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Journal Articles

Organization of malonamides from the interface to the organic bulk phase

Micheau, C.; Ueda, Yuki; Motokawa, Ryuhei; Akutsu, Kazuhiro*; Yamada, Norifumi*; Yamada, Masako*; Moussaoui, S. A.*; Makombe, E.*; Meyer, D.*; Berthon, L.*; et al.

Journal of Molecular Liquids, 401, p.124372_1 - 124372_12, 2024/05

Supramolecular organization of extractant molecules impacts metal ions separation behavior. Probing bulk and interfacial structures of the relevant systems is expected to provide key insights into the metal ion selectivity and kinetic aspects. The supramolecular features of two solvent extraction systems based on malonamide extractants THMA in toluene and DBMA in n-heptane were studied using small-angle X-ray scattering for the organic bulk phases, as well as interfacial tension and neutron reflectivity measurements for the interfaces. In the bulk solution, THMA forms dimeric/trimeric associates but no aggregates in toluene, while DBMA forms large aggregates in n-heptane. On the other hand, THMA accumulates in a diffuse layer at the interface at high THMA concentration, whereas DBMA forms a compact but thinner layer. After Pd(II) extraction, the thickness of interfacial layers decreases in the case of THMA, and totally vanishes in the case of DBMA. Based on these new structural information, two mechanisms are proposed for Pd(II) and Nd(III) extraction with malonamides. In toluene, THMA associates slightly accumulate in the vicinity of the interface, then coordinate Pd(II) and diffuse into the organic bulk phase. In n-heptane, DBMA aggregates adsorb at the interface then pick up Nd(III) cations in their polar cores and finally diffuse into the bulk.

JAEA Reports

Contribution to risk reduction in decommissioning works by the elucidation of basic property of radioactive microparticles (Contract Research); FY2020 Nuclear Energy Science & Technology and Human Resource Development Project

Collaborative Laboratories for Advanced Decommissioning Science; Ibaraki University*

JAEA-Review 2023-021, 112 Pages, 2024/02

JAEA-Review-2023-021.pdf:7.1MB

The Collaborative Laboratories for Advanced Decommissioning Science (CLADS), Japan Atomic Energy Agency (JAEA), had been conducting the Nuclear Energy Science & Technology and Human Resource Development Project (hereafter referred to "the Project") in FY2020. The Project aims to contribute to solving problems in the nuclear energy field represented by the decommissioning of the Fukushima Daiichi Nuclear Power Station, Tokyo Electric Power Company Holdings, Inc. (TEPCO). For this purpose, intelligence was collected from all over the world, and basic research and human resource development were promoted by closely integrating/collaborating knowledge and experiences in various fields beyond the barrier of conventional organizations and research fields. The sponsor of the Project was moved from the Ministry of Education, Culture, Sports, Science and Technology to JAEA since the newly adopted proposals in FY2018. On this occasion, JAEA constructed a new research system where JAEA-academia collaboration is reinforced and medium-to-long term research/development and human resource development contributing to the decommissioning are stably and consecutively implemented. Among the adopted proposals in FY2018, this report summarizes the research results of the "Contribution to Risk Reduction in Decommissioning Works by the Elucidation of Basic Property of Radioactive Microparticles" conducted from FY2018 to FY2021 (this contract was extended to FY2021). The present study aims to understand the basic properties (size, chemical composition, isotopic composition - including concentration of $$alpha$$-emitters, electrostatic properties, and optical properties, etc.) of fine particles composed of silicate with insoluble properties which contain regions of highly concentrated radioactive cesium (Cs) released to the environment by the accident at the Fukushima Daiichi Nuclear Power Station of TEPCO in 2011 March.

