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JAEA Reports

Structural investigation of borosilicate glasses by using XAFS measurement in soft X-ray region, 3 (Joint research)

Nagai, Takayuki; Okamoto, Yoshihiro; Yamagishi, Hirona*; Shibata, Daisuke*; Kojima, Kazuo*; Hasegawa, Takehiko*; Sato, Seiichi*; Fukaya, Akane*; Hatakeyama, Kiyoshi*

JAEA-Research 2023-004, 45 Pages, 2023/09

JAEA-Research-2023-004.pdf:6.07MB

The local structure of glass-forming elements and waste elements in borosilicate glasses varies with its chemical composition. In this study, simulated waste glass samples were prepared and the chemical state regarding boron (B), silicon (Si) and waste elements of iron (Fe), cesium (Cs) were estimated by using XAFS measurement in soft X-ray region. To understand the chemical stability of simulated waste glasses, XANES spectra of B K-edge, Fe L$$_{3}$$, L$$_{2}$$-edge, and Cs M$$_{5}$$, M$$_{4}$$-edge were measured on the glass surface exposed to the leachate. As a result, it was found that the glass surface exposed to the leachate was changed and it was difficult to obtain a clear XANES spectrum. From the B K-edge XANES spectra on glass surfaces exposed to the leachate, an increase in three-coordination of B-O (BO$$_{3}$$) and a decrease in four-coordination of B-O (BO$$_{4}$$) were observed compared to the glass surfaces before immersion. The XANES spectra of Fe L$$_{3}$$, L$$_{2}$$-edge, and Cs M$$_{5}$$, M$$_{4}$$-edge show that as the exposure time in the leachate increases, the Cs present on the glass surface dissolves into the leachate. The XANES spectra of Si K-edge were measured on simulated waste glass surfaces before immersion, and it was confirmed that the change in XANES spectra given by Na$$_{2}$$O concentration had a larger effect than the waste component concentration.

Journal Articles

Raman identification and characterization of chemical components included in simulated nuclear fuel debris synthesized from uranium, stainless steel, and zirconium

Kusaka, Ryoji; Kumagai, Yuta; Watanabe, Masayuki; Sasaki, Takayuki*; Akiyama, Daisuke*; Sato, Nobuaki*; Kirishima, Akira*

Journal of Nuclear Science and Technology, 60(5), p.603 - 613, 2023/05

 Times Cited Count:1 Percentile:31.61(Nuclear Science & Technology)

Journal Articles

Phase analysis of simulated nuclear fuel debris synthesized using UO$$_{2}$$, Zr, and stainless steel and leaching behavior of the fission products and matrix elements

Tonna, Ryutaro*; Sasaki, Takayuki*; Kodama, Yuji*; Kobayashi, Taishi*; Akiyama, Daisuke*; Kirishima, Akira*; Sato, Nobuaki*; Kumagai, Yuta; Kusaka, Ryoji; Watanabe, Masayuki

Nuclear Engineering and Technology, 55(4), p.1300 - 1309, 2023/04

 Times Cited Count:1 Percentile:72.91(Nuclear Science & Technology)

Simulated debris was synthesized using UO$$_{2}$$, Zr, and stainless steel and a heat treatment method under inert or oxidizing conditions. The primary U solid phase of the debris synthesized at 1473 K under inert conditions was UO$$_{2}$$, whereas a (U,Zr)O$$_{2}$$ solid solution formed at 1873 K. Under oxidizing conditions, a mixture of U$$_{3}$$O$$_{8}$$ and (Fe,Cr)UO$$_{4}$$ phases formed at 1473 K whereas a (U,Zr)O$$_{2+x}$$ solid solution formed at 1873 K. The leaching behavior of the fission products from the simulated debris was evaluated using two methods: the irradiation method, for which fission products were produced via neutron irradiation, and the doping method, for which trace amounts of non-radioactive elements were doped into the debris. The dissolution behavior of U depended on the properties of the debris and aqueous medium the debris was immersed in. Cs, Sr, and Ba leached out regardless of the primary solid phases. The leaching of high-valence Eu and Ru ions was suppressed, possibly owing to their solid-solution reaction with or incorporation into the uranium compounds of the simulated debris.

