Optimization of dissolved hydrogen concentration for mitigating corrosive conditions of pressurised water reactor primary coolant under irradiation, 2; Evaluation of electrochemical corrosion potential

Hata, Kuniki; Hanawa, Satoshi; Chimi, Yasuhiro; Uchida, Shunsuke; Lister, D. H.*

Journal of Nuclear Science and Technology, 14 Pages, 2022/00

https://doi.org/10.1080/00223131.2022.2127955

One of the major subjects for evaluating the corrosive conditions in the PWR primary coolant was to determine the optimal hydrogen concentration for mitigating PWSCC without any adverse effects on major structural materials. As suitable procedures for evaluating the corrosive conditions in PWR primary coolant, a couple of procedures, i.e., water radiolysis and ECP analyses, were proposed. The previous article showed the radiolysis calculation in the PWR primary coolant, which was followed by an ECP study here. The ECP analysis, a couple of a mixed potential model and an oxide layer growth model, was developed originally for BWR conditions, which was extended to PWR conditions with adding Li (Na) and H effects on the anodic polarization curves. As a result of comparison of the calculated results with INCA in-pile-loop experiment data as well as other experimental data, it was confirmed that the ECPs calculated with the coupled analyses agreed with the measured within 100mV discrepancies.

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.

Evaluation of brittle crack arrest toughness for highly-irradiated reactor pressure vessel steels

Iwata, Keiko; Hata, Kuniki; Tobita, Toru; Hirota, Takatoshi*; Takamizawa, Hisashi; Chimi, Yasuhiro; Nishiyama, Yutaka

Proceedings of ASME 2021 Pressure Vessels and Piping Conference (PVP 2021) (Internet), 7 Pages, 2021/07

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.

A Simulation of radiolysis of chloride solutions containing ferrous ion

Hata, Kuniki; Inoue, Hiroyuki*

Journal of Nuclear Science and Technology, 56(9-10), p.842 - 850, 2019/09

https://doi.org/10.1080/00223131.2019.1585986

To investigate the effect of dissolved species from steels on the radiolysis processes of Cl, radiolysis simulations of solutions containing both Cl and Fe were carried out. The results showed that the generation of radiolytic products (HO, O and H) increased mainly by the addition of Fe, and a drop in the pH was caused by the hydrolysis of Fe. This pH drop enhanced the reactivity of Cl with OH, which induced additional generation of HO and O. These results show that low concentrations of Cl (1 10 mol/dm = 35ppm) in the presence of Fe could influence the generation of HO and O during water radiolysis. However, it is considered that these effects of Fe and low concentration of Cl on water radiolysis are less important for corrosion of steels due to the low concentrations of HO and O generated. The other process, such as dissolution of iron enhanced by FeOOH, might predominantly induce corrosion under the conditions of solutions with low concentrations of HO and O.

Influence of applied load on oxidation in the vicinity of crack tips of stainless steel under high temperature water

Kasahara, Shigeki; Chimi, Yasuhiro; Hata, Kuniki; Hanawa, Satoshi

Zairyo To Kankyo, 68(9), p.240 - 247, 2019/09

https://doi.org/10.3323/jcorr.68.240

In order to study environment assisted cracking mechanism of stainless steel under BWR primary coolant condition, effects of applied load on oxidation in the vicinity of crack tips of CT specimens were evaluated. Loaded CT specimens were immersed in an aqueous condition at 290C as a simulated BWR coolant condition, and microstructural observation on oxide near the tips of pre-cracks was carried out. Oxide inner layers, which consisted of fine grain magnetite containing Fe and Cr were formed, and oxide outer layers consisting of large grains of FeO were observed to cover the inner layers. FEM analysis of stress and strain in the loaded CT specimen suggests that both of dislocations due to localized plastic deformation and elastic strain could play important roles to accelerate inner oxide formation in the vicinity of the crack tip of the specimens.

