagne
* Ce r a p p o r t o r i g i n e l l e m e n t p u b l i é dans G e s e l l s c h a f t fu rKernforschung m . b . H . , Karl s h r u h e (Rappor t KFK-Ext.6 / 7 3 - 6 , Mars 1973) a é t é t r a d u i t d ' a l l e m a n d en a n g l a i spour l ' E n e r g i e Atomique du Canada , L i m i t é e p a rR. G e r a r t s e t L.G. S e l l .
Résumé
Ces données glanées dans les publications con-cernent quelques propriétés mécaniques et physiques duZircaloy-4 pour la gamine de températures allant de 600°C"a 1800°C. On décrit le comportement des efforts-contrain-tes de la résistance ultime et de 1s ductilité dans lasconditions de pression interne, d1expansion thermique, deconductivité thermique et d'émissivite totale.
L'Energie Atomique du Canada, LimitéeGroupe électronuelêaire
Sheridan Park Research CommunityMississauga, Ontario
Mars 1975
AEÇ.U5T&Ï.
LITERATURE SEARCH ON SOME PROPERTIES OFZIRCALOY-4 AT HIGH TEMPERATURES*
by
C. PetersenKernforschungs zen trum
(Nuclear Research Centre)Karlsruhe, Germany
Translation by R. Gerarts and L.G. Bell
ABSTRACT
In this literature search some mechanical andphysical properties of Zircaloy-4 are compiledfor the temperature interval of 600 to 1800°C.The behaviour of stress-strain, ultimate strength,and ductility under internal pressure, thermalexpansion, thermal conductivity, and totalemissivity are described.
Po^sr ProjectsSheridan Park Research Coiamunity
Mississauga, OntarioMarch, 1975
^Translated from thE German for Atomic Energy of AECL-5101Canada Limited from Gesellschaft filr Kernforschungni.b.E. „ Karlsruhe, report KFK-̂ Bst; 6/7S-6, March. 1973.
TABLE CF CONTENTS
1 . Introduction
2. Stress vs Strain Properties of Zircaloy-4 and Zr-0.7 5n
3. Ultimate Stress Behavior of Zircaloy-4
4. Expansion Behavior of Zircaloy-4
5. Thermal Expansion of Zircaloy-4
6. Thermal Conductivity of Zircaloy-4
7. Emissivity of Zircaloy-4
8. Summary
Bibliography
Tables
Fig. 1 - 2 2
— 1 ~
1. Introduction
The loss of coolant arc w!r-nt (LOCA) i :; vuris ir]f-rr-<i f; y-jf- the- mcst scnfjus
failure in the operation of light water reactors. This accident is caused
by a rupture in the piping system of the primary coolant circuit and results
in a rapid loss and pressure drop of the coolant followed by a rapid tem-
perature rise of the fuel element sheath. D'.ring the heat-up period of
the sheath, ballooning and isolated bursts may occur due to the inner proa-
sure of the fission i;as.
Zircaloy-4 is used as a sheath maceriaJ in light water reactors; it melts at
about 1871 C. During heat-up it passes an allotropic transformation from the
denser hexagon structure (a) to the cubic epicentric structure (B). This
transformation starts at about 815"C and ends at about 9fc>5 C. fig. 1 shows
the temperature range for the analysis of the loss of coolant accident in
connection with the stress-strain properties of the sheath. The lower limit
of the test temperature range for the analysis of the loss of coolant accident
is given by the normal operating temperature of tne sheath (approx. 320 C).
The actual critical test analysis range for the loss of coolant accidento o
between 600 C and 1200 C was supplied by General Electric, Combustion En-
gineering, Westinghouse, Babcock and VJilcox and ORNL, using internal pres-
sures* between 0.035 and 1.41 kp/min . The sheath may be damaged in this
temperature range.
2. Stress vs Strain Properties of Zirculoy-4 and Zr-0.7 r-
oTensile strength data are available for Zircaloy-4 up to 500 C; this may
be the upper limit of the operating temperatures of boiling and pressurized
water reactors. Few data are available for higher temperatures.
Data from tensile tests performed by J.F. White on Zircaloy-4 plate-*1
at a crosshead speed of 0.05 min in a helium atmosphere, have been
incorporated in fig. 2 for temperatures of 650, 900, 1200 and 1500 C.
* Editor's note: kp = kilopond = kilocrram force,i.e., 9.B06 65 N.
" 2 —
This clearly shows that there is no longer ary hardening at temperatures
of 650 and 900°C for strains V" beyond 0.5. At temperatures of 1200 and0
ISOC^C it can even be assumed that the yield stress will just about equal
the ultimate stress.
M..1. Luton iind J.J. Jonas' performed covnpx'ess"" on tests on various
zirconium-tin alloys at high temperatures. The aJ loy with a 0.7'!, Sn
content has the closest resemblance to Zircaloy-4 even though the tin
jontenr is half of what it is in Sircaloy-4. The tests were done at 775 C- 4 - 1 -.1
at a ief orinat ion rate between 10 s and 1 s in an argon atmosphere.
ffiq. 3). At the test temperature of 775 C, lower stress values are obtained
as the deformation rate is reduced. At the hi<jh deformation rate of 1 s """,
the stres-i incivcsss until the strain reaches 0.4. At a deformation rate
of 10 s , the stress only incrtrases up to a strain of 0.04. The stress/
strain graphs also show that at larger expansions there is no more hardening.