Journal Articles

Study on the relation between the crystal structure and thermal stability of FeUO$$_{4}$$ and CrUO$$_{4}$$

Akiyama, Daisuke*; Kusaka, Ryoji; Kumagai, Yuta; Nakada, Masami; Watanabe, Masayuki; Okamoto, Yoshihiro; Nagai, Takayuki; Sato, Nobuaki*; Kirishima, Akira*

Journal of Nuclear Materials, 568, p.153847_1 - 153847_10, 2022/09

 Times Cited Count:3 Percentile:68.71(Materials Science, Multidisciplinary)

FeUO$$_{4}$$, CrUO$$_{4}$$, and Fe$$_{x}$$Cr$$_{1-x}$$UO$$_{4}$$ are monouranates containing pentavalent U. Even though these compounds have similar crystal structures, their formation conditions and thermal stability are significantly different. To determine the factors causing the difference in thermal stability between FeUO$$_{4}$$ and CrUO$$_{4}$$, their crystal structures were evaluated in detail. A Raman band was observed at 700 cm$$^{-1}$$ in all the samples. This Raman band was derived from the stretching vibration of the O-U-O axis band, indicating that Fe$$_{x}$$Cr$$_{1-x}$$UO$$_{4}$$ was composed of a uranyl-like structure in its lattice regardless of its "x"' value. M$"o$ssbauer measurements indicated that the Fe in FeUO$$_{4}$$ and Fe$$_{x}$$Cr$$_{1-x}$$UO$$_{4}$$ were trivalent. Furthermore, Fe$$_{x}$$Cr$$_{1-x}$$UO$$_{4}$$ lost its symmetry around Fe$$^{mathrm{III}}$$ with increasing electron densities around Fe$$^{mathrm{III}}$$, as the abundance of Cr increased. These results suggested no significant structural differences between FeUO$$_{4}$$ and CrUO$$_{4}$$. Thermogravimetric measurements for UO$$_{2}$$, FeUO$$_{4}$$, and CrUO$$_{4}$$ showed that the temperature at which FeUO$$_{4}$$ decomposed under an oxidizing condition (approximately 800 $$^{circ}$$C) was significantly lower than the temperature at which the decomposition of CrUO$$_{4}$$ started (approximately 1250 $$^{circ}$$C). Based on these results, we concluded that the decomposition of FeUO$$_{4}$$ was triggered by an "in-crystal" redox reaction, i.e., Fe$$^{mathrm{III}}$$ $${+}$$ U$$^{mathrm{V}}$$ $$rightarrow$$ Fe$$^{mathrm{II}}$$ $${+}$$ U$$^{mathrm{VI}}$$, which would not occur in the CrUO$$_{4}$$ lattice because Cr$$^{mathrm{III}}$$ could never be reduced under the investigated condition. Finally, the existence of Cr$$^{mathrm{III}}$$ in FexCr$$_{1-x}$$UO$$_{4}$$ effectively suppressed the decomposition of the Fe$$_{x}$$Cr$$_{1-x}$$UO$$_{4}$$ crystal, even at a very low Cr content.

Journal Articles

Structure, stability, and actinide leaching of simulated nuclear fuel debris synthesized from UO$$_{2}$$, Zr, and stainless-steel

Kirishima, Akira*; Akiyama, Daisuke*; Kumagai, Yuta; Kusaka, Ryoji; Nakada, Masami; Watanabe, Masayuki; Sasaki, Takayuki*; Sato, Nobuaki*

Journal of Nuclear Materials, 567, p.153842_1 - 153842_15, 2022/08

 Times Cited Count:4 Percentile:78.52(Materials Science, Multidisciplinary)

