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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

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:0

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

Structural Approach to Understanding the Formation of Amorphous Metal Hydroxides

Kobayashi, Taishi*; Fushimi, Tomokazu*; Mizukoshi, Hirofumi*; Motokawa, Ryuhei; Sasaki, Takayuki*

Langmuir, 38(48), p.14656 - 14665, 2022/12

 Times Cited Count:0 Percentile:0(Chemistry, Multidisciplinary)

no abstracts in English

Journal Articles

Materials science and fuel technologies of uranium and plutonium mixed oxide

Kato, Masato; Machida, Masahiko; Hirooka, Shun; Nakamichi, Shinya; Ikusawa, Yoshihisa; Nakamura, Hiroki; Kobayashi, Keita; Ozawa, Takayuki; Maeda, Koji; Sasaki, Shinji; et al.

Materials Science and Fuel Technologies of Uranium and Plutonium mixed Oxide, 171 Pages, 2022/10

Innovative and advanced nuclear reactors using plutonium fuel has been developed in each country. In order to develop a new nuclear fuel, irradiation tests are indispensable, and it is necessary to demonstrate the performance and safety of nuclear fuels. If we can develop a technology that accurately simulates irradiation behavior as a technology that complements the irradiation test, the cost, time, and labor involved in nuclear fuel research and development will be greatly reduced. And safety and reliability can be significantly improved through simulation of nuclear fuel irradiation behavior. In order to evaluate the performance of nuclear fuel, it is necessary to know the physical and chemical properties of the fuel at high temperatures. And it is indispensable to develop a behavior model that describes various phenomena that occur during irradiation. In previous research and development, empirical methods with fitting parameters have been used in many parts of model development. However, empirical techniques can give very different results in areas where there is no data. Therefore, the purpose of this study is to construct a scientific descriptive model that can extrapolate the basic characteristics of fuel to the composition and temperature, and to develop an irradiation behavior analysis code to which the model is applied.

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:3 Percentile:83.13(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:1 Percentile:62.84(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.

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

Sorption of Cs$$^{+}$$ and Eu$$^{3+}$$ ions onto sedimentary rock in the presence of gamma-irradiated humic acid

Zhao, Q.*; Saito, Takeshi*; Miyakawa, Kazuya; Sasamoto, Hiroshi; Kobayashi, Taishi*; Sasaki, Takayuki*

Journal of Hazardous Materials, 428, p.128211_1 - 128211_10, 2022/04

 Times Cited Count:1 Percentile:45.14(Engineering, Environmental)

The influence of humic acid and its radiological degradation on the sorption of Cs$$^{+}$$ and Eu$$^{3+}$$ by sedimentary rock was investigated to understand the sorption process of metal ions and humic substances. Aldrich humic acid (HA) solution was irradiated with different doses of gamma irradiation using a Co-60 gamma-ray source prior to the contact between the metal ions and the solid sorbent. The HA molecule decomposed to smaller molecules with a lower complexation affinity. Batch sorption experiments were performed to evaluate the effect of gamma-irradiated HA on the sorption of Cs$$^{+}$$ and Eu$$^{3+}$$ ions. The addition of non-irradiated HA weakened the sorption of Eu because of the lower sorption of the neutral or negatively charged Eu-HA complexes compared with free Eu ions. The sorption of monovalent Cs ions was barely affected by the presence of HA and its gamma irradiation. The concentration ratio of HA complexed species and non-complexed species in the solid and liquid phases was evaluated by sequential filtration and chemical equilibrium calculations. The ratios supported the minimal contribution of HA to Cs sorption. However, the concentration ratio for Eu$$^{3+}$$ in the liquid phase was high, indicating that the complexing ability of HA to Eu$$^{3+}$$ was higher than that of HA to Cs$$^{+}$$ ions. Therefore, the sorption of free Eu$$^{3+}$$ would predominate with the gamma irradiation dose applied to the HA solution under a radiation field near the HLW package.

Journal Articles

The Chemistry of thorium, plutonium and MA

Sato, Nobuaki*; Kirishima, Akira*; Watanabe, Masayuki; Sasaki, Takayuki*; Uehara, Akihiro*; Takeda, Shino*; Kitatsuji, Yoshihiro; Otobe, Haruyoshi; Kobayashi, Taishi*

The Chemistry of Thorium, Plutonium and MA, 254 Pages, 2022/03

The chemistry of nuclear materials such as Thorium (Part 1) and Plutonium (Part 2) was described in relation from the fundamentals on solid chemistry and solution chemistry to the practicals on the experiment and evaluation method in detail. Minor actinides such as Neptunium, Americium, Curium and Protoactinium, was introduced the basics on the solid and solution chemistry.

