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.     

利用神经网络方法研究合金元素对反应堆压力容器钢辐照脆化的影响

反应堆压力容器（RPV）作为压水堆中不可更换的关键部件之一,其安全和稳定是决定反应堆安全经济运行的重要因素。RPV钢的辐照脆化问题是制约RPV在堆内安全服役的关键。RPV钢的辐照脆化与其合金成分关系密切。本文利用神经网络方法研究了RPV钢中关键合金成分（Cu、Mn、Ni、Si、P）与辐照脆化之间的关系。研究结果表明,基于神经网络方法得到合金成分与辐照脆化的关系与传统认知基本一致,辐照脆化对Cu含量最敏感,Cu-Ni对辐照脆化存在协同作用,低Cu合金中Mn-Ni、Ni-Si对脆化存在协同作用。     

Effects of Alloy Elements on Irradiation Embrittlement of Reactor Pressure Vessel Steel: Insights from Neural Network Modelling

As one of the key components that can not be replaced in PWR, the safety and stability of reactor pressure vessel (RPV) steel determine the safety and economy of the reactor. The irradiation embrittlement of RPV steel is the limiting factors for the operation of PWR. The irradiation embrittlement of RPV steel is closely related to its alloy composition. Based on the machine learning method, the relationship between key alloy components (Cu/Mn/Ni/Si/P) and irradiation embrittlement of RPV steel was constructed. The results show that the relationship between the alloy composition and irradiation embrittlement is basically consistent with the traditional cognition. The irradiation embrittlement is sensitive to Cu content, and Cu-Ni has synergistic effect on irradiation embrittlement. In low Cu alloys, Mn-Ni and Ni-Si have synergistic effects on embrittlement.     

Evolution of the nanostructure of VVER-1000 RPV materials under neutron irradiation and post irradiation annealing

A high nickel VVER-1000 (15Kh2NMFAA) base metal (1.34 wt% Ni, 0.47% Mn, 0.29% Si and 0.05% Cu), and a high nickel (12Kh2N2MAA) weld metal (1.77 wt% Ni, 0.74% Mn, 0.26% Si and 0.07% Cu) have been characterized by atom probe tomography to determine the changes in the microstructure during neutron irradiation to high fluences. The base metal was studied in the unirradiated condition and after neutron irradiation to fluences between 2.4 and 14.9 × 10²³ m⁻² (E > 0.5 MeV), and the weld metal was studied in the unirradiated condition and after neutron irradiation to fluences between 2.4 and 11.5 × 10²³ m⁻² (E > 0.5 MeV). High number densities of ∼2-nm-diameter Ni-, Si- and Mn-enriched nanoclusters were found in the neutron irradiated base and weld metals. No significant copper enrichment was associated with these nanoclusters and no copper-enriched precipitates were observed. The number densities of these nanoclusters correlate with the shifts in the ΔT_{41 J} ductile-to-brittle transition temperature. These nanoclusters were present after a post irradiation anneal of 2 h at 450 °C, but had dissolved into the matrix after 24 h at 450 °C. Phosphorus, nickel, silicon and to a lesser extent manganese were found to be segregated to the dislocations.     

Effects of solute elements on hardening and microstructural evolution in neutron-irradiated and thermally-aged reactor pressure vessel model alloys

Nanometer-sized Cu-enriched solute clusters containing Mn, Ni, and Si atoms are considered as the primary embrittling feature in reactor pressure vessel steels. In order to understand the effects of solute atoms Mn, Ni, and Si on hardening and cluster formation, reactor pressure vessel model alloys FeCu, FeCuSi, FeCuNi, and FeCuNiMn were irradiated at 290 °C in a research reactor. Thermal ageing at 450 °C was also carried out to compare with the results in the neutron irradiation. The addition of Mn resulted in larger hardening and higher cluster number density in both thermal ageing and neutron irradiation. In FeCu0.8NiMn alloy, the size distribution of Cu-enriched clusters formed in 62-h thermal ageing (almost peak hardening) was very similar to that formed in the neutron irradiation, indicating they are on a similar growing stage. But the average Ni and Mn composition in clusters formed in neutron irradiation was higher. A good linear relationship between hardening and the square root of cluster volume fraction for both neutron irradiation and thermal ageing data was found.     