Journal Articles

Effect of dissolved oxygen concentration on dynamic strain aging and stress corrosion cracking of SUS304 stainless steel under high temperature pressurized water

Hirota, Noriaki; Nakano, Hiroko; Fujita, Yoshitaka; Takeuchi, Tomoaki; Tsuchiya, Kunihiko; Demura, Masahiko*; Kobayashi, Yoshinao*

The IV International Scientific Forum "Nuclear Science and Technologies"; AIP Conference Proceedings 3020, p.030007_1 - 030007_6, 2024/01

Dynamic strain aging (DSA) and intergranular stress corrosion cracking (intragranular SCC) occur in high temperature pressurized water simulating a boiling water reactor environment due to changes in dissolved oxygen (DO) content, respectively. In order to clearly understand the difference between these phenomena, the mechanism of their occurrence was summarized. As a result, it was found that DSA due to intragranular cracking occurred in SUS304 stainless steel at low DO $$<$$ 1 ppb, while DSA was suppressed at DO 100 to 8500 ppb due to the formation of oxide films on the surface. On the other hand, when DO was increased to 20000 ppb, the film was peeled from the matrix, O element diffused to the grain boundary of the matrix, resulting in intergranular SCC. These results are indicated that the optimum DO concentration must be adjusted to suppress crack initiation due to DSA and intergranular SCC.

Journal Articles

Mutual separation of Am and Cm using ADAAM (alkyl DiAmide AMine) and reduction of volumes for liquid waste generated via batch-wise multistage extractions

Sasaki, Yuji; Kaneko, Masashi; Ban, Yasutoshi; Suzuki, Hideya*

Journal of Nuclear Science and Technology, 11 Pages, 2023/11

 Times Cited Count:0 Percentile:0.01(Nuclear Science & Technology)

The mutual separation of Am and Cm is conducted using an alkyl-diamide amine (ADAAM) extractant. ADAAM exhibits extremely high separation factor with respect to Am and Cm separation (5.9) in a nitric acid-$$n$$-dodecane system. The batch-wise multistage extractions are performed using a system containing 0.2 M ADAAM and 1.5 M nitric acid. In this multistage extraction, an organic solvent give 96.5% and 1.06% yields of Am and Cm. After the mutual separation of Am and Cm, an additional extraction step is included to reduce the volumes of these aqueous and organic phases. Taking these steps, Am and Cm can be recovered in just two or three stages in the aqueous phases.

Journal Articles

Random media criticality analysis methods in Monte Carlo solver Solomon

Ueki, Taro

Proceedings of 12th International Conference on Nuclear Criticality Safety (ICNC2023) (Internet), 9 Pages, 2023/10

A Monte Carlo Solver Solomon has been under development as an object-oriented code written in the C++14 standards. It consists of regular capabilities of criticality safety analysis and a special capability of random media criticality. In the latter capability, Solomon is equipped with a class for the random media modeled by the incomplete randomized Weierstrass function (IRWF). By this modeling, the uncertainty of random media criticality can be evaluated by executing criticality calculations over many IRWF-replicas. However, it is impossible to know beforehand how many IRWF-replicas should be computed. To deal with this issue, a bounded amplification (BA) technique has been newly equipped in Solomon. Applying BA to IRWF, it is possible to reduce the number of IRWF-replicas by more than 95% in terms of the upper limit estimation of neutron effective multiplication factor. Solomon is also equipped with a voxel-overlay (VO). This functionality is shown to be valuable for evaluating the resonance self-shielding effect.

Journal Articles

Elemental analysis and radioactivity evaluation of aerosols generated during heating of simulated fuel debris; The Urasol project in the framework of Fukushima Daiichi fuel debris removal

Tsubota, Yoichi; Porcheron, E.*; Journeau, C.*; Delacroix, J.*; Suteau, C.*; Lallot, Y.*; Bouland, A.*; Roulet, D.*; Mitsugi, Takeshi

Proceedings of International Conference on Environmental Remediation and Radioactive Waste Management (ICEM2023) (Internet), 6 Pages, 2023/10

In order to safely remove fuel debris from the Fukushima Daiichi Nuclear Power Station (1F), it is necessary to quantitatively evaluate radioactive airborne particulate generated by the cutting of nuclear fuel debris. We fabricated Uranium-bearing simulated fuel debris (SFD) with In/Ex-Vessel compositions and evaluated the physical and chemical properties of aerosols generated by heating the SFDs. Based on these results, we estimated the isotopic composition and radioactivity of aerosols produced when 1F-Unit2 fuel debris is laser cut, which is a typical example of a heating method. Plutonium, mainly $$^{238}$$Pu,$$^{241}$$Am, and $$^{244}$$Cm were found to be the alpha nuclide, and $$^{241}$$Pu, $$^{137}$$Cs-Ba, and $$^{90}$$Sr-Y were found to be the beta nuclide of interest.

