Influence of the crack-tip hydride concentration on the fracture toughness of Zircaloy-4

The influence of a hydrogen concentration gradient at the crack-tip and hydride platelet orientation on the fracture toughness, fracture mode and micromechanisms of a Zircaloy-4 commercial alloy was studied. Fracture toughness was measured on CT specimens and the analysis was performed in terms of J-integral resistance curves at temperatures ranging from 293 to 473 K. Fracture toughness results of specimens containing higher hydrides concentration near the crack-tip region, preferentially orientated in the crack plane, were compared to those obtained from specimens with a homogeneous hydrogen distribution and different platelet orientation; specimens were obtained by charging them in loaded and unloaded condition, respectively. Changes on both macroscopic and microscopic fracture behaviour were observed at temperatures ranging from 293 to 343 K, and the results show the relevance of both hydride concentration and platelet orientation. The existence of a ductile-to-brittle transition is discussed at the light of these new results.     

The influence of hydride blisters on the fracture of Zircaloy-4

The fracture behavior under near plane-strain deformation conditions of Zircaloy-4 sheet containing solid hydride blisters of various depths has been examined at 25 and 300 °C. The study was based on material with either model ‘blisters’ having diameters of 2 and 3 mm or a continuous layer of hydride; in all cases, the substrate material contained discrete hydride precipitates. The fracture strains decrease rapidly with increasing hydride blister/layer depth to levels of about 100 μm deep, and then remain roughly constant. For a given blister depth, the material is significantly more ductile at 300 °C than at room temperature although measurable ductility is retained even at 25 °C and for large blister depths. The material is somewhat more ductile if the hydride is in the form of a blister than in the form of a continuous layer (rim). The hydride blisters/layers are brittle at all temperatures, and crack shortly after yielding of the ductile substrate. Consequently, both experimental evidence and analytical modeling indicate that fracture of the sheet is controlled by the crack growth resistance of the substrate at 25 °C. At elevated temperatures, the hydride particles within the substrate are quite ductile, inhibit crack growth, and failure eventually occurs due to a shear instability.     

Effects of hydrogen content and temperature on fracture toughness of Zircaloy-4

The influence of hydrogen content and temperature on the fracture toughness of a Zircaloy-4 commercial alloy was studied in this work. Toughness was measured on CT specimens obtained from a rolled material. The analysis was performed in terms of J-integral resistance curves. The specimens were fatigue pre-cracked and hydrogen charged before testing them at different temperatures in the range of 293–473 K. A negative influence of the H content on material toughness was important even at very small concentrations, being partially restored when the test temperature increased. Except for some specimens with high H concentration tested at room temperature, the macroscopic fracture behaviour was ductile. The role of Zr-hydrides and Zr(Fe,Cr)₂ precipitates in the crack growth and the dependence with hydrogen content were analysed by observation of the fracture surfaces and determination of the Zr(Fe,Cr)₂ precipitates density on them.     

Identification and quantification of hydride phases in Zircaloy-4 cladding using synchrotron X-ray diffraction

Zirconium hydrides precipitate in fuel cladding alloys as a result of hydrogen uptake from the high-temperature corrosion environment of light water reactors. Synchrotron X-ray diffraction was performed at room temperature on stress-relieved Zircaloy-4 cladding with two distributions of hydrides - (1) uniformly distributed hydrides across the entire cladding wall and (2) hydride rim next to the outer surface. The δ-hydride phase was found to be the predominant hydride phase to precipitate for hydrogen contents up to 1250 weight parts per million (wt ppm). At a higher content, about 3000 wt ppm, although δ-hydride is still the majority phase, a significant amount of γ-hydride is also observed. At even higher hydrogen contents, in excess of approximately 6000 wt ppm, such as can occur in a highly dense hydride layer, peaks associated with the ε-hydride phase are also observed in the diffraction pattern. The volume fraction of hydrides was estimated as a function of hydrogen content using the integrated intensities of select diffraction peaks corresponding to the α-Zr matrix and the hydride phases. These estimated values agree well with calculated values from the independently measured concentrations. The results of this study indicate that hydride precipitation in Zircaloy-4 is a complex process of evolving hydride phases with increasing local hydrogen content.     