Design concept of a small nuclear reactor for large-diameter NTD-Si using a conventional PWR full-length fuel assembly

A design concept for a small nuclear reactor dedicated to large-diameter neutron transmutation doping silicon (NTD-Si) is proposed. Conventional PWR (Pressurized Water Reactor) full-length fuel assembly is used to assure stable and reliable supply of fuel. Criticality, neutron transportation, and core burn-up calculations are performed using the MVP/GMVP II code and MVP-BURN code. The calculation results show that the proposed reactor can be critical over 18 years, and excess reactivity can be suppressed by a combination of Gd₂O₃ burnable poison and soluble boron. Preliminary steady-state single-channel thermal hydraulic analysis showed that heat removal from core is possible under 1 atm operating pressure. Si ingots up to 30 cm in diameter can be irradiated in the reactor irradiation channels, and the uniform irradiation condition can be achieved for a large-diameter Si ingot.     

Effect of the Cu-rich precipitates on thermal conductivity of RPV model steel

Cu-rich precipitates are the important influence factors for the irradiation embrittlement of the reactor pressure vessel model steels. The microstructure of the Cu-rich precipitates could be revealed by mechanical and magnetic properties. In this article, the effect of the Cu-rich precipitates on thermal conductivity was studied. The reactor pressure vessel (RPV) model steels were aged for different time at 500°C. The results show that the thermal conductivity of RPV model steel is first decreased and then increased during the experiment, with a minimum value at 48.33 ± 0.21 W·m^?1·K^?1 after being aged for 200 h. The changing thermal conductivity is decided by the synergistic effect of the following three factors: (1) the crystal structure transformation of Cu-rich precipitates, (2) the orientation relationship between the matrix and Cu-rich precipitates, (3) the content of Cu atoms in the matrix.     

Precipitates induced in austenitic stainless steel by nitrogen injection

Samples of solution-annealed Type 316 stainless steel were irradiated at 803 K with 1.1 MeV nitrogen ions up to 60 dpa at peak and the precipitates induced by the irradiation were examined by electron microscopy. The ratio of injected nitrogen concentration to dpa is estimated to be about 0.3 at%/dpa in an observed area. An ordered γ'-phase of nominally Ni₃Si is identified to form in the sample irradiated to 20 dpa; it shows superlattice spots in the electron diffraction pattern and enrichment of Si and Ni at the precipitate in EDS analysis. In the sample irradiated to 42 dpa, platelet precipitates of 18 nm in average diameter were observed with the number density of 7.4 × 10²¹/m³. The precipitate grows to an average diameter of 28 nm with little change in number density during irradiation from 42 to 60 dpa. The precipitate formed in the sample irradiated to 60 dpa was confirmed to be in the CrN phase with electron diffraction patterns and the spacing of moiré fringes.     

The microstructure of neutron irradiated 20Cr/25Ni/TiN austenitic stainless steel

A nitrided, titanium-stabilised, 20Cr/25Ni austenitic stainless steel was examined in the electron microscope, after 1000 h irradiation at 783 K to doses of 5.0× 10²⁴ n/m² (thermal) and 2.5× 10²⁴ n/m² (fast), in the PLUTO reactor. Microstructures were compared with those of as-received and thermal control samples. The austenitic matrix and M₂₃C₆ particles were free of irradiation-induced damage, while the TiN particles contained loops 2 nm in diameter which coarsened into a network on annealing at 1083 K. Annealing also resulted in a low density of transmutation-induced helium bubbles, ~ 4 nm in diameter, located in precipitate-free regions of grain boundaries. We conclude that 20/25/TiN is relatively unaffected by irradiation at these dose levels and that helium bubble embrittlement is unlikely under normal stresses.     

