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.

Geochemical factors for secondary mineral formation at naturally-occurring hyperalkaline spring in Oman ophiolite

Anraku, Sohtaro; Matsubara, Isamu*; Morimoto, Kazuya*; Sato, Tsutomu*

Nendo Kagaku, 55(2), p.17 - 30, 2017/00

http://doi.org/10.11362/jcssjnendokagaku.55.2_17

Anionic radionuclides are important for the long-term safety assessment of Japanese transuranic (TRU) waste disposal facilities. Degradation of cementitious materials used to construct the TRU waste disposal facilities, however, can produce a hyperalkaline leachate and so it is necessary to understand the reaction mechanisms that will control the behavior and fate of anionic radionuclides under these hyperalkaline conditions. An excellent natural analogue site to study relevant reaction mechanisms is provided in Oman where hyperalkaline spring waters (pH 11) from serpentinized peridotites discharge into moderately alkaline rivers. Aragonite was found in all secondary mineral samples, with accessory minerals of calcite, layered double hydroxide (LDH) and brucite. LDH was observed at the high Al concentration springs and brucite at the low Al concentration springs. Calcite was only found close to the springs. Distal calcite formation was inhibited due to high Mg concentrations in the river water. The spatial distribution of minerals therefore implicates the importance of the mixing ratio of spring to river water and the relative chemical compositions of the spring and river waters. Supporting mixing model calculations could successfully reproduce the precipitation of aragonite and LDH. The observed decrease in Ca concentration could be explained by aragonite precipitation. pH exerted a strong control on the precipitation of LDH and so too, therefore, on Al concentration. In the mixing water experiments containing up to 40% river water, LDH and brucite were both oversaturated, but brucite was not always identified by XRD. The possible inhibition of brucite by LDH precipitation was an unexpected result.

Impact assessment of the forest fires on Oarai Research and Development Center Waste Treatment Facility

Shimomura, Yusuke; Hanari, Akira*; Sato, Isamu*; Kitamura, Ryoichi

JAEA-Technology 2015-062, 47 Pages, 2016/03

JAEA-Technology-2015-062.pdf:1.85MB

In response to new standards for regulating waste management facilities, it was carried out impact assessment of forest fires on the waste management facilities existed in Oarai Research and Development Center of Japan Atomic Energy Agency. At first, a fire spread scenario of forest fires was assumed. The intensity of forest fires was evaluated from field surveys, forest fire evaluation models and so on. As models of forest fire intensity evaluation, Rothermel Model and Canadian Forest Fire Behavior Prediction (FBP) System were used. Impact assessment of radiant heat to the facilities was carried out, and temperature change of outer walls for the assumed forest fires was estimated. The outer wall temperature of facilities was estimated around 160C at the maximum, it was revealed that it doesn't reach allowable temperature limit. Consequently, it doesn't influence the strength of concrete. In addition, a probability of fire breach was estimated to be about 20%. This report illustrates an example of evaluation of forest fires for the new regulatory standards through impact assessment of the forest fires on the waste management facilities.

Development of evaluation procedure of vapor species transition behavior; Investigation of applicable measurement technology for estimation of chemical form and physical parameters, and validity verification

Takai, Toshihide; Sato, Isamu*; Yamashita, Shinichiro; Furukawa, Tomohiro

JAEA-Technology 2015-043, 56 Pages, 2016/02

JAEA-Technology-2015-043.pdf:23.14MB

Fundamental research on FP-chemistry for fission product release behaviors under severe accident was carried out for reinforcement of source term evaluation, and implementation of the 1F decommissioning R&D project. There were subjects to clarified (1) FP chemistry behavior between vapor species release and aerosol formation and (2) physical parameters which would be affect subsequent aerosol's chemical behavior, for improvement of FP transport model. Applicability of measuring/analyzing techniques presently used was studied for evaluating foregoing properties. And the validity was verified by trial measurements. In conclusion, Raman spectrometry and high temperature X-ray diffraction were hopeful to determine FP-chemical form against vapor/aerosol species and aerosol species, respectively. Combination use of cascade impactor and scanning type electron microscope with energy-dispersive X-ray spectrometry was hopeful to determine physical parameters of aerosol.

Thermophysical properties of americium-containing barium plutonate

Tanaka, Kosuke; Sato, Isamu; Hirosawa, Takashi; Kurosaki, Ken*; Muta, Hiroaki*; Yamanaka, Shinsuke*

Journal of Nuclear Science and Technology, 52(10), p.1285 - 1289, 2015/10

https://doi.org/10.1080/00223131.2015.1029554

Polycrystalline specimens of americium-containing barium plutonate have been prepared by mixing the appropriate amounts of (PuAm)O and BaCO powders followed by reacting and sintering at 1600 K under the flowing gas atmosphere of dry-air. The sintered specimens had a single phase of orthorhombic perovskite structure and were crack-free. The elastic moduli were determined from the longitudinal and shear sound velocities. The Debye temperature was also determined from the sound velocities and lattice parameter measurements. The thermal conductivity was calculated from the measured density at room temperature, literature values of heat capacity, and thermal diffusivity measured by laser flash method in vacuum. The thermal conductivity of americium-containing barium plutonate was roughly independent of the temperature and was almost the same magnitude as that of BaPuO and BaUO.

