Analysis of particles containing alpha emitters in stagnant water in Fukushima Daiichi Nuclear Power Station's Unit 3 reactor building

Yomogida, Takumi; Ouchi, Kazuki; Morii, Shiori; Oka, Toshitaka; Kitatsuji, Yoshihiro; Koma, Yoshikazu; Konno, Katsuhiro*

Scientific Reports (Internet), 14, p.14945_1 - 14945_11, 2024/06

https://doi.org/10.1038/s41598-024-65522-2

Particles containing alpha () nuclides were identified from sediment in stagnant water in the Unit 3 reactor building of the Fukushima Daiichi Nuclear Power Station (FDiNPS). We analyzed different concentrations of alpha nuclides samples collected at two sampling sites, torus room and Main steam isolation valve (MSIV) room. Most of the -nuclides in the stagnant water samples of the torus room and the MSIV room were present in particle fractions larger than 10 m. We detected uranium-bearing particles in m-size by scanning electron microscopy-energy dispersive X-Ray (SEM-EDX) observation. Other short lived -nuclides were detected by alpha track detection. The -nuclide-containing particles with several tens to several hundred m in size were mainly comprised iron (Fe) by SEM-EDX analysis. This study clarifies that the morphologies of U and other -nuclides in the sediment of stagnant water in the FDiNPS's Unit 3 reactor building.

Determination of Sr in highly radioactive aqueous samples via conversion to a kinetically stable 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid complex followed by concentration-separation-fractionation based on capillary electrophoresis-liquid scintillation

Ouchi, Kazuki; Haraga, Tomoko; Hirose, Kazuki*; Kurosawa, Yuika*; Sato, Yoshiyuki; Shibukawa, Masami*; Saito, Shingo*

Analytica Chimica Acta, 1298, p.342399_1 - 342399_7, 2024/04

https://doi.org/10.1016/j.aca.2024.342399

Given that conventional methods of high-dose sample analysis pose substantial exposure risks and generate large amounts of secondary radioactive waste, faster procedures allowing for decreased radiation emission are highly desirable. To address this need, we developed a Sr quantitation technique that is based on liquid scintillation counting-coupled capillary transient isotachophoresis (ctITP) with two-point detection and relies on the rapid concentration, separation, and fractionation of 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid (DOTA)-complexed Sr in a single run. This method, which allows for the handling of high-dose radioactive specimens at the microliter level and is substantially faster than conventional ion-exchange protocols, was used to selectively quantify Sr in real high-dose waste. The successful concentration-separation in ctITP was ascribed to the inertness of the Sr-DOTA complex to dissociation.

Studies on complex reactions of actinides in solution and development of analytical methods for small amounts of samples

Ouchi, Kazuki

Hosha Kagaku, (49), p.3 - 7, 2024/03

I introduce the elucidation of the deposition following the oxidation state of uranium and the electrochemical behavior of uranium(IV) chloride in an ionic liquid-organic mixture, as a basic study of in-solution reactions. In addition, I introduce the development of separation methods for actinides using a microchemical chip and polyacrylamide gel electrophoresis, as an applied study for quantitative analytical methods for small amounts of samples.

Development of a quantification method for Zr isotopes in solid samples by LA-ICP-MS for rapid analysis of Zr-93 in high-level radioactive wastes

Morii, Shiori; Yomogida, Takumi; Asai, Shiho*; Ouchi, Kazuki; Oka, Toshitaka; Kitatsuji, Yoshihiro

Bunseki Kagaku, 72(10.11), p.441 - 448, 2023/10

https://doi.org/10.2116/bunsekikagaku.72.441

Rapid analytical method for the determination of Zr-93 in radioactive wastes has been developed. Laser ablation (LA)-ICP-MS was applied to the analysis of Zr isotopes in simulated high-level radioactive waste (HLW). Sample preparation time was dramatically reduced by using a DGA resin as the adsorbent for Zr. Direct quantification of Zr isotopes in this resin sample was carried out by LA-ICP-MS. Laser settings were optimized to obtain a reliable isotope ratio of the sample by LA-ICP-MS. Quantification of Zr isotopes in the simulated HLW solution by isotope dilution mass spectrometry (IDMS) was examined. The amount of Zr-90 in the sample obtained by IDMS corresponded to a value calculated from the given concentration of Zr in the sample within uncertainty. Thus, this method can be applied for the quantification of Zr-93 in radioactive wastes.

New measurement system based on small-angle neutron scattering for structural analysis of light-responsive materials

Iwase, Hiroki*; Akamatsu, Masaaki*; Inamura, Yasuhiro; Sakaguchi, Yoshifumi*; Morikawa, Toshiaki*; Kasai, Satoshi*; Ouchi, Keiichi*; Kobayashi, Kazuki*; Sakai, Hideki*

Journal of Applied Crystallography, 56(1), p.110 - 115, 2023/02

https://doi.org/10.1107/S1600576722011104

With the increasing importance of light-responsive materials, it is vital to analyze the relationship between function and structural changes induced by light irradiation. Small-angle scattering (SAS) is effective for such structural analysis. However, quantitatively capturing local molecular structure formation and molecular reactions at a scale of less than 1 nm via SAS is difficult. In this study, to analyze the structure of non-equilibrium phenomena in light-responsive materials, a new sample environment has been developed for a time-of-flight small- and wide-angle neutron scattering instrument (TAIKAN), comprising a UV-Vis irradiation system, UV-Vis absorption measurement equipment and photodetector. Simultaneous measurement of small-angle neutron scattering and UV-Vis absorption was achieved. This system was used to demonstrate the in situ observation of UV-Vis irradiation-induced structural change of micelles formed by a light-responsive surfactant sample in an aqueous solution.