Journal Articles

Rabi-oscillation spectroscopy of the hyperfine structure of muonium atoms

Nishimura, Shoichiro*; Torii, Hiroyuki*; Fukao, Yoshinori*; Ito, Takashi; Iwasaki, Masahiko*; Kanda, Sotaro*; Kawagoe, Kiyotomo*; Kawall, D.*; Kawamura, Naritoshi*; Kurosawa, Noriyuki*; et al.

Physical Review A, 104(2), p.L020801_1 - L020801_6, 2021/08

 Times Cited Count:7 Percentile:81.08(Optics)

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:5 Percentile:64.77(Nuclear Science & Technology)

Journal Articles

Radiocaesium accumulation capacity of epiphytic lichens and adjacent barks collected at the perimeter boundary site of the Fukushima Dai-ichi Nuclear Power Station

Dohi, Terumi; Omura, Yoshihito*; Yoshimura, Kazuya; Sasaki, Takayuki*; Fujiwara, Kenso; Kanaizuka, Seiichi*; Nakama, Shigeo; Iijima, Kazuki

PLOS ONE (Internet), 16(5), p.e0251828_1 - e0251828_16, 2021/05

 Times Cited Count:4 Percentile:45.72(Multidisciplinary Sciences)

Journal Articles

The Chemistry of uranium (II); Method and practice

Sato, Nobuaki*; Kirishima, Akira*; Watanabe, Masayuki; Sasaki, Takayuki*; Uehara, Akihiro*; Takeda, Shino*

Uran No Kagaku (II); Hoho To Jissen, 143 Pages, 2021/03

This book describes necessary facts when readers would have an opportunity to treat Uranium for experiments. In the content, the method section shows experimental facilities and equipment including method, and the practical section mentions solution and solid state experiments using Uranium and/or radioisotopes.

Journal Articles

Vertical distribution of $$^{90}$$Sr and $$^{137}$$Cs in soils near the Fukushima Daiichi Nuclear Power Station

Sasaki, Takayuki*; Matoba, Daisuke*; Dohi, Terumi; Fujiwara, Kenso; Kobayashi, Taishi*; Iijima, Kazuki

Journal of Radioanalytical and Nuclear Chemistry, 326(1), p.303 - 314, 2020/10

 Times Cited Count:2 Percentile:32(Chemistry, Analytical)

JAEA Reports

Analysis of the radioactivity concentrations in low-level radioactive waste generated from JRR-2, JRR-3 and hot laboratory facilities

Tobita, Minoru*; Haraga, Tomoko; Sasaki, Takayuki*; Seki, Kotaro*; Omori, Hiroyuki*; Kochiyama, Mami; Shimomura, Yusuke; Ishimori, Kenichiro; Kameo, Yutaka

JAEA-Data/Code 2019-016, 72 Pages, 2020/02


In the future, radioactive wastes which generated from research and testing reactors in Japan Atomic Energy Agency are planning to be buried for the near surface disposal. Therefore, it is required to establish the method to evaluate the radioactivity concentrations of radioactive wastes by the time it starts disposal. In order to contribute to this work, we collected and analyzed the samples generated from JRR-2, JRR-3 and Hot laboratory facilities. In this report, we summarized the radioactivity concentrations of 25 radionuclides ($$^{3}$$H, $$^{14}$$C, $$^{36}$$Cl, $$^{60}$$Co, $$^{63}$$Ni, $$^{90}$$Sr, $$^{94}$$Nb, $$^{93}$$Mo, $$^{99}$$Tc, $$^{108m}$$Ag, $$^{126}$$Sn, $$^{129}$$I, $$^{137}$$Cs, $$^{152}$$Eu, $$^{154}$$Eu, $$^{233}$$U, $$^{234}$$U, $$^{238}$$U, $$^{238}$$Pu, $$^{239}$$Pu, $$^{240}$$Pu, $$^{241}$$Pu, $$^{241}$$Am, $$^{243}$$Am, $$^{244}$$Cm) which were obtained from radiochemical analysis of those samples.