Stress corrosion cracking on irradiated 316 stainless steel

Tests on irradiation-assisted stress corrosion cracking (IASCC) were carried out by using cold-worked (CW) 316 stainless steel (SS) in-core flux thimble tubes which were irradiated up to 5×10²⁶ n/m² (E>0.1 MeV) at 310°C in a Japanese PWR. Unirradiated thimble tube was also tested for comparison with irradiated tubes. Mechanical tests such as the tensile, hardness tests and metallographic observations were performed. The susceptibility to SCC was examined by the slow strain rate test (SSRT) under PWR primary water chemistry condition and compositional analysis on the grain boundary segregation was made. Significant changes in the mechanical properties due to irradiation such as a remarkable increase of strength and hardness, and a considerable reduction of elongation were seen. SSRT results revealed that the intergranular fracture ratio (%IGSCC) increased as dissolved hydrogen (DH) increased. In addition, SSRT results in argon gas atmosphere showed a small amount of intergranular cracking. The depletion of Fe, Cr, Mo and the enrichment of Ni and Si were observed in microchemical analyses on the grain boundary.     

Neutron induced damage in reactor pressure vessel steel: An X-ray absorption fine structure study

The radiation damage produced in reactor pressure vessel (RPV) steels during neutron irradiation is a long-standing problem of considerable practical interest. In this study, an extended X-ray absorption fine structure (EXAFS) spectroscopy has been applied at Cu, Ni and Mn K-edges to systematically investigate neutron induced radiation damage to the metal-site bcc structure of RPV steels, irradiated with neutrons in the fluence range from 0.85 to 5.0 × 10¹⁹ cm⁻². An overall similarity of Cu, Ni and Mn atomic environment in the iron matrix is observed. The radial distribution functions (RDFs), derived from EXAFS data have been found to evolve continuously as a function of neutron fluence describing the atomic-scale structural modifications in RPVs by neutron irradiations. From the pristine data, long range order beyond the first- and second-shell is apparent in the RDF spectra. In the irradiated specimens, all near-neighbour peaks are greatly reduced in magnitude, typical of damaged material. Prolonged annealing leads annihilation of point defects to give rise to an increase in the coordination numbers of near-neighbour atomic shells approaching values close to that of non-irradiated material, but does not suppress the formation of nano-sized Cu and/or Ni-rich-precipitates. Total amount of radiation damage under a given irradiation condition has been determined. The average structural parameters estimated from the EXAFS data are presented and discussed.     

Irradiation-creep in a materials testing reactor

Helical springs made from titanium, zirconium, Nimonic PE 16 alloy and two austenitic stainless steels namely Firth-Vickers FV 548 and a steel with a composition within the AISI 316 specification have been irradiated in the Dounreay Materials Testing Reactor, at temperatures between 85 °C and 100 °C and to neutron fluences up to about 4 × 10²⁴ m^?2 (> 1 MeV), whilst loaded in tension. Irradiation-creep was observed in all the materials studied and initial strain rates/unit stressneutron ranged from 1 to 1.9 × 10^?35 m⁴/N for Nimonic PE 16 and zirconium respectively. Data obtained from an earlier experiment are re-presented and compared with the present results.Springs which received no heat-treatment after coiling unwound during irradiation at rates which were independent of the supported loads. The phenomenon is attributed to the relaxation of internal stresses (produced during the manufacture of the springs) with an irradiation-creep constant which is an increasing function of prior cold-work.A mechanism of irradiation-creep is proposed which involves the re-arrangement of the dislocation network in a crystal as the dislocations climb by absorbing interstitials produced by irradiation.     

