Small-angle neutron scattering study on the effect of hydrogen in irradiated reactor pressure vessel steels

Hydrogen uptake can enhance the neutron embrittlement of reactor pressure vessel (RPV) steels. This suggests that irradiation defects act as hydrogen traps. The evidence of hydrogen trapping was investigated using the small-angle neutron scattering (SANS) method on four RPV steels. The samples were examined in the unirradiated and irradiated states and both in the as-received condition and after hydrogen charging. Despite the low bulk content of hydrogen achieved after charging with low current densities, an enrichment of hydrogen in small microstructural defects could be identified. Preferential traps were microstructural defects in the size range of ≈ > 10 nm in the unirradiated and irradiated samples. However, the results do not show any evidence for hydrogen trapping in irradiation defects.     

Study of a neutron irradiated reactor pressure vessel steel by X-ray absorption spectroscopy

Reactor pressure vessel (RPV) reference steel samples submitted to neutron irradiations followed by thermal annealing were investigated by X-ray absorption fine structure (XAFS) spectroscopy. Several studies revealed that Cu and Ni impurities can form nanoclusters. In the unirradiated sample and in the only-irradiated sample no significant clustering is detected. In all irradiated and subsequently annealed samples increases of Cu and Ni atom densities are recorded around the absorber. Furthermore, the density of Cu and Ni atoms determined in the first and second shells around the absorber is found to be affected by the irradiation and annealing treatment. The comparison of the XAFS data at Cu and Ni K-edges shows that these elements reside in arrangements similar to bcc Fe. However, the local irradiation damage yields vacancy fractions which were determined from the analysis of XAFS data with a precision of ∼5%.     

Considerations about irradiation-induced precipitates in Soviet type reactor pressure vessel steels

Small angle neutron scattering (SANS) results on neutron irradiated Fe-Cu are presented and discussed and compared to positron annihilation results. An extended discussion is presented regarding a comparison of earlier positron annihilation and SANS measurements and their interpretation for different Soviet type reactor pressure vessel steels. It is suggested that the irradiation-induced precipitates contain vacancies and might be metal carbides.     

Positron annihilation lifetime study of JRQ and JPA irradiated and annealed reactor pressure vessel steels

The model reactor pressure vessel steels known as JRQ and JPA were manufactured in Japan for the IAEA neutron embrittlement research studies. These model alloys belong to the commercially used steel A533B-1 type and show relatively large changes in mechanical properties after relevant neutron irradiation. The neutron irradiation was performed by different neutron fluxes as well as different neutron fluences (up to about 150 × 10¹⁸ cm⁻² (E > 0.5 MeV)). For a better understanding of the neutron embrittlement, the Positron Annihilation Lifetime Spectroscopy (PALS) technique was applied in 2014. PALS measurement of irradiated specimens was performed using three detectors set-up due to induced ⁶⁰Co radioactivity of the studied specimens. We confirmed that the JPA steel, considered to be high-copper steel, is much more sensitive to defect creation due to neutron irradiation than the low-copper JRQ steel.     

Positron annihilation study of neutron irradiated model alloys and of a reactor pressure vessel steel

The hardening and embrittlement of reactor pressure vessel steels are of great concern in the actual nuclear power plant life assessment. This embrittlement is caused by irradiation-induced damage, and positron annihilation spectroscopy has been shown to be a suitable method for analysing most of these defects. In this paper, this technique (both positron annihilation lifetime spectroscopy and coincidence Doppler broadening) has been used to investigate neutron irradiated model alloys, with increasing chemical complexity and a reactor pressure vessel steel. It is found that the clustering of copper takes place at the very early stages of irradiation using coincidence Doppler broadening, when this element is present in the alloy. On the other hand, considerations based on positron annihilation spectroscopy analyses suggest that the main objects causing hardening are most probably self-interstitial clusters decorated with manganese in Cu-free alloys. In low-Cu reactor pressure vessel steels and in (Fe, Mn, Ni, Cu) alloys, the main effect is still due to Cu-rich precipitates at low doses, but the role of manganese-related features becomes pre-dominant at high doses.     

