Abstract

It is now well acknowledged that, after a prototypical loss of coolant accident (LOCA) transient, the resultant mechanical properties of fuel cladding tubes depend strongly on the oxygen content of the residual prior-β layer, as this phase is the only metallic part of the high-temperature oxidized cladding that may show some residual ductility. The aim of this study is to obtain relevant information on the evolution of the mechanical properties, on the one hand, of the prior-β structure as a function of the oxygen content, assuming that there is a critical oxygen content that leads to a ductile-to-brittle failure mode transition at low testing temperatures (20–135°C); and on the other hand, of the α(O) structure as a function of the oxygen content. Sheets of Zircaloy-4, 1 to 3 mm thick, and M5®

M5® is a registered trademark of AREVA-NP.

advanced alloys from AREVA NP have been studied. To obtain different oxygen contents, they were oxidized at high temperature and then annealed under vacuum in order to reduce the oxide layer. Systematic post-treatment measurements of the oxygen concentration and of its homogeneity within the sheet thickness were performed. The different prior-β and α(O) structures thus obtained have homogeneous oxygen content between ∼0.14 wt. % and 0.9 wt. % and ∼2 wt. % and 7 wt. %, respectively. Such oxygen concentration ranges cover the solubility values that are expected in the β phase and in the α(O) phase at high temperatures typical of LOCA transients. Detailed microstructure investigations were subsequently performed on the prior-β structures since it is considered to be the most important layer when regarding the post-quench mechanical behavior of the material. Continuous cooling temperature (CCT) phase diagrams as a function of the oxygen content were established to correctly interpret the results. Electron backscattered diffraction (EBSD) analysis has then allowed the crystallographic orientations and the morphology of prior-β phase sub-grains to be determined. For each considered prior-β grain, it was possible to interpret the data by taking into account the “Bürgers” crystallographic relationship between the parent β phase and the resultant α phase. Complementary electron probe microanalysis (EPMA) was also used. These last experiments have shown a spatial fluctuation of the oxygen content within the microstructure that depends both on the nominal oxygen content and on the cooling rate. Nanohardness measurements were also performed and correlated with this oxygen spatial partition. These measurements proved to be useful for the understanding of the tensile macroscopic mechanical behavior. Finally, on the one hand, tensile tests were performed on prior-β phase at testing temperatures ranging from −100°C up to 260°C. The ductile-to-brittle temperature transition and the mechanical constitutive laws as a function of the oxygen content were then described. These tests show the existence of a ductile-to-brittle failure mode transition at 20°C for a critical oxygen concentration of ∼0.5 wt. %. A detailed fractographic analysis was performed to assess the failure mechanism. On the other hand, four-point bending tests were conducted on α(O) phase at 25°C and 135°C in order to obtain behavior laws. Preliminary finite element calculations were performed to simulate ring compression tests carried out on multi-layered high-temperature oxidized cladding tubes.

1.
Portier
,
L.
,
Bredel
,
T.
,
Brachet
,
J. C.
,
Maillot
,
V.
,
Mardon
,
J. P.
, and
Lesbros
,
A.
, “
Influence of Long Service Exposures on the Thermal-Mechanical Behavior of Zy-4 and M5™ Alloys in LOCA Conditions
,”
Zr in the Nuclear Industry: 14th. Int. Symp.
, 13–17 June
2004
,
Stockholm, Sweden
, ASTM-STP 1467,
ASTM International
,
West Conshohocken, PA
, pp.
896
920
.
2.
Maillot
,
V.
,
Brachet
,
J. C.
,
Portier
,
L.
,
Gilbon
,
D.
,
Lesbros
,
A.
,
Waeckel
,
N.
, and
Mardon
,
J. P.
, “
Hydrogen Content, Pre Oxidation and Cooling Scenario Influences on Post-Quench Mechanical Properties of Zy-4 and M5 Alloys in LOCA Conditions—Relationship with the Post-Quench Microstructure
,”
Zr in the Nuclear Industry: 15th. Int. Symp.
, 24–27 June
2007
,
Oregon, USA
,
ASTM International
,
West Conshohocken, PA
.
3.
Mardon
,
J. P.
,
Charquet
,
D.
, and
Senevat
,
D.
, “
Optimization of PWR Behaviour of Stress-Relieved Zircaloy-4 Cladding Tubes by Improving the Manufacturing and Inspection Process
,”
ASTM STP 1245
,
ASTM International
,
West Conshohocken, PA
, pp.
329
348
.
4.
Stern
,
A.
,
Brachet
,
J. C.
,
Maillot
,
V.
, and
Pineau
,
A.