3. Ultimate Stress Behavior of Zircaloy-4
Th? ultimate strength values 0B depend mainly on the degree of cold work
which is still latent in the material at the individual test temperature.4) •>
Tests performed by Woods indicated a strength of 78.7 kp/mm ; the tensile
tests were carried out at room temperature on 78% cold formed Zircaloy-4O 2
sheaths *rhich had been annealed at 510 C, Compared with 57 kp/mm for 78%
cold formed material annealed at 650 C, a difference of about 40% in strength
is obtained. Apart from this, the tensile strength of material annealed ato !'
510 C is already 50% lower than the cold formed material. At temperatures
above 600 C the effects of cold forming disappear rapidly,- the difference in
strength between the cold formed material and material which was annealed
after cold forming is wiped out. Fig. 4 shows the ultimate strength at
temperatures of up to 1800°C (i.e. about 70°C below the melting point) of
annealed Zircaloy-4 plate specimens with load applied in the direction
of rolling. Tests at higher temperatures were performed at a strain rate
of 0.06 min . Scott's values for the cold formed tube samples corres-
pond favorably with annealed plate samples.
Fig. 5 snows a comparison of ultimate stress tests a which were made
using transient temperature tests ' with a heat-up rate of 25 C/s and
3 other tests " oi" boiling-water, reactor sheaths, Although the graph?
follow a similar pattern, the ultimate strength values measured by
Hardy are at higher temperatures than the other tests. 7/his is partly9)
due to different test conditions. Tests performed by Emmerich et al,
'were terminated when the expansion reached 34% as at a greater expansion it
is no longer possible to assure an unhindered coolant flow in case of
emergency cooling. Therefore, the valuer measured by Emmerich et al. at
a heat~up rate of 22°C/s are not necessarily always ultimate stresses.
Moreoverf these tests were performed in a steam atmosphere as were those
carried cut by Hobson and Rittenhouse and th.is reduces the expansion
because the Zircaioy oxidizes especially at high temperature?.
Waddell and Rittenhouse made use of the rupture strength by first
heating up to the desired temperature and than subjecting the tubular2
specimen to a pressure of 0.035 kp/ram . The lower expansion velocity
obtained in this manner may cause creep at the set high temperature. Failure
could therefore occur at lower temperatures. Test results t. -tained by Hobson
et al. correspond most closely to those obtained by Hardy ' , These tests
were performed in an inert cover gas citmosphere with a heat-up rate of
28 C/s and with expansion unhindered in both the axial and radial direction.
Nevertheless.- the tensile stresses are xower than those measured by Hardy.
This may be due to a more uniform wall thickness of the sheath? tested oy
Hardy as compared with the boiling water reactor sheaths tested by Hobson
Hobson noticed that variations in the wall thickness have a considerable
bearing oil the ultimate strength. Moreover, the ultimate strength values
given by Silpbsdn very clearly show a drop within the a-B phase transformation
range. ,'Hobson suspects that tho a-3 transformation, being a shear action,
adds to the force eserted on the specimen wall and causes an earlier rupture.
Eme*y c?t .al.10) checked the strength of Sircaloy-4 sheaths with internal
pressure tests at pressures of 0.14-1.76 kp/irat̂ and hat-up rates of
1 •;. ~> - 96.2 C'/s in a helium atmosphere. As can be seen from fig.6 the
rupturt temperature T aoes not depend on the inner pressure to a great
extent. The differences ir. failure temperatures for all pressures are
tairly small, being o. ly about 194°C max. The same figure shows the
ultimate strenqth values for 'Zircaloy-4 sheaths which were distorter! in
an axial direction. Compared with the values for transient temperatures,
there is no big difference.
ilibsoi! and Ri tti-r.hrnse " made similar test's at higher temperatures. They
checked for failure v.ith internal pres.- r s as a function of temperature
under transient test conditions (pressures of 0.035-0.703 kp/mm2 and heat
up rates of 5.5-55.5 C/i). Fiq.'1 gives the maximum pressure P _ v.-.
temperature, using the heat-up rate as a parameter. This shows that in
the two-phase ar-̂ a (a+6) at pressures between 0.14 and 0.42 kp/mm'' a burst
occurs at low circumferential expansion.
Osborne and Parker carried out burst tests on individual tubes of
irradiated Zircaloy-4. The tast conditions were similar to those of Hob-12)
son except that measurements ware made in a closed environment of a
steam-argon atmosphere. The maximum expansion recorded for irradiated
material was 50% whereas the majority of values were in th<= 50-40% range.
Short-duration tests were made at General Electric on Zircaloy-4 plate
specimens at high temperatjres (up to 1800 C ) . The tests were made in
an argon atmosphere with a constant distortion velocity of 0.13 cm/min
in order to obtain data on ultimate strength. Supplemertary tests were
made in a helium atmosphere at temperatures in the range of 650-r.500°C,
using the same Zircaloy-4 plate specimen (0.76 mm thick) in order to
obtain the yiald stress values of the material. The distortion velocity
was measured with an electrical optical extensometer. The results are
shown in fig.8. This graph shows that in the temperature range of 6r-0 -o -i
900 C at a distortion velocity of 0.005 min the ultimate stress is lower
for each temperature than in the report mentioned above. This means that
the strength depends on the distortion velocity. In order to check this
more accurately, additional measurements were taken with distortion velo-
cities of 0.05 and 0.1 min . These results are also shown in fig.8 and
seem to confirm the relation between the strength and the distortion
velocity.