Conceptual design of a small nuclear reactor for large-diameter NTD-Si using short PWR fuel assemblies

A design of a small nuclear reactor for a large-diameter NTD-Si using a conventional Pressurized Water Reactors (PWR) full-length assembly was proposed in previous works. The height of the full-length assembly was 400 cm, and the overall size of the reactor and reflector around the core became large. In addition, the irradiation channel became very long, making handling of the Si ingots in the channel more difficult. The use of a short PWR fuel assembly, with a height of 100 cm, was considered in the current work. With the shorter assembly, the design of the reactor became compact and more practical. Gd₂O₃ and control rods were used to suppress excess reactivity. Criticality, neutron transport, and core burn-up calculations were performed using the MVP/GMVP II code and MVP-BURN code. Steady-state single-channel thermal hydraulic analyses were also performed. The calculation results showed that the reactor could be critical over 1200 days, and that heat removal from core was possible under 1 atm operating pressure. Large-diameter ingot up to 20 cm in height could be doped with sufficient uniformity. The reactor semiconductor production rate was estimated, and varied between 48 tons/year and 70 tons/year for the 50 Ω cm target resistivity depending on the position of the control rod.     

Precipitation in long term thermally aged high copper,high nickel model RPV steel welds

Copper precipitation in irradiated RPV steels is well known to have a deleterious effect on mechanical properties. In order to understand the contribution of thermal ageing to RPV embrittlement a high copper (0.44 at.%), high nickel (1.6 at.%) model RPV weld was thermally aged at 365 °C for times up to 90,000 h. Atom Probe Tomography (APT) was employed to study the precipitation of solutes, primarily copper, nickel, manganese and silicon within the matrix and at grain boundaries. As expected, a high number density of 1–4 nm radius copper rich precipitates was observed. Nickel, manganese and silicon were found at the precipitate matrix interface, and the evolution of the composition of this interface was investigated with ageing time. Segregation of solutes to grain boundaries particularly P, Mo and C was observed, along with enrichments of Ni, Mn and Si, which have not previously been reported in long term thermally aged RPV steels. Preliminary results on several large (>10 nm) Ni–Mn–Si rich features observed at a grain boundary are also presented. These features are rich in Ni (∼30%), Mn (∼15%) and Si (∼12%) and are virtually copper-free.     

Irradiation of U3Si-based compounds in the high-voltage electron microscope

U₃Si and U-3.5 wt% Si-1.5 wt% Al have been irradiated in a high-voltage electron microscope (HVEM) at 500–1180 keV and 300–660 K. The creation of ‘black spot’ damage and removal of deformation twins are observed. Defects about 10 nm diameter averaging 4 × 10²¹ m^?3 are seen only in samples pre-injected with 10^?5 atomic fraction argon and are tentatively identified as voids. The atomic displacement rate during HVEM irradiation of U₃Si-based compounds is about two orders of magnitude higher than that for fuel at power reactor ratings. It is inferred that displacement of silicon, and possible uranium, atoms in U₃Si-based compounds occurred in the HVEM at accelerating voltages in the range 700–1180keV.     

Evaluation of impact properties of weld joint of reactor pressure vessel steels with the use of miniaturized specimens

The effects of specimen size and location of V-notch on the Charpy impact properties were investigated with different sizes of specimens, standard, CVN-1/2, CVN-1/3, and CVN-1.5 mm, for A533B steel, low Mn, high Cu, high phosphorus (P), and high Cu/P steel weld joint. A part of the specimens was irradiated with neutron at 563 K up to 8 × 10¹⁹ n/cm². The heat affected zone (HAZ) specimen is the best in the impact properties among the specimens of base metal, HAZ, and weld metal in the steels with 0.003 wt.% P, while it is the worst in the steels with ～ 0.3 wt.% P. This indicates that the surveillance test of HAZ specimen can be represented by base metal in the case of A533B steels with lower P content (～ 0.003 wt.%). The effects of notch location and chemical contents on ductile to brittle transition temperature (DBTT) are almost independent of specimen size within an error of ±5 K, indicating that the miniaturized Charpy specimens are applicable and effective in the surveillance tests of reactor pressure vessel steel of extended operation period. After irradiation, the highest DBTT was observed for the specimen with V-notch in base metal in the case of A533B steel and high Cu steel with 0.003 wt.% P.     