Embrittlement recovery due to annealing of reactor pressure vessel steels

The irradiation embrittlement of nuclear reactor pressure vessels (RPV) can be reduced by thermal annealing at temperatures higher than the normal operating conditions. The objective of this work was to analyze the pertinent data and develop quantitative models for estimating the recovery in 41 J (30 ft-lb) Charpy transition temperature (TT) and Charpy upper shelf energy (USE) due to annealing. An analysis data base was developed, reviewed for completeness and accuracy, and documented as part of this work. Models were developed based on a combination of statistical techniques, including pattern recognition and transformation analysis, and the current understanding of the mechanisms governing embrittlement and recovery. The quality of models fitted in this project was evaluated by considering both the Charpy annealing data used for fitting and a surrogate hardness data base. This work demonstrates that microhardness recovery is a good surrogate for shift recovery and that there is a high level of consistency between the observed annealing trends and fundamental models of embrittlement and recovery processes.     

Irradiation experiments related to reactor safety in particular pressure vessel steels

The dependence of neutron induced embrittlement of reactor pressure vessel steels on irradiation temperature and neutron exposure was investigated for steels with different copper content. A pronounced increase of the ductile to brittle transition temperature shift with decreasing irradiation temperature was found and quantitatively determined. The influence of the neutron energy spectrum and flux density on the embrittlement was not significant.Rigs for irradiating assemblies of fracture mechanics specimens (CT and WOL) up to 100 mm thickness and also for irradiation experiments under cyclic loading were developed. Irradiation experiments with these rigs are in progress.Creep experiments on canning tubes under different load conditions (uniaxial load and biaxial load under internal and external overpressure) as well as an irradiation device for investigating defective PWR fuel rods are briefly reported.     

Positron affinity for precipitates in reactor pressure vessel steels

The sensitivity of positron annihilation spectroscopy to irradiation-induced precipitates in reactor pressure vessel steels is discussed in the light of recent positron affinity and lifetime calculations. Carbide and nitride precipitates are found to trap positrons only if they contain metal vacancies. Copper precipitates are also attractive to positrons but they are probably detected through annihilation at the precipitate-matrix interface. These findings are related to available experimental data.     

Microstructural aspects of neutron embrittlement of reactor pressure vessel steels - A view from positron annihilation spectroscopy

A comprehensive review of positron annihilation studies of Cr---Mo---V reactor pressure vessel (RPV) steels (Soviet type 15Kh2MFA) in unirradiated and neutron irradiated states is presented. The influences of lattice defects, impurity atom distribution, irradiation temperature, flux and fluence of fast neutrons on positron annihilation parameters, especially during isochronal annealing, are discussed in terms of the positron trapping model. In contrast to the literature, where irradiation-enhanced Cu precipitates and solute coated microvoids are thought to be major defect types responsible for strengthening and hence embrittling of RPV steels, we suggest irradiation-induced precipitates, i.e. probably carbides, to play this role. Possibilities to probe this model are suggested.     

Suggested toughness/temperature relations for reactor pressure vessel steels

Relations are suggested for the means and standard deviations of three toughness measures for reactor pressure vessel steels: static initiation, dynamic initiation, and arrest. All of the relations are of the form: K_Ix = K_LS{1 + exp[(T − [RT_NDT + δT])/T_O]}, where K_Ix is the toughness measure of interest, K_LS is the lower-shelf toughness, T is the temperature, RT_NDT is the reference transition temperature, δT is a temperature shift, and T_O is a temperature which characterizes the breadth of the transition. The mean of K_LS differs for initiation and arrest and its standard deviation accounts for variation within a single heat. The mean of δT differs for all three toughness measures and its standard deviation accounts for heat-to-heat variability. However, it is shown that a value of T_o = 33.2°C can be used for all of the toughness measures. Finally, the lower bound curves of the ASME Boiler and Pressure Vessel Code are shown to represent toughness levels of low probability.     