White" tested zii'caloy-4 tubes with irit_rnal pressure under steam and
an inert atmosphere. These tests toe were halted when the expansion
reached 34%, because at: a greater expansion Lt is no lonqer possible to
ensure an unhindered coolant flow m case of emergency coolino. Fig.9
shews ditferent heat-up rates vs strep U ff, caused by internal pres-
sure in the tube wall. Moreover, i* . >ws the point where ductility
changes to brittleness in a steam at' sphere. The results of this check
show the general behavior of Zircaloy-4 tubes under an internal pressure
with a steam atmosphere present dating heating.
Following is a summary of the test results:
1) The material fails by rupture at less than 34% circumferential ex-
panr.ion with internal pressures under 0.05 kp/nun (= 0,35 kp/mm effective
stress) with heat-up rates of less than 50 C/s. At higher heat-up
rates, an uneven behavior is noted; it includes so:tie sheaths which,
even at temperatures of up to 1700 (
failure at low to medium expansion.
even at temperatures of up to 1700 C, did not show any material
2) Sheaths subjected to an internal pressure of 0.06 kp/mm2 (= 0.43 kp/mm
effective stress) fail by rupture at a circumferential expansion of less
than 24?o at heat-up rates of over 200 C/s.
3) Sheaths which are subjected to internal pressures between 0.07 and 0.C8
kp/mm (=0.51 - 0.58 kp/mm'' effective stress)fail either because of a ducx.il
brittle rupture. The basic rupture behavior in this pressure range
cannot be defined easily, because the rupture mechanism is very sen-
sitive to slight variations in correlated reactions such as the mechanic-
al properties of the sheath, the internal pressure, temperature and
degree of oxidation.
- 6
4) At internal pressures above 0.08 kp/tran2 (= 0.58 kp/ram2 effective stress) and
heat-up rates of a few tenths of a degree Celsius per second, a ductile
rapture occurs similar to i.he one which was observed during annealing
9)tests" in an argon atmosphere.
Emery et al.10' checked the effect of the hea'-. up rate (12.7 - 96.2°C/s)
on the rupture for temperatures up to 750 C and at an internal pressure
of 1.76 kp/r.r: . As can V een from fig. 10, it is hardly possible to
observe a dependence of the rupture temperature on the heat-up rate in this
temperature range. However, at temperatures higher than those used during
tests performed by Hobson and Rittenhouse , an increase in the rupture
temperature occurs at an internal pressure of 0,07 kp/mm2 and heat-up rates
of 5.5 - 55.5 C/s. This effect was not noted in the a-phase nor in the
2-phase area (a+fi) . However, iiobson and Rittenhouse suspect that the
shear action during the transformation through the 2-phase area (a+3) is
the reason for the dependence on the heat-up rate. According x> Hobson,
the heat-up rate of the test sample could be lowered since t..e phase trans-
formation is endothermic.
4. Expansion Behavior of Zircaloy-4
12)Hobson and Rittenhouse investigated the circumferential expansion which
occurs at higher temperatures under transient test conditions when the
sheath ruptures (pressures between 0.035 and 0.703 kp/mm2 and heat-up
rates of 5.5 - 55.5 C/s). Fig.11 shows the circumferential expansion E
vs max. pressure P . From this can be seen that in the 2-phase area
(a+3) at pressures between 0.14 and 0.42 kp/mm2 the circumferential expan-
sions (20-40%) reach a minimum.
l graphs representing the expansion are difficult to compare be-
cause both material and test conditions were too varied.
In reference 5 , the elongation of tensile test specimens, measuring
25.4 x 6.3 x 0.76 mm (length x width x thickness) is shown as a function
of temperature (fig.12) . Below 400°C, the elongation of the specimen in
general does not depend on the ttmperature. Thereafter the elongation
increases and reaches a maximum of about 85% at 1200 C. In comparing with4)
burst tests performed on tube samples with 78% cold work , a difference
is found in the temperature range of 360-550 C; in this latter case, the
elongation increases to only about 25%.
In another test , the elongation £ of Zircaloy-4 plate samples was also
represented as a function of temperature where the distortion velocity e
was varied (fig.13). Except foi: the test performed at 900°C, the curve
follows the same trend. Maximum ductility is reached around 1200 C. The
values do net indicate a dependence of the specimen elongation or. the
distortion velocity.
Hardy investigated the behavior of Sircaloy-4 sheaths at high tempera-
tures and made internal pressure tests from 0.035 to 1.41 kp/mm2 at a
heat-up rate of 25 C/s. After a certain temperature was reached, it
was maintained until rupture. Fig.14 shows that at an increasing temper-
ature and an internal pressure of 0.07 kp/mm2 the tube initially shows
little circumferential expansion. The maximum circumferential expansion
from 815 to 940°C, i.e. a rise of 125°C, is only 0.1 to 1%. At a con-
tinuing temperature rise the circumferential expansion also increases from
1% to 10%. The semi-logarithmic representation shows a further circum-
ferential expansion from 10 to 11C% up to rupture for the next 10 C.