To understand the chemical structure and stability of nuclear fuel debris consisting of UO$$_{2}$$, Zr, and Stainless Steel (SUS) generated by the Fukushima Daiichi Nuclear Power Plant accident in Japan in 2011, simulated debris of the UO$$_{2}$$-SUS-Zr system and other fundamental component systems were synthesized and characterized. The simulated debris were synthesized by heat treatment for 1 to 12 h at 1600$$^{circ}$$C, in inert (Ar) or oxidative (Ar + 2% O$$_{2}$$) atmospheres. $$^{237}$$Np and $$^{241}$$Am tracers were doped for the leaching tests of these elements and U from the simulated debris. The characterization of the simulated debris was conducted by XRD, SEM-EDX, Raman spectroscopy, and M$"o$ssbauer spectroscopy, which provided the major uranium phase of the UO $$_{2}$$-SUS-Zr debris was the solid solution of U$$^{mathrm{IV}}$$O$$_{2}$$ (s.s.) with Zr(IV) and Fe(II) regardless of the treatment atmosphere. The long-term immersion test of the simulated debris in pure water and that in seawater revealed the macro scale crystal structure of the simulated debris was chemically very stable in the wet condition for a year or more. Furthermore, the leaching test results showed that the actinide leaching ratios of U, Np, Am from the UO$$_{2}$$-SUS-Zr debris were very limited and less than 0.08 % for all the experiments in this study.

Journal Articles

Uranium dissolution and uranyl peroxide formation by immersion of simulated fuel debris in aqueous H$$_{2}$$O$$_{2}$$ solution

Kumagai, Yuta; Kusaka, Ryoji; Nakada, Masami; Watanabe, Masayuki; Akiyama, Daisuke*; Kirishima, Akira*; Sato, Nobuaki*; Sasaki, Takayuki*

Journal of Nuclear Science and Technology, 59(8), p.961 - 971, 2022/08

 Times Cited Count:2 Percentile:53.91(Nuclear Science & Technology)

We investigated potential degradation of fuel debris caused by H$$_{2}$$O$$_{2}$$, which is the oxidant of major impact from water radiolysis. We performed leaching experiments on different kinds of simulated debris comprising U, Fe, Cr, Ni, and Zr in an aqueous H$$_{2}$$O$$_{2}$$ solution. Chemical analysis of the leaching solution showed that U dissolution was induced by H$$_{2}$$O$$_{2}$$. Raman analysis after the leaching revealed that uranyl peroxides were formed on the surface of the simulated debris. These results demonstrate that uranyl peroxides are possible alteration products of fuel debris from H$$_{2}$$O$$_{2}$$ reaction. However, the sample in which the main uranium-containing phase was a U-Zr oxide solid solution showed much less uranium dissolution and no Raman signal of uranyl peroxides. Comparison of these results indicates that formation of an oxide solid solution of Zr with UO$$_{2}$$ improves the stability of fuel debris against H$$_{2}$$O$$_{2}$$ reaction.

JAEA Reports

Stabilization treatment of nuclear fuel material contained with organic matter

Senzaki, Tatsuya; Arai, Yoichi; Yano, Kimihiko; Sato, Daisuke; Tada, Kohei; Ogi, Hiromichi*; Kawanobe, Takayuki*; Ono, Shimpei; Nakamura, Masahiro; Kitawaki, Shinichi; et al.

JAEA-Testing 2022-001, 28 Pages, 2022/05

JAEA-Testing-2022-001.pdf:2.33MB

In preparation for the decommissioning of Laboratory B of the Nuclear Fuel Cycle Engineering Laboratory, the nuclear fuel material that had been stored in the glove box for a long time was moved to the Chemical Processing Facility (CPF). This nuclear fuel material was stored with sealed by a polyvinyl chloride (PVC) bag in the storage. Since it was confirmed that the PVC bag swelled during storage, it seems that any gas was generated by radiolysis of the some components contained in the nuclear fuel material. In order to avoid breakage of the PVC bag and keep it safety for long time, we began the study on the stabilization treatment of the nuclear fuel material. First, in order to clarify the properties of nuclear fuel material, radioactivity analysis, component analysis, and thermal analysis were carried out. From the results of thermal analysis, the existence of organic matter was clarified. Then, ion exchange resin with similar thermal characteristics was selected and the thermal decomposition conditions were investigated. From the results of these analyzes and examinations, the conditions for thermal decomposition of the nuclear fuel material contained with organic matter was established. Performing a heat treatment of a small amount of nuclear fuel material in order to confirm the safety, after which the treatment amount was scaled up. It was confirmed by the weight change after the heat treatment that the nuclear fuel material contained with organic matter was completely decomposed.