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.     

Deuterium and helium retentions of V–4Cr–4Ti alloy used as first wall of breeding blanket in a fusion reactor

The deuterium and helium retention properties of V–4Cr–4Ti alloy were investigated by thermal desorption spectroscopy (TDS). Ion energies of deuterium and helium were taken at 1.7 and 5 keV, respectively. The retained amount of deuterium in the sample irradiated at 380 K increased with the ion fluence and was not saturated to fluence of up to 1 × 10²³ D/m². For the irradiation at 773 K, 0.1% of implanted deuterium was retained at the highest fluence. For the helium ion irradiation at room temperature, three groups of desorption peaks appeared at around 500, 850, and 1200 K in the TDS spectrum. In the lower fluence region (<1 × 10²¹ He/m²), the retained helium desorbed mainly at around 1200 K. With increasing fluence, the amount desorbed at 500 K increased. Total amount of retained helium in the samples saturated at fluence up to 5 × 10²¹ He/m² and saturation level was 2.7 × 10²¹ He/m².     

Research of Radioisotope Production with Fast Neutrons, (V)

The preparation of carrier-free ⁶⁵Ni was studied using the reaction ⁶⁵CU(n,/p)⁶⁵.Ni in a nuclear reactor. High purity copper metal was irradiated for 20 min in the JRR-2 reactor. Nickel-65 formed in the copper target was separated by anion exchange method. About 1 μ ⁶⁵Ni per gram of copper was obtained by irradiation with a fast neutron flux of 9×10¹¹ n/cm=²/sec and thermal neutron flux of 3.6 ×10¹³ n/cm²/sec. The specific activity was greater than 3 mc/mg Ni which was over 600 times more than that produced by n, γ) reaction on nickel irradiated at the same time. However, the reaction yield of ⁶⁵Ni per gram of target by the (n, p) reaction was only 1/5,000 of that by the (n, γ) reaction, so that it proved that the method would be unsuitable for practical application.

The cross section for the reaction ⁶⁵Cu(n/p)⁶⁵Ni has been estimated semi-theoretically to be 0.6 mb, an experimental value of 0.2 mb was calculated from the results of the present work.     

In-Pile Eddy Current Test on PWR Fuel Rod Failed by Pellet-Cladding Interaction

Zirconium oxide nodules formed on BWR fuel rods were characterized quantitatively and correlated statistically with the rod operational parameters. Cladding specimens were obtained from fuel rods irradiated in a commercial BWR. Their burnup and fast neutron fluence ranged 17~38 GWd/t and 4×10²⁵~8×10²⁵ n/m², respectively. Characteristic variables of the nodules such as maximum thickness T ^max (μm) were measured on metallographs of the cladding cross sections. These variables were correlated by multiple regression analyses with the operational parameters, such as irradiation time t (d), linear heat rate p (kW/m) and fast neutron flux ø (n/m²-s). For example, the maximum thickness depended on linear heat rate and showed a saturating tendency with burnup B (GWd/t) (T^max ∝ t0.8+0.5 p2.3±0.9 or T ^max ∝B0.8+0.4p1.5±0.5). This decrease of growth rate with irradiation time was interpreted in terms of a microstructure change of Zircaloy-2 during neutron irradiation. Results of transmission microscopy and energy dispersive X-ray spectroscopy indicated that the alloying elements such as Fe, Cr and Ni dissolved from intermetallic precipitates into the base metal during neutron irradiation. Dissolution of the alloying elements might be effective in decreasing the growth rate of nodules.