Stress and temperature-dependent hydride reorientation of Zircaloy-4 cladding and its effect on the ductility degradation

A hydride reorientation can deteriorate the mechanical ductility of spent fuel cladding and make it more susceptible to failure. Therefore, an evaluation of the reorientation under dry storage conditions and their effects on the cladding ductility are critical issues in terms of the regulation criteria. In this work, biaxial stress was applied to Zircaloy-4 cladding by pressurizing Ar gas. The study showed that the hydride reorientation can occur at around 60 and 80 MPa at 400 and 300 °C, respectively. The ring compression test at room temperature showed that the ductility decreases with an increase in radial hydride quantity: Fl(45) and radial hydride continuity factor. In addition, a significant hydride reorientation can occur at high temperature conditions even if the hoop stress is equal to or less than 90 MPa which can bring a significant ductility degradation.     

Generalized creep model of Zircaloy-4 cladding tubes

Zircaloy-4 cladding tubes with different area reductions at the final cold working were subjected to creep testing at temperatures of 350 to 500°C. The creep testing was carried out mainly at the biaxial stress state. The creep rate and creep strain of the Zircaloy-4 cladding tube increased with increasing area reduction at the final cold working. The creep model was derived to cover the effect of area reduction and then verified by using supplementary creep data obtained at 350°C and 138 MPa. Furthermore, this generalized creep model was verified to well describe the thermal creep of Duplex tubes and low Sn Zircaloy-4 tubes. The creep rate of Zircaloy-4 cladding tubes followed the exponential stress dependence, not the power law creep. The creep activation energy was determined to be 60 kcal/mol, leading to the conclusion that creep is controlled by dislocation creep. Thus, it is suggested that the increase of creep rates and creep strains with the increase in cold working is due to an enhanced climb rate arising from the increased concentration of vacancy.     

In situ crack growth observation and fracture toughness measurement of hydrogen charged Zircaloy-4

The effect of hydrogen on the fracture behaviour of a Zircaloy-4 alloy was analysed performing simultaneous fracture mechanics tests of small SE(B) specimens and in situ observation of crack initiation and propagation inside the chamber of a scanning electron microscope. Load and displacement were continuously measured and J_IC, J-R curves and CTOD determinations were obtained. Detailed images of the zone close to the crack tip were taken and the resistance to crack growth was correlated with hydrogen content and hydride morphology. The size and orientation of hydride precipitates showed an important influence on the fracture process. A good agreement with results obtained using standard CT specimens was met.     

Effect of radial hydrides on the axial and hoop mechanical properties of Zircaloy-4 cladding

The effect of radial hydrides on the mechanical properties of stress-relief annealed Zircaloy-4 cladding was studied. Specimens were firstly hydrided to different target hydrogen levels between 100 and 600 wt ppm and then thermally cycled in an autoclave under a constant hoop stress to form radial hydrides by a hydride reorientation process. The effect of radial hydrides on the axial properties of the cladding was insignificant. On the other hand, the cladding ductility measurements decreased as its radial hydride content increased when the specimen was tested in plane strain tension. A reference hydrogen concentration for radial hydrides in the cladding was defined for assessing the fuel cladding integrity based on a criterion of the tensile strength 600 MPa. The reference hydrogen concentration increased with the specimen (bulk) hydrogen concentration to a maximum of ∼90 wt ppm at the bulk concentration ∼300 wt ppm H and then decreased towards higher concentrations.     

The effect of hydride morphology on the failure strain of stress-relieved Zircaloy-4 cladding with an outer surface pre-crack under biaxial stress states

Hydride precipitates are considered to affect cladding integrity adversely during pellet-cladding mechanical interaction (PCMI) in a reactivity-initiated accident (RIA). This study aims to clarify the role of hydride precipitates in cladding failure under the biaxial stress condition. A displacement-controlled loading method was applied with a biaxial expansion-due-to-compression (biaxial-EDC) test apparatus to maintain a constant ratio of axial to hoop strains. The tests were conducted at room temperature on unirradiated stress-relieved Zircaloy-4 cladding tube samples with various hydrogen contents, pre-crack depths, and strain ratios. The amount and distribution of hydride precipitates (hydride morphology) were evaluated quantitatively and hydrogen content was measured to assess its effect on the decrease in outer surface hoop strain at failure (failure strain) of the samples. The decrease in failure strain of the hydrided sampleswas found to be more significant under lower strain ratios in the samples with shallower pre-crack. The failure strain of sample tended to be more sensitive to hydrogen content under the strain ratio with a higher axial component in the case of samples with hydrogen contents higher than ~150 wppm. This tendency might be explained by a scenario that considered the formation of micro-cracks in the hydride precipitates during the EDC test.     