-i \
In tests performed by Waddell and Bittenhouse^ , 5 distinct temperatures
were selected: 590, 790, 890, 980 and 1150 C where:
590 C is in the range of phase af
790°C is just below the phase transformation a-*-(ct+3),
89Q°C is in the middle of-the (a+B5 phase,
980°C is just above the phase transformation (a+3)-»-$,
1150 C is in the range of phase (3.
The internal pressure tests were made isotherrnally at the temperatures
mentioned above at different pressure gradients from 0.035 to 0.039
kp/mm2...Pig.15.shows the circumferential expansion E V S temperature.
The lowest circumferential expansion (50 - 70%) was measured at 1150 C,
the highest (50 to >1403,} at 790°C. It should be noted that the size
- 3 -
of the rupture cannot be determined from the circumferential expansion.
Besides, the circumferential expansion also depends on the variations8)
in the wall thickness. Hobson et al. checked this out in transient
burst tests and found differences in expansion up to a factor of 2.
There follows a summary of the rupture behavior of Zircaloy-4 in relation
to time.
Fia.16 shows the ultimate stress graphs as a function of time for the
temperature range 600-1000°C according to research done by Hardy .
The test specimenswere heated up at a rate of 100 C/s, i.e. the period
shown on the graph is the holding time before rupture ar the temperature
reached. Ultimate stress graphs are usually straight lines, but curves
for lower temperatures (650-800°C) show a deviation from the straight line
for brief periods. It could not be ascertained why this effect was
limited to the a phase.
Baker14) also measured similar graphs, except that in this case the internal
pressure .P. is shown in relation to the period before rupture for the
temperature range of 850-1100°C (fig.17) .
5. Thermal Expansion of Zircaloy-4
Scott measured the thermal expansion of Zircaloy-4 by means of an electro-
mechanical dilatometer. This instrument records the expansion of the test
sample in accordance with its temperature. Because of the strong anisotro-
py of Zircaloy-4, different graphs are obtained for the thermal expansion
coefficient a in a radial and axial direction of the specimen as a function
of the temperature. These are shown in fig. 18 and 19. A fltop in the
thermal expansion coefficient occurs in the (a+B) phase in the radial (sic)
direction.
6. Thermal Conductivity of zircaloy-4 : : •
It is not unusual to have differences of one or two decades of thermal con-
ductivity values for one and the same material. Some of these are due to
the difficulty of measuring the thermal conductivity. However, considerable
- 9 -
changes in thermal conductivity oncur in some materials when there is a
minor deviation in the chemical composition and microstructure. A single
affect may depend on the temperature, i.e. there may be a wide deviation
at low temperatures which may disappear again at high temperatures. Dur-
ing a loss of coolant accident, tho thermal conductivity of the composi-
tion may be affected to a large extent by the presence and structure of
metallic and oxide phases in the sheath material.
Faith measured the thermal conductivity X of Zircaloy-4 in the
temperature range 400-1500°C, Scott in. the range 80-700°C
and Chirigcj et al. in the range 100-350°C. All these values are
shown in fig. 20. Scott values were obtained from tests on
tube specimens; the deviation from the calculated curve of the smallest
error squared amounted tc ±10%. Feith's average values are within ±5%
of those on the curve; furthermore, these values show an increase for
temperatures over 1000 C. Values measured by Chirigos fcr Zircaloy-4
up to 600 C correspond to those obtained by Feith; over 600°C, a con-
siderable increase in the thermal conductivity is noted. The deviation
from the Feith values reaches about 13% at 850°C.
Feith values are appropriate for calculating coolant losses. However,
errors due to the high oxygen content in the metal and external oxide
layers, must be taken into account as was noted in the above
description of the factors which affect the thermal conductivity; these
conditions manifest themselves when a loss of coolant occurs.
an example shows that this consideration is important. Following is the
effect of a layer of oxide on a Zircaloy-4 sheath at 1200 C: Assuming
that the sheath has a wall thickness of 0.51 mm and that a 0.051 mm
thick layer cf oxide ZrO, has built up with a thermal conductivity of
0.0'25 ft/cm C, further, that the combined thermal conductivity of the• - . • . - . . . • - • - . - . .. • ,- .. - ,.. . •• o
oxygen richmaterial and the Sircaloy-4 together amount to 0.3.1 W/cm C,
the results then show a oropof the thermal conductivity in a radial
direction (wall thickness) from 0,31W/cm°C to 0.147 W/cm°G (a decrease of
approK. 50%) and to 0.28 W/cm°C in an axial direction fa decrease ofapprox. 10%) . The presence of a layer of oxide in a radial direction
- 10 -
has a greater effect on the thermal conductivity than a possible error
in the measurement of the values of thermal conductivity of Zircaloy-4.
7. Emissivity of Zircaloy-4
Fig.21 shows the total emission e~ of Zircaloy-4 in relation to temperature
and for different typos of oxidation. According to White , the specimen
material was oxidized in a steam or oxygen-argon atmosphere. Subsequently,
the emission was measured in a vacuum. The thickness of the oxide layer
varied from 5 to 200 \m. The radiation behavior C™ of the oxidized spe-
cimens follows a parabolic pattern. The specimens which are saturated
with oxygen as well as the non-oxidized sample are shown for comparison.
Isothermal tests were also performed on the Zircaloy-4 in a steam atmosphere
in order to check the change in emissivity when the layer of oxide increases
with relation to time. The results are shown in fig.22.