Journal Articles

Thermodynamic interpretation of uranium(IV/VI) solubility in the presence of $$alpha$$-isosaccharinic acid

Kobayashi, Taishi*; Sasaki, Takayuki*; Kitamura, Akira

Journal of Chemical Thermodynamics, 138, p.151 - 158, 2019/11

 Times Cited Count:1 Percentile:0.01(Thermodynamics)

The effect of $$alpha$$-isosaccharinic acid (ISA) on the solubility and redox of tetravalent and hexavalent uranium (U(IV), U(VI)) was investigated in the hydrogen ion concentration (pH$$_{c}$$) range of 6$$sim$$13 and at total ISA concentration ([ISA]$$_{rm tot}$$) = 10$$^{-4}$$$$sim$$10$$^{-1.2}$$ mol/dm$$^{3}$$. The dependence of U(IV) solubility on pH$$_{c}$$ and [ISA]$$_{rm tot}$$ suggested the existence of U(OH)$$_{4}$$(ISA)$$_{2}$$$$^{2-}$$ as a dominant species within the investigated pH$$_{c}$$ range of 6$$sim$$12. For the U(VI)-ISA system, UO$$_{2}$$(OH)$$_{3}$$(ISA)$$_{2}$$$$^{2-}$$ was suggested as a dominant species at pH$$_{c}$$ 7$$sim$$13. The formation constants of the U(IV)-ISA and U(VI)-ISA complexes were determined by least-squares fitting of the solubility data. The solubility of U(IV) and U(VI) in the presence of ISA and its effect on the redox behavior were thermodynamically interpreted based on the obtained constants.

Journal Articles

Structural approach to understanding the solubility of metal hydroxides

Kobayashi, Taishi*; Nakajima, Shogo*; Motokawa, Ryuhei; Matsumura, Daiju; Saito, Takumi*; Sasaki, Takayuki*

Langmuir, 35(24), p.7995 - 8006, 2019/06

 Times Cited Count:2 Percentile:10.69(Chemistry, Multidisciplinary)

Journal Articles

New precise measurements of muonium hyperfine structure at J-PARC MUSE

Strasser, P.*; Abe, Mitsushi*; Aoki, Masaharu*; Choi, S.*; Fukao, Yoshinori*; Higashi, Yoshitaka*; Higuchi, Takashi*; Iinuma, Hiromi*; Ikedo, Yutaka*; Ishida, Katsuhiko*; et al.

EPJ Web of Conferences, 198, p.00003_1 - 00003_8, 2019/01

 Times Cited Count:12 Percentile:99.37

Journal Articles

A Thermodynamic model for ZrO$$_{2}$$(am) solubility at 25$$^{circ}$$C in the Ca$$^{2+}$$-Na$$^{+}$$-H$$^{+}$$-Cl$$^{-}$$-OH$$^{-}$$-H$$_{2}$$O system; A Critical review

Rai, D.*; Kitamura, Akira; Altmaier, M.*; Rosso, K. M.*; Sasaki, Takayuki*; Kobayashi, Taishi*

Journal of Solution Chemistry, 47(5), p.855 - 891, 2018/05

 Times Cited Count:8 Percentile:9.96(Chemistry, Physical)

We have critically reviewed experimental data for Zr hydrolysis constant values for formation of several mononuclear and polynuclear species and a solubility product value for ZrO$$_{2}$$(am). We have determined new/revised values for the formation constants of Zr(OH)$$_{2}$$$$^{2+}$$, Zr(OH)$$_{4}$$(aq), Zr(OH)$$_{5}$$$$^{-}$$, Zr(OH)$$_{6}$$$$^{2-}$$ and Ca$$_{3}$$Zr(OH)$$_{6}$$$$^{4+}$$, and the solubility product for ZrO$$_{2}$$(am) after the critical review.

Journal Articles

Determination of dissolved natural thorium and uranium in Horonobe and Mizunami Underground Research Laboratory groundwater and its thermodynamic analysis

Sasaki, Takayuki*; Kokami, Takayuki*; Kobayashi, Taishi*; Kirishima, Akira*; Murakami, Hiroaki; Amano, Yuki; Mizuno, Takashi; Iwatsuki, Teruki; Sasamoto, Hiroshi; Miyakawa, Kazuya

Journal of Nuclear Science and Technology, 54(3), p.373 - 381, 2017/03

Trace amounts of natural thorium and uranium in deep groundwater were investigated at two underground research laboratories situated at Horonobe and Mizunami, Japan. The groundwater was sampled from underground boreholes, and the colloid contribution was checked by in situ two size-fractionated ultrafiltration systems. A decrease in the concentration after in situ filtration suggested the presence of natural colloids and suspended matter that were carriers of a portion of the elements. The result of the Th and U concentrations in groundwater after 10 kDa filtration was analyzed thermodynamically using existing hydrogeological and geochemical data such as the mineral components in the groundwater at a given pH, ionic strength, concentration of co-existing ions, redox potential, and solid phase assumed. A crystalline solid phase made the solubility very low compared with that of the amorphous phase, and the solubility agreed well with the concentrations measured.

143 (Records 1-20 displayed on this page)