Circumferential creep properties of stress-relieved Zircaloy-4 and Zr-Nb-Sn-Fe cladding tubes

In this study, the circumferential creep behaviors of stress-relieved Zircaloy-4 and Zr-Nb-Sn-Fe alloys were investigated. The out-of reactor creep resistance of Zircaloy-4 was found to be better than that of the Zr-Nb-Sn-Fe alloy in the temperature and stress range of this study, suggesting that the solution strengthening effect of Sn is more effective in restraining dislocation motion than the precipitate strengthening effect of Nb. Zircaloy-4 and Zr-Nb-Sn-Fe have stress exponents between 6.5 and 7.5 in the lower stress region. The stress exponent decreased to about 3 for Zircaloy-4 and to about 4.2 for Zr-Nb-Sn-Fe in the high stress region. The activation energy increased from 240 to 270 kJ/mol for Zircaloy-4 and Zr-Nb-Sn-Fe as the applied stress increased from 80 to 150 MPa. The creep activation energy observed in this study is close to those of creep for Zircaloy-2 and Zr. The lower stress exponent in the higher stress region for Zircaloy-4 with a relatively higher Sn content compared to Zr-Nb-Sn-Fe alloy may be supported by the fact that the drag force of Sn atoms acting on dislocations increases with increase of Sn content. Larson-Miller Parameter (LMP) decreased with the increase of applied stress, and Zircaloy-4 has a higher LMP than the Zr-Nb-Sn-Fe alloy, compatible with the lower creep rate in Zircaloy-4.     

Failure behavior of Zircaloy-4 cladding after oxidation and water quench

Simulated LOCA (loss of coolant accident) tests and subsequent mechanical tests on Zircaloy-4 cladding were carried out to evaluate the failure behavior of the cladding. Zircaloy-4 claddings were oxidized in a steam environment from 900 to 1250 °C for a given time period followed by a flooding of cool water to simulate LOCA tests. After the simulated LOCA test, the ductility of the oxidized cladding was evaluated by mechanical tests such as ring compression test and 3-point bend test. Evaluation of the absorbed contents such as hydrogen and oxygen were also carried out. The results showed that Zircaloy-4 cladding failed during thermal shock when the ECR (equivalent cladding reacted) value exceeded 20%. Lower boundary of brittle failure at thermal shock corresponds to 20% of ECR line calculated by the Baker-Just equation regardless of test temperature. On the other hand, boundary of ductile failure by the mechanical test did not followed after the ECR line. It rapidly decreased above 1000 °C to show that all Zircaloy-4 claddings behaved brittle fracture above 1150 °C when it oxidized at 300 s. Microstructural analysis revealed that boundary of ductile failure by the mechanical test fitted well when the absorbed oxygen content inside the prior-β layer was below 0.5 wt%.     

Improved-EDC tests on the Zircaloy-4 cladding tube with an outer surface pre-crack

In order to investigate the failure behavior of fuel cladding under a reactivity-initiated accident (RIA) condition, biaxial stress tests on unirradiated Zircaloy-4 cladding tube with an outer surface pre-crack were carried out under room temperature conditions by using an improved Expansion-Due-to-Compression (improved-EDC) test method which was developed by Japan Atomic Energy Agency. The specimens with an outer surface pre-crack were prepared by using Rolling-After-Grooving (RAG) method. In each test, a constant longitudinal tensile load of 0, 5.0 or 10.0 kN was applied along the axial direction of specimen, respectively. All specimens failed during the tests, and the morphology at the failure opening of the specimens was similar to that observed in the result of post-irradiation examinations of high burnup fuel which failed during a pulse irradiation experiment. The longitudinal strain (?_tz) at failure clearly increased with increasing longitudinal tensile loads and the circumferential strain (?_t?) at failure significantly decreased in the case of 5.0 and 10.0 kN tests, compared with the case of 0 kN tests. From these tests, the data of cladding failure were obtained in the range of strain ratio (?_tz/?_t?) between about ?0.6 and 0.7: this range of strain ratio covers the range between about 0.0 and 0.7 which is estimated in the case of RIA-simulated test. It is considered that the data obtained in this study can be used as a fundamental basis for quantifying the failure criteria of fuel cladding under a biaxial stress state.     