, “
Metallurgical and Mechanical Behaviour of Zr Base PWR Fuel Cladding Tube After Steam Oxidation at High Temperature to 1200°C
,” Proceedings on Fuel, Control Rod Assembly, Fontevraud, 18–22 Sept.
2006
.
5.
Béchade
,
J. L.
,
Brachet
,
J.-C.
,
Pelé
,
J.
, and
Guilbert
,
T.
, “
Relationships Between ThermoElectric Power (TEP) Values and Crystallographic Texture of Zircaloy-4 Plates
,”
J. Phys. (France)
 0302-0738, Vol.
10
,
2000
, pp.
203
209
.
6.
Bhattacharjee
,
A.
,
Varma
,
V. K.
,
Kamat
,
S. V.
,
Gogia
,
A. K.
, and
Bhargava
,
S.
, “
Influence of Beta Grain Size on Tensile Behavior and Ductile Fracture Toughness of Titanium Alloy Ti-10V-2Fe-3Al
,”
Metall. Mater. Trans. A
 1073-5623, Vol.
37A
,
2006
, pp. 1423.
7.
Semiatin
,
S. L.
,
Kirby
,
B. C.
, and
Salishchev
,
G. A.
, “
Coarsening Behavior of an Alpha-Beta Titanium Alloy
,”
Metall. Mater. Trans. A
 1073-5623 https://doi.org/10.1007/s11661-004-0228-z, Vol.
35
, No.
9
,
2004
, pp.
2809
2819
.
8.
Massih
,
A. R.
,
Andersson
,
T.
,
Witt
,
P.
,
Dahlbäck
,
M.
, and
Limbäck
,
M.
, “
Effect of Quenching Rate on the Beta-to-Alpha Phase Transformation Structure in Zirconium Alloy
,”
J. Nucl. Mater.
 0022-3115 https://doi.org/10.1016/S0022-3115(03)00323-4, Vol.
322
,
2003
, pp.
138
151
.
9.
Holt
,
R. A.
, “
The Beta to Alpha Phase Transformation in Zircaloy 4
,”
J. Nucl. Mater.
 0022-3115 https://doi.org/10.1016/0022-3115(70)90216-3, Vol.
35
,
1970
, pp.
322
334
.
10.
Colin
,
J. C.
, and
Lehr
,
P.
, “
Grain Growth Phenomenon in Zirconium
,” in
Etude sur la Corrosion et la Protection du Zirconium et de ses Alliages
,
M.
Saleese
and
G.
Chaudron
, Eds.,
Centre d’Etudes Nucleaires de saclay, Gif sur Yvette
,
France
,
1966
, pp.
77
96
.
11.
Stern
,
A.
,
Brachet
,
J. C.
,
Maillot
,
V.
, and
Pineau
,
A.
, “
Metallurgical and Mechanical Behaviour of Zr Base PWR Fuel Cladding Tube After Steam Oxidation at High Temperature up to 1200°C
,”
Proceeding on Fuel, Control Rod Assembly
,
Fontevraud, France
, 18–22 Sept.
2006
.
12.
Brachet
,
J. C.
,
Pelchat
,
J.
,
Hamon
,
D.
,
Maury
,
R.
,
Jacques
,
P.
, and
Mardon
,
J. P.
, “
Mechanical Behaviour at Room Temperature and Metallurgical Study of Low-Tin Zy-4 and M5™ (Zr-NbO) Alloys after Oxidation at 1100°C and Quenching
,”
Proceeding on Fuel Behaviour and LOCA Conditions
, 10–14 Sept.
2001
,
IAEA
,
Vienna
, IAEA-TECDOC-1320.
13.
Stern
,
A.
,
Brachet
,
J. C.
,
Barcelo
,
F.
, and
Pineau
,
A.
, “
Beta to Alpha Phase Transformation of Low-Tin Zircaloy-4—Part I—Influence of Cooling Rate and of Oxygen Content on CCT Curves and Resultant Prior-β Microstructure
,”
Metallurgical Transactions
, to be published.
14.
Fréchinet
,
S.
, “
Transformations et Comportements du Zircaloy-4 en Conditions Anisothermes
,” PhD Thesis, Ecole des Mines de Paris,
2001
.
15.
Forgeron
,
T.
,
Brachet
,
J. C.
, et al
, “
Experiment and Modelling of Advanced Fuel Rod Cladding Behaviour Under LOCA Conditions: Alpha-Beta Phase Transformation Kinetics and EDGAR Methodology
,”
Zirconium in the Nuclear Industry: 12th. Int. Symposium
, June 1998,
Toronto, Canada
, ASTM STP 1354,
ASTM International
,
West Conshohocken, PA
,
2000
, pp.