Empirical equations for tensile properties and stress-strain curves of neutron irradiated stainless steels in LWR conditions

Fukuya, Koji*; Fujii, Katsuhiko*; Chimi, Yasuhiro; Hata, Kuniki

Proceedings of 19th International Conference on Environmental Degradation of Materials in Nuclear Power Systems - Water Reactors (Internet), p.523 - 531, 2019/08

For structural integrity assessment on reactor internals of light water reactors, empirical equations of tensile properties as a function of neutron dose, and trend curves of stress-strain relations of neutron-irradiated austenitic stainless steels was proposed by fitting to recently developed database. The data in the database were obtained from reports of national projects in Japan and open literature, which was summarized in the form of data sheets. The empirical equations for tensile properties were formulated by using a saturation-type formulae. The equations were for CW 316 and SA 304/316 stainless steels in the temperature range of 280-350C and the dose range up to 80 dpa. Stress-strain relation curves were reproduced based on the Swift model. Obtained calculated results by the empirical equations and stress-strain relations were reasonably well fitted to experimental data. The effects of composition and cold-working, etc. on tensile properties were discussed.

Reactivity of an antioxidant, edaravone, with reactive oxygen species and its chemical repair properties against oxidative damage on DNA

Hata, Kuniki; Lin, M.*; Yokoya, Akinari*; Fujii, Kentaro*; Yamashita, Shinichi*; Muroya, Yusa*; Katsumura, Yosuke*

Hoshasen Kagaku (Internet), (103), p.29 - 34, 2017/04

Reactivity of edaravone (3-methyl-1-phenyl-2-pyrazolin-5-one), which is known to show high antioxidative properties, with oxidative species, such as hydroxyl radical (OH) and azide radical (N), was investigated by a pulse radiolysis experiment, and generation behavior of edaravone radicals produced through these reactions were observed. It was shown that OH-adducts are produced by the reaction with OH in contrast to the other oxidative radicals, which react with edaravone by an electron transfer reaction. Chemical repair properties of edaravone against DNA lesions produced by reactions of DNA with oxidative species were also investigated by a pulse radiolysis experiment with deoxyguanosine monophosphate (dGMP) and a -radiolysis experiment with plasmid DNA solutions. It was observed that edaravone reduced dGMP radicals just after produced in a dilute aqueous solution and inhibited some base lesions on plasmid DNA more effectively than single strand breaks. These results show that edaravone may protect living system from oxidative stress, such as radiation, by not only scavenging oxidative species but also reducing precursors of DNA leisons.

Evaluation of ECP measured in in-pile environment

Hanawa, Satoshi; Uchida, Shunsuke; Hata, Kuniki; Chimi, Yasuhiro; Kasahara, Shigeki*; Nishiyama, Yutaka

Proceedings of 20th Nuclear Plant Chemistry International Conference (NPC 2016) (USB Flash Drive), 11 Pages, 2016/10

ECP is the exclusive index to evaluate corrosion condition directly at the points of interest in the mixing of neutron and -ray environment. ECP can be calculated through the combination of water radiolysis and ECP model. A water radiolysis model have been applied to experiments performed in in-pile loops in the experimental reactors and applicability was confirmed. An ECP model based on the Butler-Volmer equation was also prepared. ECP of stainless steel was measured under well controlled water chemistry condition in in-pile loop in the Halden reactor, and the model was applied to evaluate ECP measured in the Halden reactor. The measured data were well explained by the water radiolysis calculation and ECP model. Accumulation of in-pile ECP data are expected for further validation of the models.

Simulation for radiolytic products of seawater; Effects of seawater constituents, dilution rate, and dose rate

Hata, Kuniki; Sato, Tomonori; Motooka, Takafumi; Ueno, Fumiyoshi; Hanawa, Satoshi; Kasahara, Shigeki; Tsukada, Takashi

Journal of Nuclear Science and Technology, 53(8), p.1183 - 1191, 2016/08

https://doi.org/10.1080/00223131.2015.1096218