Journal Articles

Aerosol characterization during heating and mechanical cutting of simulated uranium containing debris; The URASOL project in the framework of Fukushima Daiichi fuel debris removal

Porcheron, E.*; Journeau, C.*; Delacroix, J.*; Berlemont, R.*; Bouland, A.*; Lallot, Y.*; Tsubota, Yoichi; Ikeda, Atsushi; Mitsugi, Takeshi

Proceedings of International Conference on Environmental Remediation and Radioactive Waste Management (ICEM2023) (Internet), 5 Pages, 2023/10

Results of the URASOL project aimed at evaluating the generation and dispersion of radioactive aerosols during the cutting of fuel debris, a key issue in the decommissioning of the damaged reactors at the Fukushima Daiichi Nuclear Power Station (1F), are presented in this report. Characterization of aerosols generated during heating and mechanical cutting of simulated fuel debris in terms of mass concentration, real-time number density, mass-based particle size distribution, morphology, and chemical properties is reported. In the heating tests, an increase in particle size with increasing temperature was observed, and in terms of particle number density, the case using depleted uranium simulated fuel debris had a smaller number density than the test using Hf-containing simulated fuel debris. In mechanical cleavage, the aerodynamic median mass diameter of the aerosol was almost the same for the radioactive and non-radioactive samples (about 3.7$$sim$$4.4 $$mu$$m).

Journal Articles

Extraction of Rh(III) from hydrochloric acid by protonated NTAamide(C6) and analogous compounds and understanding of extraction equilibria by using UV spectroscopy and DFT calculations

Sasaki, Yuji; Kaneko, Masashi; Ban, Yasutoshi; Kinoshita, Ryoma; Matsumiya, Masahiko*; Shinoku, Kota*; Shiroishi, Hidenobu*

Analytical Sciences, 39(9), p.1575 - 1583, 2023/09

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

Extraction of Rh from HCl can be performed by NTAamide(C6) (hexahexyl-nitrilotriacetamide) and other related compounds into n-dodecane. We use ion-pair extraction of anionic species of Rh-chloride and protonated extractant. Rh behave as anion in hydrochloric acid and the tertiary nitrogen atom in extractant may be protonated to produce the quaternary amine in acidic condition. From the present work, the maximum distribution ratio of Rh(III) is 16. The D(Rh) values are changeable during preparation of the aqueous solutions because different Rh-Cl-H$$_{2}$$O complexes are formed in HCl media and show the slow exchange rate between Cl and H$$_{2}$$O. Using the UV spectrum, Rh-chloride solution having the peak of spectrum at 504 nm can be extracted effectively, where RhCl$$_{4}$$(H$$_{2}$$O)$$^-$$ and RhCl$$_5$$(H$$_2$$O)$$^2$$$$^-$$ exist mainly from DFT calculation. Stoichiometry of one-one complex of Rh and NTAamide is obtained from slope analysis, and 85 mM of concentrated Rh ion can be extracted.