The general trend shows that the values for the total emission of non-
oxidised material almost immediately increase from 0.2 to 0.7 and thereafter
very slowly increase to 0.8. After a prolonged period - dependent on the
test temperature - the emissivity again decreases. This was to be expected
since, according to Cox , the total emission of ZrC, in the corresponding
temperature range lies between 0.3 and 0.4,because the thicker the oxide
coat which forms on the surface, the sooner the emissivity of pure ZrO
is reached. However, since the times and temperatures assumed at a loss
of coolant accident are less, values of 0.7-0.8 should be considered for the
total emission.
8. Summary
The stress/strain behavior of Zircaloy-4 and Zr-0.7 Sn depends on the dis-
tortion velocity. No hardening occurs at high temperatures and low distor-
tion velocities. The ultimate stress behavior'of Zircaloy-4 is affected
by the a-3 phase transformation in both isothermal and transient tests.
It was found that rupture behavior also depended on the distortion velocity..
- 11
The expansion behavior for high temperatures and high internal pressures -
even under a steam atmosphere - if- still good. Only in the range of the
£-phase was it noted that expansion depends on heat-up rate. There is no
dependence on the distortion velocity.
Due to the strong anisotropy of "ircaloy-4, the thermal expansion co-
efficient shows different values in the radial and axial directions of
the sheath.
The thermal conductivity after oxidation rapidly decreases by about 50%
in the radial direction.
The emissivity of non-oxidized Zircaloy-4 is about 0.2-0.3, whereas values
of 0.7-0.8 were measured with an oxidized specimen.
It is often difficult to make an accurate comparison of the values given
in the publications mentioned because, unfortunately, they do not always
state the exact test conditions, how the specimens were treated or the
technological and metallurgical conditions of the material investigated.
12
P.ibliography
1) Waddeli, j r . , R.D. ..:,i.:l P.L. Rittenhouse:
"High-Temperature Burst Strength and Duc t i l i t y of Zircaloy Tubing"
Paper: 0RNL-TM-3?«c\ March 1971
2) White, J . F . :
"Physicochemical Stud ies of Clad UO? under Reactor Accident Conditions"
Paper: GEMP-1012 ( P t : 2 ) , P. 203-252
General Electr ic Co., Cincinnat i , Ohio, Nuclear Systeir, Program
3) Luton, M.J. and J.J.. Jonas:
"Solute Strengtheniric a t High Temperatures in Zirror.ium-Tin Alloys"
Canadian Metallurgical Quarterly, Vol. 11 , Mo. 1 (1972)
4) Woods, C.R.:
"Propert ies of Zircaloy-4 Tubing"
Paper: WARD-TM-5B5, Appendix C
5) Sixth Annual Report •;- High Temperature Materials Program, Part-A r
GE-13MPO
Paper: GEMP-475A, Me; rch 31 , 1967, P . 261-263
6) S c o t t , D.B.:
"Physical and Mecha-r.caJ Properties of Zircaloy-2 and 4"
Paper: WCAP-3269-41, May 1965
7) Hardy, D.G.:
"High Temperature Expansion and Rupture Behaviour of Zircaloy Tubing"
Fuel Engineering Branch Atomic Energy of Canada Limited, Chalk River,
Nuclear Laboratory Chalk River, Ontario, Canada, March 1973
8) Hobson, D.O.; M.F. Osborne and G.W. Parker:
"Comparison of Rupture Data from Irradiated Fuel Rods and Unirradiated
Cladding", Nuclear Technology, Vol. 11, Aug. 1971, P. 479
9) Emmerich, K.M.; E.F. Juenke and J.F. White:
"Failure of Pressurized zircaloy Tubes During Thermal Excursion in Steam
and Inert Atmospheres", ASTM--STP.458 American Society for Testing and
Materials, Philadelphia, Pennsylvania, 1969
13
10) Emery, A.D.; D.B. Scott and J.P, Stewart:
"Effect of Heating Rate and Pressure on Expansion of Zircaloy Tubing
During Sudden Heating Conditions"
Nuclear Technology, Vol. 11, Aug. 1971, P. 474-479
11) Hobson, D.O. and P.L. Rittenhouse:
"Embrittlement of Zircaloy-Clad Fuel Rods by Steam During LOCAL
Transients", Paper: ORNL.4758, Jan. 1972
12) Hobson, D.O. and P.L. Rittenhcuse:
"Deformation and Rupture Behaviour of Light Water Reactor Fuel Cladding"
Paper: ORNL-4727, UC-80-Reactor Technology, October 1971
13) Osborne, M.F. and G.W. Parker:
"The Effects of Irradiation on the Failure of Zircaloy-Clad-Fuel-Rods"
Paper: ORNL-TM-3626, Jan. 1972
14) Baker, J.N.:
"Fuel Element Integrity and Behaviour in a Loss of Coolant Accident"
Paper No. 14 of the CREST Specialist Meeting on Emergency Core Cooling
for Light Water Reactors, Munich, October 18-20, 1972
15) Feith:
"High Temperature Materials Program Progress Report No. 61"
GE-NMPO; Paper: GEMP-61, September 30, 1966
16) Chirigos, J.N.j s . Kass, W,W. Kirk, G.J. Sal', sggio:
"Development of Zircaloy-4 Fuel Element Fabrication - I . "
International Atomic Agency 1961f P. 45
17) Cox, R.L.:
"fimittance of Zirconia to 4600°F"
Boeing Report No. 3-100012R19, Catalogued by DDC as AD-434003, April 30,
1962
*̂ ^
Fig Author
2)
Relationship
3) c.