Journal Articles

A Study of H$$_{2}$$O$$_{2}$$-induced oxidative degradation of simulated fuel debris

Kumagai, Yuta; Kusaka, Ryoji; Nakada, Masami; Watanabe, Masayuki; Akiyama, Daisuke*; Kirishima, Akira*; Sato, Nobuaki*; Sasaki, Takayuki*

Hoshasen Kagaku (Internet), (113), p.61 - 64, 2022/04

The severe accident at TEPCO's Fukushima Daiichi Nuclear Power Station resulted in generation of fuel debris. The fuel debris is in contact with water and the radiolysis of water can accelerate degradation of the debris. The analysis of particles sampled from inside or near the damaged reactors indicates the complicated compositions of the fuel debris. It is challenging to estimate the effect of water radiolysis on such a complicated material. Therefore, in this study, we investigated the potential degradation process by leaching experiments of simulated fuel debris in aqueous H$$_{2}$$O$$_{2}$$ solution. The results show that the reaction of H$$_{2}$$O$$_{2}$$ induced uranium dissolution from most of the samples and then formation of uranyl peroxides. In contrast, a sample that had U-Zr oxide solid solution as the major phase exhibited remarkable resistance to H$$_{2}$$O$$_{2}$$. These findings revealed that the degradation of the simulated debris reflects the reactivity and stability of the uranium phase in the matrices.

Journal Articles

Speciation on the reaction of uranium and zirconium oxides treated under oxidizing and reducing atmospheres

Uehara, Akihiro*; Akiyama, Daisuke*; Ikeda, Atsushi; Numako, Chiya*; Terada, Yasuko*; Nitta, Kiyofumi*; Ina, Toshiaki*; Takeda-Homma, Shino*; Kirishima, Akira*; Sato, Nobuaki*

Journal of Nuclear Materials, 559, p.153422_1 - 153422_11, 2022/02

 Times Cited Count:2 Percentile:53.91(Materials Science, Multidisciplinary)

Journal Articles

Validation of ATDMs at early after the lF accident using air dose rate estimated by airborne concentration and surface deposition density

Moriguchi, Yuichi*; Sato, Yosuke*; Morino, Yu*; Goto, Daisuke*; Sekiyama, Tsuyoshi*; Terada, Hiroaki; Takigawa, Masayuki*; Tsuruta, Haruo*; Yamazawa, Hiromi*

KEK Proceedings 2021-2, p.21 - 27, 2021/12

no abstracts in English

Journal Articles

Investigation of chemical state of uranium included in simulated waste glass

Nagai, Takayuki; Akiyama, Daisuke*; Kirishima, Akira*; Sato, Nobuaki*; Okamoto, Yoshihiro

2020-Nendo "Busshitsu, Debaisu Ryoiki Kyodo Kenkyu Kyoten" Oyobi "Hito, Kankyo To Busshitsu O Tsunagu Inobeshion Soshutsu Dainamikku, Araiansu" Kenkyu Seika, Katsudo Hokokusho (CD-ROM), 1 Pages, 2021/11

no abstracts in English

Journal Articles

Distribution of studtite and metastudtite generated on the surface of U$$_{3}$$O$$_{8}$$; Application of Raman imaging technique to uranium compound

Kusaka, Ryoji; Kumagai, Yuta; Yomogida, Takumi; Takano, Masahide; Watanabe, Masayuki; Sasaki, Takayuki*; Akiyama, Daisuke*; Sato, Nobuaki*; Kirishima, Akira*

Journal of Nuclear Science and Technology, 58(6), p.629 - 634, 2021/06

 Times Cited Count:7 Percentile:66.68(Nuclear Science & Technology)

Journal Articles

Meteorological aspects of gamma-ray glows in winter thunderstorms

Wada, Yuki*; Enoto, Teruaki*; Kubo, Mamoru*; Nakazawa, Kazuhiro*; Shinoda, Taro*; Yonetoku, Daisuke*; Sawano, Tatsuya*; Yuasa, Takayuki*; Ushio, Tomoo*; Sato, Yosuke*; et al.