Journal Articles

Evaluation of the remaining spent extraction solvent in vermiculite after leaching tests via PIXE analysis

Arai, Yoichi; Watanabe, So; Hasegawa, Kenta; Okamura, Nobuo; Watanabe, Masayuki; Takeda, Keisuke*; Fukumoto, Hiroki*; Ago, Tomohiro*; Hagura, Naoto*; Tsukahara, Takehiko*

Nuclear Instruments and Methods in Physics Research B, 542, p.206 - 213, 2023/09

 Times Cited Count:1 Percentile:0.02(Instruments & Instrumentation)

Journal Articles

Solubility of FeSe$$_{2}$$(cr) at 318 K in the presence of iron

Yoshida, Yasushi*; Kitamura, Akira; Shibutani, Sanae*

Journal of Nuclear Science and Technology, 60(8), p.900 - 910, 2023/08

 Times Cited Count:0 Percentile:0.01(Nuclear Science & Technology)

Journal Articles

The Development of a Multiphysics Coupled Solver for Studying the Effect of Dynamic Heterogeneous Configuration on Particulate Debris Bed Criticality and Cooling Characteristics

Li, C.-Y.; Wang, K.*; Uchibori, Akihiro; Okano, Yasushi; Pellegrini, M.*; Erkan, N.*; Takata, Takashi*; Okamoto, Koji*

Applied Sciences (Internet), 13(13), p.7705_1 - 7705_29, 2023/07

 Times Cited Count:1 Percentile:56.82(Chemistry, Multidisciplinary)

Journal Articles

Local electronic structure of interstitial hydrogen in MgH$$_2$$ inferred from muon study

Kadono, Ryosuke*; Hiraishi, Masatoshi*; Okabe, Hirotaka*; Koda, Akihiro*; Ito, Takashi

Journal of Physics; Condensed Matter, 35(28), p.285503_1 - 285503_13, 2023/07

 Times Cited Count:0 Percentile:0(Physics, Condensed Matter)

Journal Articles

Extraction of Se(iv) and Se(vi) from aqueous HCl solution by using a diamide-containing tertiary amine

Narita, Hirokazu*; Maeda, Motoki*; Tokoro, Chiharu*; Suzuki, Tomoya*; Tanaka, Mikiya*; Shiwaku, Hideaki; Yaita, Tsuyoshi

RSC Advances (Internet), 13(25), p.17001 - 17007, 2023/06

 Times Cited Count:1 Percentile:44.81(Chemistry, Multidisciplinary)

no abstracts in English

JAEA Reports

Research on atmospheric radioactivity concentration in the specified reconstruction and revitalization base (FY2018-FY2021)

Abe, Tomohisa; Funaki, Hironori; Yoshimura, Kazuya; Shiribiki, Natsu*; Sanada, Yukihisa

JAEA-Data/Code 2023-001, 38 Pages, 2023/05

JAEA-Data-Code-2023-001.pdf:3.04MB
JAEA-Data-Code-2023-001-appendix(CD-ROM).zip:32.02MB

In this study, commissioned by the Cabinet Office, we conducted a survey on radioactive materials in atmospheric dust in three municipalities (Futaba Town, Okuma Town, and Tomioka Town) in Fukushima Prefecture to contribute to the assessment of internal exposure in the Specified Reconstruction and Revitalization Base (SRRB). Air dust samplers were installed in the targeted municipalities to investigate the atmospheric $$^{137}$$Cs concentrations and to evaluate internal exposure doses based on measured value. This report summarizes the results of measurements between 2018 and 2021. A database of information on internal exposure dose assessment results based on atmospheric radioactivity concentrations and actual measurements, and meteorological observation data was compiled.

Journal Articles

Double diffusive dissolution model of UO$$_{2}$$ pellet in molten Zr cladding

Ito, Ayumi*; Yamashita, Susumu; Tasaki, Yudai; Kakiuchi, Kazuo; Kobayashi, Yoshinao*

Journal of Nuclear Science and Technology, 60(4), p.450 - 459, 2023/04

 Times Cited Count:0 Percentile:0.01(Nuclear Science & Technology)

JAEA Reports

Challenge of novel hybrid-waste-solidification of mobile nuclei generated in Fukushima Nuclear Power Station and establishment of rational disposal concept and its safety assessment (Contract research); FY2021 Nuclear Energy Science & Technology and Human Resource Development Project

Collaborative Laboratories for Advanced Decommissioning Science; Tokyo Institute of Technology*