Temp.Range°
Heat-OpRate
650-1500
775
DistortionVelocity
0.05 min
TestSample
Plate
Kf4-1 s Plate Argon I leTestAllov
rupture, l. •.-.
hardening IJT. to be eK^i*dt hi ah temperatures
^o harden!nq occurs ar lewdistortion velocities
4) (!„, T RT Tube51C°C/
Air Up to 600"C affected bythe cold work snd heattreatment
5)
6)
1)
7)
» T
B'
0 ,TBO
RT-1800
RT-750
560-1150
0.06 !nin Plate Annealed inert ' Terusi le: Test
Plate
Tube
10%kv
750-1225 25 Tube
TensileTest
inert ; Internali Pressure
inert ', ]nt"rialP r*'c sure
CiMii :nat .-b i;i-i of theVdhn-: di'Sj.ite differentprior treatment
Creep action possible
Highest Ultimatestress values due tosiiqhr variations in vra1.1thickness
o2
fin <v
•w o u• i aE* < Dt
4 i-4 > i <fl •!->O H 0) Cwt id n a)a. c &•• e
4J Q,Hi 6O 3
a m> •o
1/1 XW 0i>
4> JQIA
•O
»J «
5 S3 3
at
u -f
XI
o t >g P*
u w. § fi
y w ©« uU O I'l
4 h
S 3ID
<u a
uu•
9»
n si
HI t)0i "rt Mi-S H 3+1 41 J3J in
s
Si
•§
! !
5> e
H V
H ft
igUl X
Is I
s tn
ISl-tCM
H UIB JJ HC O -W
•3»o d•p o
-H 01Q >
?
ino ino O •-»
J1in1
O 1
<TiI
O
o
r-t
iCO
83<
w i tin nj i
0 B K
Fig.
f
• • I . , i i
10..
\<S
\\
r J,
LZ
r
1-i
^13
^itythor
i
" 1 2 ) , 'r1
-U
>.
< 4f
, 2)
1
Relationship j
TBnich' - (Heat-Uj* 1rate1 ^
TBruchf• . J
Heat-OpRate L
flx' V-:
V T"
r
Temp. -Bange^£°C> "
(b40-7^!0
10'ao- i1200
v. ^
780- -1430
RT-550i
lRt-1700
600-1500
Heaf-U|>R^te<°c/*0
12,7-96,5
5r,5-!:5(5
b,5-55,5
I
-
DistortionVelocity
0,00b .0,05 }mm"0,1
TestSample
Tube
"JPabe
lube
ifabe
Plate
Plate
Prelimi-naryTreat-menr
Cold .Formed
Sam; leaindi rectiorofrolling
( -Testfitoos-phere
inert
inert
inert
inert
inert
inert
Notes
InternalPrass ire
Interna!Pressure
InternalPressure
InternalPressure
TensileStrength
TensileTest
Results
Failure temperatureTBruch a s C Q t a f f c c t e d
by heat~up rate
Since o+S cransfofmationis endothermic, lowering •of h»at-up iata ispossible
in 2-Pha«;e area (a+B)m m . expansion -at -P ^ 0.14 - 0.42 Jcp/BSR
Expansion between 3C0and 53O°C is lower thanm tensile cest.
Up to 300 C temperature doesnot affect expansion, max.expansion occurs -at 1200°c
Expansion is not affectedby distortion velocityMax. expansion at 1200°C
Figr.
14
15
16
17
]
t
!r
io,'.
author
7/
1)
7}
14)
6)
6)
ev
Relationship
VT
0 , TB Bruch
xr Bruch „
n, T"
A, T f
Temp.Range(°C)
830-1050
590-1150
650-1000
850-1100
RT-1000
St-600
80-780
Heat-UpBate("C/s)
100
100
•
DistortionVelocity
0,035-0,039kp/mm2
min
TestSample
Tube
Tube
Tube
Tube
Tube
Tube
Prelimi-naryTreat-ment
TestAtmos-phere
inert
inert
inert
inert
inert
Notes
InternalPressure
InternalPressure
InternalPressure
InternalPressure
RadialDirection
AxialPirecticii
Results
Rapid increase inexpansion in the range ofthe '.'.-Phase in thelogistic representation
Max. expansion at 80D°C;niin. expansion at 1150 C;it is not possible todefine the type of rupture
Deviation of the TensileStrength curve from astraight line in thea-region
Similar development as initem 5
In a radial direction dropin o+© area, in general:thermal expansion variesdue to stiongrayiisotrophyof Zircaloy-4
Correspond to values initeia 14
ii•RltS
i l lIPlip##»fli
ill
i l:«*ti'-*!-,
«f
mm§m
mmStSfipf
nn
lititiifmill
'mmmmmm::&latibnshipi
^ ^
IliiiiiSii
mmm
mpm
ffioblaid
Illmfcoimtfffaooj
;-;\'1V-:"-;'-"-::.\f,.Vt : - ? . • • . . • -_-•- . : ;"""•"
liiii;'.?-&sXjjr.~~.-z£t:. •••:••"
illiSSSS ;.- |v;;::V '̂VA-'' • -.ft.'.: . .
S f f i S :•••';;: r ri,?,i::.'\ '-;v .-.-.i! , ; ' « i ; . . ; • . ^ . • •;.,
.?|ii(otheaj
SlDil^rtioi^;Svel6ciiy;^;::
s i - . - ; ? J ? / i ^ ••.'•.•!"
