The Role of silicon on solute clustering and embrittlement in highly neutron-irradiated pressurized water reactor surveillance test specimens

Takamizawa, Hisashi; Hata, Kuniki; Nishiyama, Yutaka; Toyama, Takeshi*; Nagai, Yasuyoshi*

Journal of Nuclear Materials, 556, p.153203_1 - 153203_10, 2021/12

https://doi.org/10.1016/j.jnucmat.2021.153203

Solute clusters (SCs) formed in pressurized water reactor surveillance test specimens neutron-irradiated to a fluence of 1 10 n/cm were analyzed via atom probe tomography to understand the effect of silicon on solute clustering and irradiation embrittlement of reactor pressure vessel steels. In high-Cu bearing materials, Cu atoms were aggregated at the center of cluster surrounded by the Ni, Mn, and Si atoms like a core-shell structure. In low-Cu bearing materials, Ni, Mn, and Si atoms formed cluster and these solutes were not comprised core-shell structure in SCs. While the number of Cu atoms in clusters was decreased with decreasing nominal Cu content, the number of Si atoms had clearly increased. The cluster radius () and number density () decreased and increased, respectively, with increasing nominal Si content. The shift in the reference temperature for nil-ductility transition (RT) showed a good correlation with the square root of volume fraction () multiplied by r (). This suggested that the dislocation cutting through the particles mechanism dominates the precipitation hardening responsible for irradiation embrittlement. The negative relation between the nominal Si content and RT indicated that increasing of nominal Si content reduces the degree of embrittlement.

Effect of BC addition on the solidus and liquidus temperatures, density and surface tension of type 316 austenitic stainless steel in the liquid state

Fukuyama, Hiroyuki*; Higashi, Hideo*; Yamano, Hidemasa

Journal of Nuclear Materials, 554, p.153100_1 - 153100_11, 2021/10

https://doi.org/10.1016/j.jnucmat.2021.153100

The effects of BC addition on the solidus and liquidus temperatures of type 316 austenitic stainless steel (SS), and on the density and surface tension of molten SS, were experimentally studied. The solidus temperature of SS-x mass% BC (from 0 to 10) monotonically decreased from 1666 to 1307 K with BC addition. The liquidus temperature had a minimum at around 2.5 mass% BC, and increased with further BC addition up to 10 mass%. The density and surface tension of molten SS-x mass %BC were successfully measured over a wide temperature range (including an undercooling region) via an electromagnetic-levitation technique. The density of each sample decreased linearly with temperature. The density also monotonically decreased with BC content. Although the addition of BC had no clear effect on the surface tension of SS-x mass %BC, sulfur dissolved in SS316L caused a significant decrease in the surface tension.

Viscosities of molten BC-stainless steel alloys

Nishi, Tsuyoshi*; Sato, Rika*; Ota, Hiromichi*; Kokubo, Hiroki*; Yamano, Hidemasa

Journal of Nuclear Materials, 552, p.153002_1 - 153002_7, 2021/08

https://doi.org/10.1016/j.jnucmat.2021.153002

Determining high precision viscosities of molten BC-stainless steel (BC-SS) alloys is essential for the core disruptive accident analyses of sodium-cooled fast reactors and for analysis of severe accidents in boiling water reactors (BWR) as appeared in Fukushima Daiichi. However, there are no data on the high precision viscosities of molten BC-SS alloys due to experimental difficulties. In this study, the viscosities of molten SS (Type 316L), 2.5mass%BC-SS, 5.0mass%BC-SS, and 7.0mass%BC-SS alloys were measured using the oscillating crucible method in temperature ranges of 1693-1793 K, 1613-1793 K, 1613-1793 K, and 1713-1793 K, respectively. The viscosity was observed to increase as the BC concentration increased from 0 to 7.0 mass%. Using the experimental data of the molten 2.5mass%BC-SS and 5.0mass%BC-SS and 7.0mass%BC-SS in the temperature range of 1713-1793 K, the equation for the viscosity of molten BC-SS alloys was determined, and the measurement error of the viscosity of molten BC-SS alloys is less than 8%.