The properties of WWER-440 type reactor pressure vessel steels cut out from operated units

This paper presents the results of study on radiation degradation occurring in WWER-440 reactor pressure vessel (RPV) steel, using subsize impact specimens (5×5×27.5 mm³). The results of testing trepans and templates cut out from WWER-440 reactor pressure vessels are considered. Ductile-to-brittle transition temperatures (DBTT) obtained using standard Charpy and subsize impact specimens are compared. The relation between these two values is established.     

Stress corrosion cracking of low-alloy reactor pressure vessel steels under boiling water reactor conditions

The stress corrosion cracking (SCC) behaviour of different reactor pressure vessel (RPV) steels and weld filler/heat-affected zone materials was characterized under simulated boiling water reactor (BWR) normal water (NWC) and hydrogen water chemistry (HWC) conditions by periodical partial unloading, constant and ripple load tests with pre-cracked fracture mechanics specimens. The experiments were performed in oxygenated or hydrogenated high-purity or sulphate/chloride containing water at temperatures from 150 to 288 °C. In good agreement with field experience, these investigations revealed a very low susceptibility to SCC crack growth and small crack growth rates (<0.6 mm/year) under most BWR/NWC and material conditions. Critical water chemistry, loading and material conditions, which can result in sustained and fast SCC well above the ‘BWRVIP-60 SCC disposition lines’ were identified, but many of them generally appeared atypical for current optimized BWR power operation practice or modern RPVs. Application of HWC always resulted in a significant reduction of SCC crack growth rates by more than one order of magnitude under these critical system conditions and growth rates dropped well below the ‘BWRVIP-60 SCC disposition lines’.     

Study of atomic clusters in neutron irradiated reactor pressure vessel surveillance samples by extended X-ray absorption fine structure spectroscopy

Copper and nickel impurities in nuclear reactor pressure vessel (RPV) steel can form nano-clusters, which have a strong impact on the ductile-brittle transition temperature of the material. Thus, for control purposes and simulation of long irradiation times, surveillance samples are submitted to enhanced neutron irradiation. In this work, surveillance samples from a Swiss nuclear power plant were investigated by extended X-ray absorption fine structure spectroscopy (EXAFS). The density of Cu and Ni atoms determined in the first and second shells around the absorber is affected by the irradiation and temperature. The comparison of the EXAFS data at Cu and Ni K-edges shows that these elements reside in arrangements similar to bcc Fe. However, the EXAFS analysis reveals local irradiation damage in the form of vacancy fractions, which can be determined with a precision of ∼5%. There are indications that the formation of Cu and Ni clusters differs significantly.     

Cohesive modelling of the fracture of a neutron irradiated pressure vessel steel

The cohesive fracture process zone model was used to account for the neutron irradiation embrittlement of a pressure vessel steel. The tensile testing and fracture of axisymmetrically notched round specimens were numerically modelled assuming a rectangular traction separation law and the irradiation effects were introduced by due modification of this law. The results corroborate those of the experiments performed in a previous work. The cohesive strength and the cohesive energy of the cohesive model were not considered as adjusting parameters, but they were determined from the data of conventional tensile tests and fracture toughness tests on the assumption that the failure of the specimens in these tests also follows the cohesive model.     

Fracture toughness of irradiated and recovered vessel steels

This paper presents the fracture toughness measurements carried out on three vessel steels in an irradiated condition and after a post-irradiation recovery treatment. A statistical approach and the fracture parameters corresponding to two theoretical models of the fracture tests are used for evaluating toughness. Test results show that the neutron fluence gradually transforms the fracture behaviour of the vessel steels from ductile to brittle and seriously reduces their fracture toughness. The effectiveness of the recovery treatment, as evaluated from the toughness measurements, is confirmed, although the efficiency is not the same for the steels and depends on the evaluation parameter except in the case of almost complete recovery. The recovery effect increases with the received neutron fluence if the toughness values after treatment are compared with those in the irradiated condition rather than those in the as received condition.     