Geophysical Research Letters, 48(7), 11 Pages, 2021/04

 Times Cited Count:20 Percentile:90.11(Geosciences, Multidisciplinary)

During three winter seasons from November 2016 to March 2019, 11 gamma-ray glows were detected at a single observation site of our ground-based gamma-ray monitoring network in Kanazawa, Japan. These events are analyzed with observations of an X-band radar network, a ceilometer, a disdrometer, and a weather monitor. All the detected glows were connected to convective high-reflectivity regions of more than 35 dBZ, developed up to an altitude of $$>$$2 km. They were also accompanied by heavy precipitation of graupels. Therefore, graupels in the lower layer of thunderclouds that correspond to high-reflectivity regions can form strong electric fields producing gamma-ray glows. Also, these events are compared with a limited sample of nondetection cases, but no significant differences in meteorological conditions were found between detection and nondetection cases in the present study.

Journal Articles

High temperature gas-cooled reactors

Takeda, Tetsuaki*; Inagaki, Yoshiyuki; Aihara, Jun; Aoki, Takeshi; Fujiwara, Yusuke; Fukaya, Yuji; Goto, Minoru; Ho, H. Q.; Iigaki, Kazuhiko; Imai, Yoshiyuki; et al.

High Temperature Gas-Cooled Reactors; JSME Series in Thermal and Nuclear Power Generation, Vol.5, 464 Pages, 2021/02

As a general overview of the research and development of a High Temperature Gas-cooled Reactor (HTGR) in JAEA, this book describes the achievements by the High Temperature Engineering Test Reactor (HTTR) on the designs, key component technologies such as fuel, reactor internals, high temperature components, etc., and operational experience such as rise-to-power tests, high temperature operation at 950$$^{circ}$$C, safety demonstration tests, etc. In addition, based on the knowledge of the HTTR, the development of designs and component technologies such as high performance fuel, helium gas turbine and hydrogen production by IS process for commercial HTGRs are described. These results are very useful for the future development of HTGRs. This book is published as one of a series of technical books on fossil fuel and nuclear energy systems by the Power Energy Systems Division of the Japan Society of Mechanical Engineers.

Journal Articles

The Effects of addition of carbon dioxide and water vapor on the dynamic behavior of spherically expanding hydrogen/air premixed flames

Katsumi, Toshiyuki; Yoshida, Yasuhito*; Nakagawa, Ryo*; Yazawa, Shinya*; Kumada, Masashi*; Sato, Daisuke*; Thwe Thwe, A.; Chaumeix, N.*; Kadowaki, Satoshi

Journal of Thermal Science and Technology (Internet), 16(2), p.21-00044_1 - 21-00044_13, 2021/00

 Times Cited Count:5 Percentile:36.79(Thermodynamics)

The effects of addition of CO$$_{2}$$ and water vapor on characteristics of dynamic behavior of hydrogen/air premixed flames were elucidated experimentally. By Schlieren photography, wrinkles on the flame surface were clearly observed in low equivalence ratios. The propagation velocity increased monotonically as the flame radius became larger and flame acceleration was found. Increasing the addition of inert gas, the propagation velocity decreased, especially in the case of CO$$_{2}$$ addition. Moreover, the Markstein length and the wrinkling factor decreased. This indicated that the addition of Co$$_{2}$$ or H$$_{2}$$O promoted the unstable motion of hydrogen flames, which could be due to the enhancement of the diffusive-thermal effect. Based on the characteristics of dynamic behavior of hydrogen flames, the parameters used in the mathematical model on propagation velocity including flame acceleration was obtained, and then the flame propagation velocity under various conditions was predicted.