Grain-boundary phosphorus segregation in highly neutron-irradiated reactor pressure vessel steels and its effect on irradiation embrittlement

Hata, Kuniki; Takamizawa, Hisashi; Hojo, Tomohiro*; Ebihara, Kenichi; Nishiyama, Yutaka; Nagai, Yasuyoshi*

Journal of Nuclear Materials, 543, p.152564_1 - 152564_10, 2021/01

https://doi.org/10.1016/j.jnucmat.2020.152564

Reactor pressure vessel (RPV) steels for pressurized water reactors (PWRs) with bulk P contents ranging from 0.007 to 0.012wt.% were subjected to neutron irradiation at fluences ranging from 0.3 to 1.210 n/cm (E 1 MeV) in PWRs or a materials testing reactor (MTR). Grain-boundary P segregation was analyzed using Auger electron spectroscopy (AES) on intergranular facets and found to increase with increasing neutron fluence. A rate theory model was also used to simulate the increase in grain-boundary P segregation for RPV steels with a bulk P content up to 0.020wt.%. The increase in grain-boundary P segregation in RPV steel with a bulk P content of 0.015wt.% (the maximum P concentration found in RPV steels used in Japanese nuclear power plants intended for restart) was estimated to be less than 0.1 in monolayer coverage at 1.010 n/cm (E 1 MeV). A comparison of the PWR data with the MTR data showed that neutron flux had no effect upon grain-boundary P segregation. The effects of grain-boundary P segregation upon changes in irradiation hardening and ductile-brittle transition temperature (DBTT) shifts were also discussed. A linear relationship between irradiation hardening and the DBTT shift with a slope of 0.63 obtained for RPV steels with a bulk P content up to 0.026wt.%, which is higher than that of most U.S. A533B steels. It is concluded that the intergranular embrittlement is unlikely to occur for RPV steels irradiated in PWRs.

Oxygen potential measurement of (U,Pu,Am)O and (U,Pu,Am,Np)O

Hiroka, Shun; Matsumoto, Taku; Kato, Masato; Sunaoshi, Takeo*; Uno, Hiroki*; Yamada, Tadahisa*

Journal of Nuclear Materials, 542, p.152424_1 - 152424_9, 2020/12

https://doi.org/10.1016/j.jnucmat.2020.152424

The measurement of oxygen potential was conducted at 1,673, 1,773, and 1,873 K for (UPuAm)O and at 1,873 and 1,923 K for (UPuAmNp)O by using a thermo-gravimeter and an oxygen sensor. Am inclusion in terms of substituting the U significantly increased the oxygen potential. Similarly, the inclusion of Np as a substitute for U increased the oxygen potential; however, the effect was not as large as that with the Pu or Am addition at the same rate. The results were analyzed via defect chemistry and certain defect formations were suggested in the reducing region and the near-stoichiometric region by plotting the relationship between PO and the deviation from the stoichiometry. The equilibrium constants of the defect reactions were arranged to reproduce the experiment such that Am/Np contents were included in the entropy with coefficients fitting the experimental data.

Atomistic modeling of hardening in spinodally-decomposed Fe-Cr binary alloys

Suzudo, Tomoaki; Takamizawa, Hisashi; Nishiyama, Yutaka; Caro, A.*; Toyama, Takeshi*; Nagai, Yasuyoshi*

Journal of Nuclear Materials, 540, p.152306_1 - 152306_10, 2020/11

https://doi.org/10.1016/j.jnucmat.2020.152306

Spinodal decomposition in thermally aged Fe-Cr alloys leads to significant hardening, which is the direct cause of the so-called 475C-embrittlement. To illustrate how spinodal decomposition induces hardening by atomistic interactions, we conducted a series of numerical simulations as well as reference experiments. The numerical results indicated that the hardness scales linearly with the short-range order (SRO) parameter, while the experimental result reproduced this relationship within statistical error. Both seemingly suggest that neighboring Cr-Cr atomic pairs essentially cause hardening, because SRO is by definition uniquely dependent on the appearance probability of such pairs. A further numerical investigation supported this notion, as it suggests that the dominant cause of hardening is the pinning effect of dislocations passing over such Cr-Cr pairs.

Release behavior of radionuclides from MOX fuels irradiated in a fast reactor during heating tests

Tanaka, Kosuke; Sato, Isamu*; Onishi, Takashi; Ishikawa, Takashi; Hirosawa, Takashi; Katsuyama, Kozo; Seino, Hiroshi; Ohno, Shuji; Hamada, Hirotsugu; Tokoro, Daishiro*; et al.