Stress-induced reorientation of hydrides and mechanical properties of Zircaloy-4 cladding tubes

Stress-induced reorientation of hydrides and its effect on the stress–strain response of Zircaloy-4 cladding tubes were investigated. The reorientation of hydrides along the radial direction was most pronounced if the tube was cooled from 300 to 200 °C under circumferential loading. Reorientation occurred much less frequently at either higher (cooled from 400 to 300 °C) or lower (cooled from 200 to 100 °C) temperature range. The population of radial hydrides in R43H7 (which was cooled from 400 to 300 °C and maintained at 300 °C for 7 h) increased drastically during annealing at 300 °C, suggesting time dependent stress-aided dissolution of circumferential hydrides and reprecipitation of radial hydrides. The drastic decrease of the strength and the complete loss of the ductility were observed in R32AC and R43H7.     

Effects of oxide and hydrogen on the circumferential mechanical properties of Zircaloy-4 cladding

Mechanical properties of Zircaloy-4 cladding were evaluated by the ring tension test to simulate the cladding behavior under the reactivity-initiated accident (RIA) in a high burnup environment. Zircaloy-4 cladding was controlled to have a hydrogen content up to 1000 ppm and a oxide thickness up to 100 μm, followed by a circumferential ring tension test with a strain rate in the range of 0.01 and 1/s. The results showed that both the ductility and toughness decreased as the hydrogen content and the oxide thickness increased. Hydride inside the cladding played an important role in the brittle failure mechanism by a decohesion between the hydride and the metal matrix as well as a preferential fracture of the brittle hydride. Surface oxide also affected the mechanical property such as a reduction of the load bearing area, stress relieving effect, and so on. Correlation between the in-reactor RIA parameters such as the fuel enthalpy and out-reactor mechanical toughness was postulated and it was concluded that the change of the mechanical toughness caused by the oxide was more significant than that by the hydrogen.     

Zircaloy-4 cladding corrosion model covering a wide range of PWR experiences

A phenomenological corrosion model for Zircaloy-4 cladding was developed by focusing on the effect of the metallurgy of cladding and the water chemistry combined with the thermo-hydraulic conditions. The metallurgical effect was formulated by considering the Sn content in the cladding and the heat treatment of the cladding. Concerning the effect of the water chemistry, it is assumed that lithium and boron have an influence on the corrosion under the condition of subcooled void formation on the cladding surface. The developed corrosion model was implemented in a fuel performance code, COSMOS, and verified using the database obtained for the UO₂ and MOX fuel rods irradiated in various PWRs. It was elucidated that the corrosion by lithium was enhanced in the case where the fuel rods were irradiated with a high linear power so that a significant subcooled void could be formed on the cladding surface. On the other hand, there was no evidence of the lithium effect even though its concentration was high enough if the void in the coolant was negligible. This result shows that the acceleration of corrosion by an increased lithium concentration occurs only when subcooled voids are formed on the cladding surface. In addition, the comparison between the measurement and the prediction for the MOX fuel rods indicates that no distinguishable difference is found in the corrosion behavior between the MOX and the UO₂ fuels as expected.     