Application of high-energy-resolution X-ray absorption spectroscopy at the U L-edge to assess the U(V) electronic structure in FeUO

Yomogida, Takumi; Akiyama, Daisuke*; Ouchi, Kazuki; Kumagai, Yuta; Higashi, Kotaro*; Kitatsuji, Yoshihiro; Kirishima, Akira*; Kawamura, Naomi*; Takahashi, Yoshio*

Inorganic Chemistry, 61(50), p.20206 - 20210, 2022/12

https://doi.org/10.1021/acs.inorgchem.2c03208

FeUO was studied to clarify the electronic structure of U(V) in a metal monouranate compound. We obtained the peak splitting of HERFD-XANES spectra utilizing high-energy-resolution fluorescence detection-X-ray absorption near edge structure (HERFD-XANES) spectroscopy at the U L-edge, which is a novel technique in the U(V) compounds. Theoretical calculations revealed that the peak splitting was caused by splitting the 6d orbital of U(V). Such distinctive electronic states are of major interest to researchers and engineers working in various fields, from fundamental physics to the nuclear industry and environmental sciences for actinide elements.

Analysis of particles containing alpha-emitters in stagnant water at torus room of Fukushima Dai-ichi Nuclear Power Station's Unit 2 reactor

Yomogida, Takumi; Ouchi, Kazuki; Oka, Toshitaka; Kitatsuji, Yoshihiro; Koma, Yoshikazu; Konno, Katsuhiro*

Scientific Reports (Internet), 12(1), p.7191_1 - 7191_10, 2022/05

AA2021-0706.pdf:2.48MB

https://doi.org/10.1038/s41598-022-11334-1

Particles containing alpha () nuclides were identified from sediment in stagnant water at the torus room of the Fukushima Dai-ichi Nuclear Power Station (FDiNPS)'s Unit 2 reactor. Several uranium-bearing particles were identified by SEM observation. These particles contained Zr and other elements which constituted fuel cladding and structural materials. The U/U isotope ratio in the solid fractions that included U particles was consistent with the nuclear fuel in the Unit 2 reactor, which indicated that the U particles had been derived from nuclear fuel. The particles with alpha-emitters detected by alpha track analysis were several tens to several hundred m in size. The EDX spectra showed that these particles mainly comprised iron, which indicated Pu, Am, and Cm were adsorbed on the Fe-baring particles. This study clarifies that the major morphologies of U and other -nuclides were differed in the sediment of stagnant water in the torus room of FDiNPS's Unit 2 reactor.

Electrochemical studies of uranium (IV) in an ionic liquid-DMF mixture to build a redox flow battery using uranium as an electrode active material

Ouchi, Kazuki; Komatsu, Atsushi; Takao, Koichiro*; Kitatsuji, Yoshihiro; Watanabe, Masayuki

Chemistry Letters, 50(6), p.1169 - 1172, 2021/06

https://doi.org/10.1246/cl.210060

The electrochemical behavior of uranium (IV) tetrachloride in ionic liquid-DMF mixture was studied for first time in order to build a redox flow battery (RFB) using U as an electrode active material. We found a quasi-reversible U/U couple that could be applied to the anode reaction of the RFB.

Deposition of uranium oxide following the reduction in weak acid solution using Electrochemical Quartz Crystal Microbalance (EQCM)

Ouchi, Kazuki; Otobe, Haruyoshi; Kitatsuji, Yoshihiro; Yamamoto, Masahiro

ECS Transactions, 75(27), p.51 - 57, 2017/01

https://doi.org/10.1149/07527.0051ecst

We investigated the deposition of U(IV) following a valence change of U as electrodeposition using an electrochemical quartz crystal microbalance (EQCM). When measurements of the reduction of U(VI) in a weak acid solution were performed, deposits of U(IV) were observed on the electrode surface. From deposition rates, pH dependence of them, and oxidation potentials of deposits, we proposed the following deposition mechanism. The deposition is divided into the three phases; First, in the induction phase, U(IV) produced by the disproportionation forms U(IV) hydroxide nucleus. Next, in the growth phase, U(IV) deposits begin to grow. In this phase, the deposits catalyze the reduction of U(V) to U(IV), resulting an increase of the reduction current. Finally, in the transformation phase, U(IV) hydroxide species transform into U dioxide having more stable state.

Determination of the absolute two-photon ionization cross section of He by an XUV free electron laser

Sato, Takahiro*; Iwasaki, Atsushi*; Ishibashi, Kazuki*; Okino, Tomoya*; Yamanouchi, Kaoru*; Adachi, Junichi*; Yagishita, Akira*; Yazawa, Hiroki*; Kannari, Fumihiko*; Aoyama, Makoto; et al.

Journal of Physics B; Atomic, Molecular and Optical Physics, 44(16), p.161001_1 - 161001_5, 2011/08

https://doi.org/10.1088/0953-4075/44/16/161001

The resonant and non-resonant two-photon single ionization processes of He were investigated using intense free electron laser light in the extreme ultraviolet (XUV) region (53.4-61.4 nm) covering the 1s-2p and 1s-3p resonant transitions of He. On the basis of the dependences of the yield of He on the XUV light-field intensity at 53.4, 58.4, 56.0 and 61.4 nm, the absolute values of the two-photon ionization cross sections of He at the four different wavelengths and their dependence on the light-field intensity were determined for the first time.