• ; S ; _ . ' - ' V ' V ' i : " - . •• - • : ••
••Si':- Vv;?'-?"--'--:.'--'."--:;: i
^ : U - T v J ^ ' ; ..'• '•.-' •''
p . ' : ' ? ' ' ' ' - '•'•'-'• :'
|,^st&
• " • ' ; ' • ' v _ :1 . , ' ""-*;• . " •
'••'.'•".- '-' • - • ' . ' . • •
' • / • - . . • : ' • ' • - ' • - ' • " . - " • -
• • • ' . • . ' ' • ' ' ' •
. Tube
: : -"
• | . . ; . - ; ' " . ' ' ' : •Tube •:
• • ' - ' * • - ' . • " • ' : ' • . ' .
;nisry": "^al iea t - X'•'.iaient £:/:*/-•
- • •• . ,• • ' • • -•
Test,•Atmos-•phere
SteamorOxy-gen-Argon
SteamorOxy-gen-Argon
Sotes
Measured•in'-.;' .Vacuum
MeasuredinVacuum
MeasuredinVacmffl
MeasuredinVacuum
i
• " - ' R e s u l t s ' •• -•'"••••".
Increasing change ofcurve above 1000OC; •
Values are higher ttianin item 14
The curve of the oxidizedspecimen shows a parabolicdevelopment
For average time periodsvalue? are E •> 0.7-0.8
::"';ffSsSSgf ••?;%::;
1600 T
1400
1200 I".
1000 - -
ZIROALGY 4
800 -F
E 600
200
REACTION
Zr-Fe EUTECTIC
TUJDC
•a.
LU
LU o
toUJ
INSIDE TEMP., OF TUBE
„_.„ PRESSURIZED WATER4 0 0 ;• BOILING WATER
'-'- .PRESSURIZED WATERBOILING WATEROUTSIDE TEMP, OF TUBE
REACTOR
REACTOR i 320°C
RT (ROOM TEMP )
TCD•z.DC
cc
1
1200°C
600°C
FIG, 1 LIMITS"OF TEMPERATURE RANGE TO CHECK STRESS/STRAINBEHAVIOR pf 2IRCAL0Y-4 SHEATHS') FOLLOWING,^ LOSS
a.
</3
t o
r 10-2
6S0*C
900 °C
0.2 0.31 0.4 0.5 O.fr - 0,7 0,8^
• f ' 1 0F I G r 2 STRESS/STRAIN CURVES FOR ZfRCALOY-V
. HELIUM6.05 mm"' (2^
tlW ' '
VitoUJ
UJ
V)
z
LL)
a:
ZIRCOKIUM - 0.7 8/0 Sn 775°C
0.3 . 0.4- 0.5>~ 6 ' oJ
FIG. 3 STRESS/STRAIN CURVES FOR A Zr-0.7« Sn ALLOY SHOWING THESFfrECT OF THE filSTOUT!ON VELOCJTY ON THJ -Yl EUD SJRESS__AT 775°C3> J "T>," " -
10"
10°
10-'
*
10"2
FIG.'4
I - , - . , ; , - , • " ' • • • •
. . .:: ;. T
L
1
' • ' . . " • . - " • ' : • ' "
v—\\\\
RCALOY-4
Q
\—A—
\\
• SCOTT6>
O 0EMP-475flS)
I WOODS* >
-
-
' i 1 1 -
—
1
1 '
d-
• , 1
p?11
0 300 600 900, 1200 1500 1
ULTIMATE STRESS OP ZIRCALOY-4 IN RELATION
UNDER ISOTHERMAL CONDITIONS*-5«J>, - - * * - -
-< - tF» i
L v^ J
>
-
T
300 (l 2100 -, ,
TO TEMPERATURE
, i^ F
'I.*
10'
• WADDELL e t . a l l }
O H0BS0N e t . a l 8 >
f> EMMERICH e t . a l 9 >
9 HARDY7
1400
FIG, 5 CIRCUMFERENTIAL ULTIMATE STRESS OF ZIRCALOY-4 AS IT ISAFFECTED BY TEMPERATURE UNDER TRANSIENT CONDITIONS1.7.6
1 rf* 5- L
1
UJ
oeC/5touia:a.
as
CCUJ
a
» Ci QC
>- UJo a.«r ixio i—OS— U4fvj CC
o a.
a ui
I*au* ui
—I UJ
<; u.
eg
ain3
U41
Is3ID
I
\- *I f J i
*
* -;
:ro.zti -
' S3
1
X
c
Ii
i A ffWm ^27
1 :^ 2BA^V^
1
>
•
CIRCUMFF
,.. op
HEAT-UP RATE °C/sO 55.5• 27.8A 13.9A 5.5
-
•RFMTIflL
EXPANSION
•>^ B8 /
82
ZIRCAl OY-4
5 = ^ 9
750 800 900 1000 1100 1200 1300 1400
FIG. 7 MAXIMUM INTERNAL PRESSURES ATTAINED IN ZIRCALOY-4 SHEATH IN RELATION TOTEMPERATURE FOR '.lEAT-UP RATES OF 5.5-55.5°C/s'2>
GEMP-475A5)Q . 0 0 5 m t n " 1
900 "1200 1500 1800 „
F IG. 8 ULTIMATE STRESS OF ZIRCALOY-4 PLATE IN A HELIUM" - ATMOSPHERE2-5^ TN RELATION TO THE'D
'\
X"-
10*
103
I/IV .o
LJ
o.I
uJ
10'
10°
10- I
ZIRCAI.OY-4
1720
aIBID
1475A12.5
0 NEITHER BURST NOR EXPANDED 34% —A BURST _O EXPANSION TO 34%
>1374
15
1437+1770 '374_
a
147
3TEMP.