Low-cycle fatigue properties of Zircaloy-2 cladding

The low-cycle fatigue properties of specimens of recrystallized Zircaloy-2 cladding have been investigated using a bend-testing rig at 20, 250, 300, 350 and 400°C. The results followed the Coffin-Manson law for low-cycle fatigue at all temperatures. Irradiated specimens were tested at 20 and 300°C. At 20°C the life of irradiated specimens was shorter than that of unirradiated specimens, whilst at 300°C the irradiated specimens fall on the same Coffin-Manson plot as the unirradiated specimens. Generally the number of cycles to failure in the present investigation was a factor of three smaller than in other investigations using push-pull testing machines. Fracture surfaces were investigated in a scanning electron microscope in order to determine the characteristic features of low-cycle fatigue failures. Twins found along the path of the fatigue cracks were explained as being a consequence of the cracks rather than as promoters of crack propagation.     

A creep rupture criterion for Zircaloy-4 fuel cladding under internal pressure

The usual criterion which limits the cladding strain to 0.01 to prevent the creep rupture under internal pressure seems too conservative for application to transport and interim storage. So we have analysed CEA’s data on this subject for CWSR Zircaloy-4 in order to find a less conservative criterion. Temperatures between 350 and 470 °C were studied for stresses between 100 and 550 MPa, according to the irradiation level from 0 to 9.5 × 10²⁵ n m⁻². Except for high stressed irradiated material (because of low ductility), the plastic instability appears as the major mechanism of rupture. For the unirradiated material, it is essentially due to the stress increase with strain. This instability is accelerated by annealing for the irradiated one at moderate or low stress. From these considerations, we propose a new rupture criterion for CWSR Zircaloy-4 cladding submitted to internal pressure, for both unirradiated and irradiated materials.     

Fracture behavior of recrystallized and stress-relieved Zircaloy-4 cladding under biaxial stress conditions

Pellet-cladding mechanical interaction (PCMI) under reactivity-initiated accident conditions may lead to failure of high-burnup fuel rods. The biaxial stress states of Zircaloy cladding tubes induced by PCMI loading presumably makes the tubes more susceptible to failure. To clarify the influence of the anisotropic mechanical properties of Zircaloy cladding tubes on their fracture behavior under biaxial stress conditions, biaxial tensile tests were performed, and the measured stresses and strains were converted to reduced parameters such as equivalent strain, equivalent stress, and stress triaxiality by using the anisotropic constants of the Hill yield function derived in our previous study. The minimum fracture strains of recrystallized (RX) and stress-relieved (SR) specimens were located where the stress ratio of axial to circumferential is 0.75. The equivalent plastic fracture strains tended to decrease monotonously with increasing stress triaxiality, which is a typical trend observed in ductile fracture, in the range of 0.65–0.78 for both specimens. In the case of SR specimens, however, the analysis with stress triaxiality did not reduce the fracture strains well to a single trend curve, showing that another influential factor is required such as an anisotropic fracture behavior or a plastic behavior deviated from that predicted by the yield function.     

Creep anisotropy of Zircaloy-2 cladding during irradiation

A procedure is described to determine the axial-radial and circumferential-radial contractile strain ratios (the R and P factors in the Backofen modified von Mises-Hill yield criterion) from post-irradiation dimensional measurements of Zircaloy-2 of boiling water reactor fuel rods, tie rods and water rods. Values for R and P have been determined for textured cold-worked stress-relieved (CWSR) Zircaloy-2 cladding. A sensitivity study was performed to evaluate the effects of measurement uncertainties on the derived values of R and P and on the engineering application of the model to predict the in-reactor deformation of CWSR Zircaloy-2 cladding.     

织构对Zr-4合金循环变形行为的影响

研究了织构对Zr-4合金循环变形行为的影响及其作用机制。结果表明，(1)合金的低周疲劳寿命遵循Coffin—Manson关系N^(β)f△εpC。在给定△εp时，轧向的寿命比横向的长。随△εp的降低，两个方向的疲劳寿命差别增大；(2)在低应变幅，合金表现为循环软化直至疲劳破坏在高应变幅，循环变形的初期表现为循环硬化，随后是循环软化直至疲劳破坏在应变幅恒定时，随着循环次数的增加，晶粒发生转动，使晶粒有更高的Schmid因子；(3)半寿命时的σs随εp的变化遵循乘幂关系σs=K^sε(^n^s),σid随σp的变化则遵循对数关系σid=K^blnεp Cb；(4)轧向和横向之间循环变形行为的差别是由于织构效应的缘故。