Journal of Nuclear Materials, 536, p.152119_1 - 152119_8, 2020/08

https://doi.org/10.1016/j.jnucmat.2020.152199

In order to obtain the release rate coefficients from fuels for fast reactors (FRs), heating tests and the subsequent analyses of the fission products (FPs) and actinides that are released were carried out using samples of uranium-plutonium mixed oxide (MOX) fuel pellets irradiated at the experimental fast reactor Joyo. Three heating tests targeting temperatures of 2773, 2973 and 3173 K were conducted using an FP release behavior test apparatus equipped with a high-frequency induction furnace and solid FP sampling systems consisting of a thermal gradient tube (TGT) and filters. Irradiated fuel pellets were placed into a tungsten crucible, then loaded into the induction furnace. The temperature was raised continuously at a heating rate of 10 K/s to the targeted temperature and maintained for 500 s in a flowing argon gas atmosphere. The FPs and actinides released from the MOX fuels and deposited in the TGT and filters were quantified by gamma-ray spectrometry and inductively coupled plasma mass spectrometry (ICP-MS) analysis. Based on the analysis, the release rates of radionuclides from MOX fuels for FR were obtained and compared with literature data for light water reactor (LWR) fuels. The release rate coefficients of FPs obtained in this study were found to be similar to or lower than the literature values for LWR fuels. It was also found that the release rate coefficient data for actinides were within the range of variation of literature values for LWR fuels.

Experimental validation of tensile properties measured with thick samples taken from MEGAPIE target

Saito, Shigeru; Suzuki, Kazuhiro; Hatakeyama, Yuichi; Suzuki, Miho; Dai, Y.*

Journal of Nuclear Materials, 534, p.152146_1 - 152146_16, 2020/06

https://doi.org/10.1016/j.jnucmat.2020.152146

A post-irradiation examination (PIE) was performed on the tensile specimens prepared from the MEGAPIE (MEGAwatt Pilot Experiment) target which were irradiated in flowing lead-bismuth eutectic (LBE). Thicknesses of the specimens were over two times larger than that of the standard specimen. The PIE revealed that the T91 specimens showed a 1.5-2.0 times larger total elongation (TE) compared to the literature values for a specimen with standard t/w (ratio of thickness to width). It could be suggested that the t/w and TE were strongly correlated. Then, we tried to investigate the effects of the t/w on the TE by comparing unirradiated specimens. We found that there was no t/w dependence on the strength and uniform elongation. On the other hand, the TE increases with increasing t/w. Based on the experimental data, we correlated the TE with various specimens t/w to estimate appropriate TE values, including that for the standard specimen.

Post-irradiation examinations of annular mixed oxide fuels with average burnup 4 and 5% FIMA

Cappia, F.*; Tanaka, Kosuke; Kato, Masato; McClellan, K.*; Harp, J.*

Journal of Nuclear Materials, 533, p.152076_1 - 152076_14, 2020/05

https://doi.org/10.1016/j.jnucmat.2020.152076

Anomalous small-angle X-ray scattering (ASAXS) study of irradiation-induced nanostructure change in Fe-ion beam irradiated oxide dispersion-strengthened (ODS) steel

Kumada, Takayuki; Oba, Yojiro; Motokawa, Ryuhei; Morooka, Satoshi; Tominaga, Aki; Tanida, Hajime; Shobu, Takahisa; Konno, Azusa; Owada, Kenji*; Ono, Naoko*; et al.

Journal of Nuclear Materials, 528, p.151890_1 - 151890_7, 2020/01

https://doi.org/10.1016/j.jnucmat.2019.151890

We have developed an anomalous small-angle X-ray scattering (ASAXS) diffractometer in SPring-8 to investigate irradiation-induced nanostructural change in ion-beam irradiated stainless steel. A thermally-aged MA956 stainless steel sample displays power-law scattering that follows the Porod law at the magnitude of scattering vector, Q, below 0.5 nm and an overlapped shoulder around 0.7 nm. After the ion-beam irradiation, the intensity of the shoulder remained unchanged, whereas that of the power-law scattering nearly doubled. This result indicates that none of the structural parameters of the Cr-rich nanoprecipitates, such as the number density, size, and interface roughness, were changed by the irradiation.