-flUPTURE EXPANSIONr2*1412
7+17
3+92
A25
13361458
1390*71390*7
1208
A11
A28
12/0 , I U
l" •I2401 1072
1110
8
\036 .
25
1038
o
1106 E
32
973 953
1480A .
11.4 1
130
26 30 ^^
•090 103S*H"A A18 i 18.6
1114
O
33
968A33
1058A 1
0.3 , 0.4 0.5 0.7
OtIOOO|270Oll54
1185 _o
1240 -
o1070
1040
1038
1010
A27
0.8
i j ?5*WYi.4 JH|AJHSJJNDER LNTfT EFFETI " T " F^"PRESSURE'(CONVERTEP TO EFFECTIVE STRESS)"AT"DIFFERENT
HEAT-UP RATES"IN ASTEAM ATMOSPHERE2)
1000
o
LU
LU '
4 500 —
I 'i
'» I
11 ,' 0
—
_ < *
•
—
—• t -
2
^~*>-
JRCALOY-4
• !
9 EMER> e t . a l 1 0 )
o HORSOM1 2 )
" l f c^ — .
800 l * 20 40 feO
; ' . ,sl . HEflT UP RATE IN ° C / s .
', F IG . \6 °, RUPTURF, TEMPERATURt BEHAVIOUR IN RELATION TO HEAT-UP RATE,! > ' PRESSURE10) 1.76 kp/mm2 , AT INTERNAL PRESSURE12> 0 ,07
100
AT INTERNAL
HEPT-UP RATE ( °C/s )
FIG. 11 CIRCUMFERENTIAL EXPANSION AT RUPTURE IN RELATION TO INTERNAL PRESSURE AT HEAT-UP RATES
OF 5 .5 -55 .5°C/s .eb l i )
noo
80
40
20
ZIRCA
• %
r i f i
LOY-4
•
o
I 1 1 1
• GEMP-475A5)
O WOODS4}
QP .- •
. i i r i0' - 500 1000
T [°C3
1500
' f\\. 12 :3L0NGATI0N IN RELATION TO TEMPERATURE FOLLOWING TINSILE TESTS ON- ,"---/ ZIRCALOY-4 PLATE IN AN ARGON ATMOSPHERE
O 0,1 .iJiin"1
0.05 roinr1
• 0.005 min"
FIGl,' 13 ' ELONGATION IN RELATiOW fp TEM||RATURE FOLLOWING TENSILE TESTS IN AN7 ARGON ATMOSPHERE AT DIFFERENT blSTdRTION VELOCITIES2^
10*
noo
FIG. 14 MAXIMUM CIRCUMFERENTIAL EXPANSION IN RELATION TO TEMPERATURE" ' " ArAHEAT-UP~WE ffF TKJ6C/V
0.07
' 1° 't I v ^"-i V~" '
cc
<3
O
T
4
O
o
o
40
oo
ooo
o
)MA
Ul
ISOT
h
z
JURE
PER/
E
o•
135-
0
^ >
CD
UJ
U lv*
CO
z<a.XUJ
H-UJCK
U.
oBE
CO
UJH-Ul
COCOUl
ocCL.
1̂UJ _
— E
' 3
ooooo« ; <. i? g
oo- - 2 o
o in
CO
'-: %
14
a.
fc?
'1,I.
F f t . 16 ULTIMATE STRESS CURVES 1SITH A HEAT^UP RATE OF 1OO°C/s7)
TBP0CH " £ a l l u r * teoperatore
FIG. 17 ULTIMATE STRESS CURVES'4>
BRUCH - failure•temperature
ooo
oLUOS
800
8
oo
BSflfi
S
z
CO
jEUJto•«?
1
o
^™* f ?CJ ECo —
»— u .o
t
J
1—
2o
u.UJ
o
'55
u.
UJ
, - . u.''
ECO
—
—
—
— c
- /
1ZIRCALOY-4
.——•-«
1
/
i \
M
1 ' 1
FIG, 19
100 200 . 300 400 500 600 700
•V T
THERMAL EXPANSION COEFFICIENT OF ZIRCALQY-4 SHEATHS
IN A flAMAi DIRECTION6)
r- ^ •'
>~' • fb v 4 r
O O SCOTT6>
J J FEITH1S>
THERMAL C6NDUCTIVITY-OF ZIRCALOY-4(°. l 5- l B> IN RELATION TO TEMPERATURE
,h .' .'
,!>
0.9
0.7
0.5
0.1800
OXIDIZED
1000
ZJRCALOY-4
OXYGEN SATURATED
NOT OXIDIZED
1200 1400
i-i , FIG. 21 OXIDATION EFFECT ON EMISSIVITY OF ZIRCAL0Y-43>
1.0
0.6
0.4
• 850°CA 1000°CO M00°C0 120Q°C
A 1300°C
ZIRGALOY-4
•20 40
: " •• : ;i-tffl.i
80
FIG. 22 EtiilSSIVITY OF ZlRCALOY-4 AS A FUNCTION OF TIME FOR DIFFERENT STEAM TEMPERATURES2>