Journal Articles

Investigation of chemical state of uranium included in simulated waste glass

Nagai, Takayuki; Akiyama, Daisuke*; Kirishima, Akira*; Sato, Nobuaki*; Okamoto, Yoshihiro

2019-Nendo "Busshitsu, Debaisu Ryoiki Kyodo Kenkyu Kyoten" Oyobi "Hito, Kankyo To Busshitsu O Tsunagu Inobeshion Soshutsu Dainamikku, Araiansu" Kenkyu Seika, Katsudo Hokokusho (CD-ROM), P. 20191107_1, 2020/11

no abstracts in English

Journal Articles

A Model intercomparison of atmospheric $$^{137}$$Cs concentrations from the Fukushima Daiichi Nuclear Power Plant accident, phase III; Simulation with an identical source term and meteorological field at 1-km resolution

Sato, Yosuke*; Sekiyama, Tsuyoshi*; Fang, S.*; Kajino, Mizuo*; Qu$'e$rel, A.*; Qu$'e$lo, D.*; Kondo, Hiroaki*; Terada, Hiroaki; Kadowaki, Masanao; Takigawa, Masayuki*; et al.

Atmospheric Environment; X (Internet), 7, p.100086_1 - 100086_12, 2020/10

The third model intercomparison project for investigating the atmospheric behavior of $$^{137}$$Cs emitted during the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident (FDNPP-MIP) was conducted. A finer horizontal grid spacing (1 km) was used than in the previous FDNPP-MIP. Nine of the models used in the previous FDNPP-MIP were also used, and all models used identical source terms and meteorological fields. Our analyses indicated that most of the observed high atmospheric $$^{137}$$Cs concentrations were well simulated, and the good performance of some models improved the performance of the multi-model ensemble. The analyses also confirmed that the use of a finer grid resolution resulted in the meteorological field near FDNPP being better reproduced. The good representation of the wind field resulted in the reasonable simulation of the narrow distribution of high deposition amount to the northwest of FDNPP and the reduction of the overestimation over the area to the south of FDNPP. In contrast, the performance of the models in simulating plumes observed over the Nakadori area, the northern part of Gunma, and the Tokyo metropolitan area was slightly worse.

Journal Articles

Insight into Kondo screening in the intermediate-valence compound SmOs$$_4$$Sb$$_{12}$$ uncovered by soft X-ray magnetic circular dichroism

Saito, Yuji; Fujiwara, Hidenori*; Yasui, Akira*; Kadono, Toshiharu*; Sugawara, Hitoshi*; Kikuchi, Daisuke*; Sato, Hideyuki*; Suga, Shigemasa*; Yamasaki, Atsushi*; Sekiyama, Akira*; et al.

Physical Review B, 102(16), p.165152_1 - 165152_8, 2020/10

 Times Cited Count:1 Percentile:6.04(Materials Science, Multidisciplinary)

Journal Articles

Production of $$^{266}$$Bh in the $$^{248}$$Cm($$^{23}$$Na,5$$n$$)$$^{266}$$Bh reaction and its decay properties

Haba, Hiromitsu*; Fan, F.*; Kaji, Daiya*; Kasamatsu, Yoshitaka*; Kikunaga, Hidetoshi*; Komori, Yukiko*; Kondo, Narumi*; Kudo, Hisaaki*; Morimoto, Koji*; Morita, Kosuke*; et al.

Physical Review C, 102(2), p.024625_1 - 024625_12, 2020/08

 Times Cited Count:6 Percentile:59.56(Physics, Nuclear)

Journal Articles

High peak-current lightning discharges associated with downward terrestrial gamma-ray flashes

Wada, Yuki*; Enoto, Teruaki*; Nakamura, Yoshitaka*; Morimoto, Takeshi*; Sato, Mitsuteru*; Ushio, Tomoo*; Nakazawa, Kazuhiro*; Yuasa, Takayuki*; Yonetoku, Daisuke*; Sawano, Tatsuya*; et al.

Journal of Geophysical Research; Atmospheres, 125(4), p.e2019JD031730_1 - e2019JD031730_11, 2020/02

 Times Cited Count:21 Percentile:80.58(Meteorology & Atmospheric Sciences)

191 (Records 1-20 displayed on this page)