JAEA-Review 2022-072, 116 Pages, 2023/03

JAEA-Review-2022-072.pdf:6.32MB

The Collaborative Laboratories for Advanced Decommissioning Science (CLADS), Japan Atomic Energy Agency (JAEA), had been conducting the Nuclear Energy Science & Technology and Human Resource Development Project (hereafter referred to "the Project") in FY2021. The Project aims to contribute to solving problems in the nuclear energy field represented by the decommissioning of the Fukushima Daiichi Nuclear Power Station (1F), Tokyo Electric Power Company Holdings, Inc. (TEPCO). For this purpose, intelligence was collected from all over the world, and basic research and human resource development were promoted by closely integrating/collaborating knowledge and experiences in various fields beyond the barrier of conventional organizations and research fields. The sponsor of the Project was moved from the Ministry of Education, Culture, Sports, Science and Technology to JAEA since the newly adopted proposals in FY2018. On this occasion, JAEA constructed a new research system where JAEA-academia collaboration is reinforced and medium-to-long term research/development and human resource development contributing to the decommissioning are stably and consecutively implemented. Among the adopted proposals in FY2021, this report summarizes the research results of the "Challenge of novel hybrid-waste-solidification of mobile nuclei generated in Fukushima Nuclear Power Station and establishment of rational disposal concept and its safety assessment" conducted in FY2021. The present study aims to establish the rational waste disposal concept of a variety of wastes generated in 1F by the novel hybrid-waste-solidification. The phosphate form of ALPS sediment wastes containing Eu$$^{3+}$$, Ce$$^{4+}$$, Sr$$^{2+}$$ and Cs$$^{+}$$ were synthesized as well as radioactive $$^{95}$$Sr, $$^{136}$$Cs and $$^{126}$$I which are both $$gamma$$ emitters, AREVA sludge and Iodine Calcium apatite were synthesized, and they were processed to the stabilization treatment such as sintering and Spark Plasma ...

Journal Articles

Selective adsorption of Pd(II) over Ag(I) in nitric acid solutions using nitrogen-donor-type adsorbents

Suzuki, Tomoya*; Otsubo, Ukyo*; Ogata, Takeshi*; Shiwaku, Hideaki; Kobayashi, Toru; Yaita, Tsuyoshi; Matsuoka, Mitsuaki*; Murayama, Norihiro*; Narita, Hirokazu*

Separation and Purification Technology, 308, p.122943_1 - 122943_7, 2023/03

 Times Cited Count:2 Percentile:22.61(Engineering, Chemical)

HNO$$_{3}$$ leaching is used in recycling Pd metal from spent products that primarily contain Ag, and most Pd residues are separated from solutions containing Ag(I). However, a small amount of Pd(II) often remains in these Ag(I) solutions. Therefore, the separation of Pd(II) and Ag(I) in HNO$$_{3}$$ solutions is essential to promote efficient Pd recycling. In this study, the separation of Pd(II) and Ag(I) in HNO$$_{3}$$ solutions was investigated using four N-donor-type adsorbents functionalized with amine (R-Amine), iminodiacetic acid (R-IDA), pyridine (R-Py), or bis-picolylamine (R-BPA). R-Amine, R-IDA, and R-Py selectively adsorbed Pd(II) over Ag(I), Cu(II), Ni(II), and Fe(III) from HNO$$_{3}$$ solutions (0.3-7 M), but R-Amine exhibited a lower Pd adsorption efficiency. In contrast, $$>$$90% of Pd(II), Ag(I), and Cu(II) were adsorbed by R-BPA over the entire range of HNO$$_{3}$$ concentrations. Structural analyses of the adsorbed metal ions using Fourier transform infrared spectroscopy and extended X-ray absorption fine structure spectroscopy revealed the separation mechanisms of the N-donor-type adsorbents. Pd(II) adsorption on R-IDA, R-Py, and R-BPA occurred via Pd(II) coordination of the functional groups (iminodiacetic acid, pyridine, and bis-picolylamine, respectively), whereas that on R-Amine occurred via anion exchange of NO$$_{3}$$$$^{-}$$ with [Pd(NO$$_{3}$$)$$_{4}$$]$$^{2-}$$. The coordinative adsorption mechanisms resulted in the higher Pd(II) adsorption behaviors of R-IDA, R-Py, and R-BPA. HCl (5.0 M) and thiourea (0.1 M) eluents desorbed 83% of Pd(II) from R-IDA and 95% from R-Py, respectively. R-Py was the most effective Pd(II) adsorbent based on adsorption selectivity and desorption efficiency.