Influence of boron vapor on transport behavior of deposited CsI during heating test simulating a BWR severe accident condition

Sato, Isamu; Onishi, Takashi; Tanaka, Kosuke; Iwasaki, Maho; Koyama, Shinichi

Journal of Nuclear Materials, 461, p.22 - 28, 2015/06

https://doi.org/10.1016/j.jnucmat.2015.02.032

We observed one of the simplified processes by conducting primitive experiments. CsI was heated at 1323 K to be vaporized and deposited on sampling parts with a temperature range of 1023 - 423 K and then BO was vaporized at 1973 K to be reacted with Cs/I there. After heating tests, each sampling part was soaked into alkali water to dissolve the surface-deposits for ICP-MS analysis. The results showed that CsI deposited at the sampling parts kept above approx. 850 K was striped by BO vapour. This behaviour will be thermodynamically discussed to study the Cs/I/B chemistry in the severe accidents.

Penetration behavior of water solution containing radioactive species into dried concrete/mortar and epoxy resin materials

Sato, Isamu; Maeda, Koji; Suto, Mitsuo; Osaka, Masahiko; Usuki, Toshiyuki; Koyama, Shinichi

Journal of Nuclear Science and Technology, 52(4), p.580 - 587, 2015/04

https://doi.org/10.1080/00223131.2014.963725

Penetration behavior of radionuclides such as Cs into dried concrete material, dried mortar material and epoxy paint for a few dozen days was observed using a solution containing fission products extracted from irradiated fuels to obtain fundamental information on the radionuclide penetration rate and depth. Hardly any radionuclides could penetrate into the epoxy paint. The radionuclide solution penetrated into concrete and mortar materials to a depth of a few millimeters for a few dozen days. The penetration behavior observed near the surface of concrete and mortar materials was similar to the diffusion of nuclides in media such as water-saturated concrete, bentonite and cement materials.

Distribution of radioactive nuclides of boring core samples extracted from concrete structures of reactor buildings in the Fukushima Daiichi Nuclear Power Plant

Maeda, Koji; Sasaki, Shinji; Kumai, Misaki; Sato, Isamu; Suto, Mitsuo; Osaka, Masahiko; Goto, Tetsuo*; Sakai, Hitoshi*; Chigira, Takayuki*; Murata, Hirotoshi*

Journal of Nuclear Science and Technology, 51(7-8), p.1006 - 1023, 2014/07

https://doi.org/10.1080/00223131.2014.915769

Since the start of the severe accident at the Fukushima Daiichi Nuclear Power Plant in March 2011, concrete surfaces within the reactor buildings have been exposed to radioactive contaminants. Released radiation sources still remain too high to permit entry into some areas of the RBs to allow the damage to be assessed and to allow carrying out the restoration of lost safety functions, decommissioning activities, etc. In order to clarify the situation of this contamination in the RBs, 18 samples were subjected to analyses to determine the surface radionuclide concentrations and to characterize the radionuclide distributions in the samples. Decontamination tests on the sample of Unit 2 were conducted to reduce the levels of radioactivity present near the sample surface. As a result of the tests, the level of radioactivity of the sample was reduced with the removal of 97% of the contamination present near the sample surface.

Penetration behavior of solution containing radioactive nuclides into floor and wall materials

Usuki, Toshiyuki; Sato, Isamu; Suto, Mitsuo; Maeda, Koji; Osaka, Masahiko; Koyama, Shinichi; Tokoro, Daishiro*; Sekioka, Ken*; Ishigamori, Toshio*

JAEA-Testing 2014-001, 29 Pages, 2014/05

JAEA-Testing-2014-001.pdf:5.33MB

The penetration tests with solution containing radioactive nuclides were experimented to understand basic data for floor and wall materials of Fukushima Daiichi reactor buildings. The solution prepared from irradiated fuels was used as solution containing radioactive nuclides. The solution was applied to surface of epoxy paint, dried concrete and mortar used as specimens. Dose-rate profiles of direction of depth were given by radiation measurement and grinding of the specimens. The penetrations of radioactive nuclides for epoxy paint specimens were not clearly observed and the penetration depths would be within 0.4 mm. The penetrations of radioactive nuclides for dried concrete specimens proceeded. The penetration rates were substantially decreased when 16 days have elapsed from start. The dose rates of penetrated dried concrete specimens were reduced to background by grinding-2.0 mm. -ray spectrometry measurement showed that penetration behavior of near surface concrete are different among nuclides and the penetration behavior of radioactive nuclides into dried concrete and mortar materials through solution is similar to migration behavior of ions into those water-saturated materials.

Evaluation of fission product and actinide release behaviors focusing on their chemical forms; Phase relation and fission product release behavior resulting from interaction between molten zircaloy and irradiated MOX fuel

Tanaka, Kosuke; Miwa, Shuhei; Sato, Isamu; Hirosawa, Takashi; Sekine, Shinichi; Seki, Takayuki*; Tokoro, Daishiro*; Obayashi, Hiroshi; Koyama, Shinichi

JAEA-Research 2013-022, 62 Pages, 2014/01

JAEA-Research-2013-022.pdf:33.64MB

In order to establish the method for heating tests focused on the fission product release resulting from the high temperature chemical interaction between fuel and cladding material and to obtain the novel data on fission product release behaviors, the heating test was carried out with irradiate MOX fuel pellet and cladding.