Fracture mechanics concepts for evaluation of irradiated reactor pressure vessel material behavior

Within the German research program Forschungsvorhaben Komponentensicherheit (FKS), irradiation experiments were performed with ferritic reactor pressure vessel (RPV) steels and welds. The materials cover a wide range of chemical composition and initial toughness to achieve different susceptibility to neutron irradiation. Different neutron flux was applied and the neutron exposure extended up to 8×10¹⁹ cm⁻². The change in material properties was determined by means of tensile, Charpy impact, drop-weight and fracture mechanics tests, including crack arrest. The results have provided more insight into the acting embrittlement mechanisms and shown that the fracture mechanics concept of the Code provides in general an upper bound for the material which can be applied in the safety analysis of the RPV.     

Magnetic properties of a highly neutron-irradiated nuclear reactor pressure vessel steel

We report results of minor B–H loop measurements on a highly neutron-irradiated A533B-type reactor pressure vessel steel. A minor-loop coefficient, which is a sensitive indicator of internal stress, changes with neutron fluence, but depends on relative orientation to the rolling direction in the low fluence regime. At a higher fluence of ～10 × 10²³ m^?2, on the other hand, an anomalous increase of the coefficient was detected irrespective of the orientation. The results were interpreted as due to competing irradiation mechanisms of the formation of Cu-rich precipitates, recovery process, and the formation of late-blooming Mn–Ni–Si-rich clusters.     

Monitoring the embrittlement of reactor pressure vessel steels by using the Seebeck coefficient

The degree of embrittlement of the reactor pressure vessel (RPV) limits the lifetime of nuclear power plants. Therefore, neutron irradiation-induced embrittlement of RPV steels demands accurate monitoring. Current federal legislation requires a surveillance program in which specimens are placed inside the RPV for several years before their fracture toughness is determined by destructive Charpy impact testing. Measuring the changes in the thermoelectric properties of the material due to irradiation, is an alternative and non-destructive method for the diagnostics of material embrittlement. In this paper, the measurement of the Seebeck coefficient () of several Charpy specimens, made from two different grades of 22 NiMoCr 37 low-alloy steels, irradiated by neutrons with energies greater than 1 MeV, and fluencies ranging from 0 up to 4.5 × 10¹⁹ neutrons per cm², are presented. Within this range, it was observed that increased by ≈500 nV/°C and a linear dependency was noted between and the temperature shift ΔT_41 J of the Charpy energy vs. temperature curve, which is a measure for the embrittlement. We conclude that the change of the Seebeck coefficient has the potential for non-destructive monitoring of the neutron embrittlement of RPV steels if very precise measurements of the Seebeck coefficient are possible.     

The development of radiation embrittlement models for US power reactor pressure vessel steels

A new approach of utilizing information fusion technique is developed to predict the radiation embrittlement of reactor pressure vessel steels. The Charpy transition temperature shift data contained in the Power Reactor Embrittlement Database is used in this study. Six parameters-Cu, Ni, P, neutron fluence, irradiation time, and irradiation temperature - are used in the embrittlement prediction models. The results indicate that this new embrittlement predictor achieved reductions of about 49.5% and 52% in the uncertainties for plate and weld data, respectively, for pressurized water reactor and boiling water reactor data, compared with the Nuclear Regulatory Commission Regulatory Guide 1.99, Rev. 2. The implications of dose-rate effect and irradiation temperature effects for the development of radiation embrittlement models are also discussed.     

Microstructural examination of reactor pressure vessel steels by positron annihilation point of view

This paper presents a comparison of commercially used German and Russian reactor pressure vessel steels from the positron annihilation spectroscopy (PAS) point of view, having in mind knowledge obtained also from other techniques from the last decades.The second generations of Russian RPV steels seems to be fully comparable with German steels and their quality enables prolongation of NPP operating lifetime over projected 40 years. The embrittlement of CrMoV steel is very low due to the dynamic recovery of radiation-induced defects at reactor operating temperatures.