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The behavior of PWR fuel rod cladding under LOCA conditions strongly depends on the interactions between the metallurgical evolution (phase transformation) and the thermomechanical behavior at high temperature. FRAMATOME needs for the qualification of advanced zirconium alloys have motivated an extensive study of the phase transformation kinetics and the development of a new test facility, EDGAR-2, to perform thermomechanical tests. The first part of the paper deals with an experimental study and modeling of the α↔β phase transformation kinetics. High-temperature/high-sensitivity calorimeter and fast dilatometer facilities have been used to measure the on-heating α⃗β and on cooling β⃗α phase transformations from near equilibrium conditions up to LOCA conditions (heating-cooling rates up to 100°C/s). The equilibrium fraction of α/β phase as a function of temperature is derived from calorimetric measurements using the Zhu and Devletian model and described using a modified Johnson-Mehl-Avrami equation. Modeling of the α↔β kinetics is given by the differential Holt equation. The present results show that the Holt model gives a good description of the α⃗β kinetics upon heating but is not able to describe accurately the β⃗α phase transformation upon cooling, probably because it does not take into account the occurrence of the partial martensitic transformation during cooling, especially for the higher cooling rates. An important feature of the current study is that, despite the α/β equilibrium temperatures for M4 (ZrSnFeV) and M5 (ZrNbO) alloys being lower than that of Zy-4, for kinetic reasons the α to β phase transformation occurs in the same temperature range for the three alloys in the case of fast thermal transients (i.e., 10°C/s). This observation could be related to the slower thermal diffusion of Nb and V atoms compared to that of Fe and Cr. This slower diffusion explains why the thermalmechanical behavior of new M4 and M5 alloys is quite equivalent to Zy-4 in LOCA conditions. The second part of this paper deals with the thermomechanical tests. The EDGAR-2 test facility performs single rod tests under any internal pressure and clad temperature transients in steam environment. The advanced zirconium alloys M4 and M5 have been tested under steady-state conditions of pressure and temperature, continuous-heating and constant-pressure conditions for various heating rates and pressure, and some LOCA representative pressure temperature transients. The experimental program covers the LOCA conditions, and the rupture occurs from a few seconds up to 2000 seconds. The results are compared with those of the SRA optimized Zy-4 clad using the Monkman-Grant correlation, rupture ductility versus burst temperature, and burst criteria. EDGAR models for the prediction of the evolution of the transformed β-phase volume fraction and of the diametral deformation, time to rupture, and uniform diametral rupture elongation in typical LOCA conditions are derived for advanced alloys from the two parts of this study. These models may easily be implemented in most accident simulation computerized codes for safety analysis.

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A multiscale characterization of the microstructural evolutions taking place in 9 to 12 pct Cr martensitic steels subjected to fatigue and creep-fatigue (CF) loadings is presented. Specimens of a P91 steel subjected to high-temperature cyclic loadings are examined using several experimental techniques. Bright-field transmission electron microscopy (TEM), electron backscattered diffraction (EBSD), and TEM orientation mapping are used to characterize and quantify the microstructural evolutions. A recovery phenomenon consisting of the coarsening of the subgrains and a decrease of the dislocation density is observed. This coarsening is heterogeneous and depends on the strain amplitude and on the applied hold time. The size distribution of subgrains and the dislocation density are measured from bright-field TEM observations. Orientation mapping on scanning electron microscopy (SEM) and TEM show that, even though a correlation between the crystallographic orientation and the recovery phenomenon is highlighted, a complex dependency related to the orientation of neighboring blocks exists. These microstructural observations are consistent with the very fast deterioration of creep properties due to cyclic loadings (reported in the first part of this study).

International audienc

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.

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