JAEA Reports

Research on radioactive aerosol control and decontamination at Fukushima Daiichi Nuclear Power Station decommissioning (Contract research); FY2021 Nuclear Energy Science & Technology and Human Resource Development Project

Collaborative Laboratories for Advanced Decommissioning Science; The University of Tokyo*

JAEA-Review 2022-061, 59 Pages, 2023/02

JAEA-Review-2022-061.pdf:2.38MB

The Collaborative Laboratories for Advanced Decommissioning Science (CLADS), Japan Atomic Energy Agency (JAEA), had been conducting the Nuclear Energy Science & Technology and Human Resource Development Project (hereafter referred to "the Project") in FY2021. The Project aims to contribute to solving problems in the nuclear energy field represented by the decommissioning of the Fukushima Daiichi Nuclear Power Station, Tokyo Electric Power Company Holdings, Inc. (TEPCO). For this purpose, intelligence was collected from all over the world, and basic research and human resource development were promoted by closely integrating/collaborating knowledge and experiences in various fields beyond the barrier of conventional organizations and research fields. The sponsor of the Project was moved from the Ministry of Education, Culture, Sports, Science and Technology to JAEA since the newly adopted proposals in FY2018. On this occasion, JAEA constructed a new research system where JAEA-academia collaboration is reinforced and medium-to-long term research/development and human resource development contributing to the decommissioning are stably and consecutively implemented. Among the adopted proposals in FY2021, this report summarizes the research results of the "Research on radioactive aerosol control and decontamination at Fukushima Daiichi Nuclear Power Station decommissioning" conducted in FY2021. The present study aims to develop a safe laser decontamination system that simultaneously incorporates an advanced particle detection and characterization system together with aerosol dispersion control in collaboration with the UK researchers. By using the UK partner's fundamental studies related to aerosol and water interface interactions, various methods such as electro-chemical processing of water-mist particles and spray droplets will be applied for effective control of ultra-fine aerosol particle dispersions in a large containment volume.

Journal Articles

Power profile analysis of criticality accidents involving fissile solution boiling with considering evaporation

Watanabe, Tomoaki; Yamane, Yuichi

Journal of Nuclear Science and Technology, 9 Pages, 2023/00

 Times Cited Count:0 Percentile:0.01(Nuclear Science & Technology)

The total fission energy released in a criticality accident involving fissile solution boiling tends to be high because the relatively high fission power continues during boiling. Simulating fission power change correctly during boiling seems essential to estimate the total fission energy. Fission power during boiling changes depending on fissile concentration and volume as the solution evaporates. In this study, we investigated the effect of concentration and volume change on estimated total fission energy for a long time of boiling. We introduced a model calculating the evaporation of fissile solution into the modified quasi-steady-state method to simulate power change during boiling. Three CRAC experiments and the Idaho Chemical Processing Plant (ICPP) criticality accident in 1959 were analyzed. As a result, the calculated energy considering concentration and volume change during boiling reproduced the measured energy well.

Journal Articles

Thermodynamic analysis for solidification path of simulated ex-vessel corium

Sato, Takumi; Nagae, Yuji; Kurata, Masaki; Quaini, A.*; Gu$'e$neau, C.*

CALPHAD; Computer Coupling of Phase Diagrams and Thermochemistry, 79, p.102481_1 - 102481_11, 2022/12

 Times Cited Count:0 Percentile:0.01(Thermodynamics)

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