256
278
.
16.
Hunt
,
C. E. L.
, and
Niessen
,
P.
, “
The Continuous Cooling Transformation Behaviour of Zirconium-Niobium-Oxygen Alloys
,”
J. Nucl. Mater.
 0022-3115 https://doi.org/10.1016/0022-3115(71)90003-1, Vol.
38
,
1971
, pp.
17
25
.
17.
Chung
,
H. M.
, and
Kassner
,
T. F.
, “
Embrittlement Criteria for Zircaloy Fuel Cladding Applicable to Accident Situations in Light-Water Reactors: Summary Report
,”
J. Nucl. Mater.
 0022-3115 https://doi.org/10.1016/0022-3115(79)90172-7, Vol.
84
,
1979
, pp.
327
349
.
18.
Dupin
,
N.
,
Ansara
,
I.
,
Servant
,
C.
,
Toffolon
,
C.
,
Lemaignan
,
C.
, and
Brachet
,
J. C.
, “
A Thermodynamic Database for Zirconium Alloys
,”
J. Nucl. Mater.
 0022-3115, Vol.
275
,
1999
, pp.
287
295
.
19.
Brachet
,
J. C.
,
Portier
,
L.
, et al
, “
Influence of Hydrogen Content on the α/β Phase Transformation Temperatures and on the Thermal-Mechanical Behavior of Zy-4, M4 (ZrSnFeV) and M5™ (ZrNbO) alloys during the first phase of LOCA transient
,”
Zr in the Nuclear Industry: 13th. Int. Symp., 10–14 June 2001
,
Annecy, France
, ASTM STP 1423,
ASTM International
,
West Conshohocken, PA
,
2002
, pp.
673
701
.
20.
Woo
,
O. T.
, and
Tangri
,
K.
, “
Transformation Characteristics of Rapidly Heated and Quenched Zircaloy-4-Oxygen Alloys
,”
J. Nucl. Mater.
 0022-3115, Vol.
79
,
1979
, pp.
82
94
.
21.
Hong
,
H. S.
,
Kim
,
S. J.
, and
Lee
,
K. S.
, “
Effect of Oxygen Content on the Beta-Quenched Microstructure of Modified Zircaloy-4
,”
J. Nucl. Mater.
 0022-3115, Vol.
265
,
1999
, pp.
108
111
.
22.
Burgers
,
W. G.
, “
On the Process of Transition of the Cubic-Body-Centered Modification into the Hexagonal-Close-Packed Modification of Zirconium
,”
Physica (Amsterdam)
 0031-8914 https://doi.org/10.1016/S0031-8914(34)80244-3,
1934
, Vol.
1
, pp.
561
586
.
23.
Crépin
,
J.
, “
Etude des Mécanismes de Déformation et d’Endommagement du Zr Grade 702 Traité Béta. Application aux Cordons de Soudure
,” Thesis Polytechnique,
1994
.
24.
Crépin
,
J.
,
Bretheau
,
T.
, and
Caldemaison
,
D.
, “
Cavity Growth and Rupture of Beta-Treated Zirconium: a crystallographic model
,”
Acta Mater.
 1359-6454 https://doi.org/10.1016/S1359-6454(96)00093-6, Vol.
44
,
1996
, pp.
4927
4935
.
25.
Gey
,
N.
,
Humbert
,
M.
,
Gautier
,
E.
, and
Béchade
,
J. L.
, “
Study of the Beta to Alpha Variant Selection for a Zircaloy-4 Rod Heated to the Beta Transus in Presence or Not of an Axial Tensile Stress
,”
J. Nucl. Mater.
 0022-3115, Vol.
328
,
2004
, pp.
137
145
.
26.
Seward
,
G. G. E.
,
Celotto
,
S.
,
Prior
,
D. J.
,
Wheeler
,
J.
, and
Pond
,
R. C.
, “
In-situ SEM-EBSD Observations of the hcp to bcc Phase Transformation in Commercially Pure Titanium
,”
Acta Mater.
 1359-6454 https://doi.org/10.1016/j.actamat.2003.10.049, Vol.
52
,
2004
, pp.
821
832
.
27.
Bunnell
,
L. R.
,
Bates
,
J. L.
, and
Mellinger
,
G. B.
, “
Some High-Temperature Properties of Zircaloy-Oxygen Alloys
,”
J. Nucl. Mater.
 0022-3115 https://doi.org/10.1016/0022-3115(83)90106-X, Vol.
116
,
1983
, pp.
219
232
.
This content is only available via PDF.
You do not currently have access to this content.