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Soma, Yasutaka; Komatsu, Atsushi; Igarashi, Takahiro
Corrosion Science, 265, p.113182_1 - 113182_13, 2026/06
Times Cited Count:0 Percentile:0.00(Materials Science, Multidisciplinary)
/Pu
couple in NaCl-2CsCl meltHayashi, Hirokazu; Minato, Kazuo*
Journal of Radioanalytical and Nuclear Chemistry, 335(6), p.4233 - 4240, 2026/06
Times Cited Count:0 Percentile:0.00(Chemistry, Analytical)Anhydrous plutonium trichloride (PuCl
) was synthesized by a solid-state reaction of plutonium nitride with cadmium chloride. The lattice constants of hexagonal PuCl
were refined from its powder X-ray diffraction pattern to be a = 0.7394
0.0006 nm and c = 0.4244
0.0006 nm, which are close to the reported values. Using the synthesized PuCl
sample, electrochemical behavior of plutonium in NaCl-2CsCl melt at 823-923 K was investigated by cyclic voltammetry and open-circuit chronopotentiometry after polarization. The results show that Pu
ions are reduced to Pu metal by single-step mechanism in the NaCl-2CsCl melt. The apparent standard potentials of Pu
/Pu
redox couple were determined to be E
(Pu
/Pu
) = -3.514 + 8.60
10
T vs. Cl
/Cl
(V). The activity coefficients of Pu
ions were determined using the previously reported Gibbs free energy of formation for PuCl
in the supercooled liquid state.
Pu
Am
O
Vauchy, R.; Horii, Yuta; Hirooka, Shun; Akashi, Masatoshi; Sunaoshi, Takeo*; Nakamichi, Shinya; Saito, Kosuke
Proceedings of 34th Nuclear Energy for New Europe (NENE2025) , p.232 - 238, 2026/01
= 0.01-600
C,
= 1-3000 bars, 
= 0.35-1.1 g cm
, and
= 0
Walker, C. S.*; Arthur, R. C.*; Anraku, Sohtaro; Sasamoto, Hiroshi; Mihara, Morihiro
Applied Geochemistry, 175, p.106086_1 - 106086_17, 2024/11
Times Cited Count:0 Percentile:0.00(Geochemistry & Geophysics)The thermodynamic properties and revised Helgeson-Kirkham-Flowers equation of state (r-H-K-F EoS) parameters of the hydrated (Si(OH)
(aq), SiO(OH)
and SiO
(OH)
) and fictive dehydrated (SiO
(aq), HSiO
and SiO
) monomeric silicon species are used extensively to describe the pH, composition, temperature, and pressure dependence of formation/breakdown reactions of all silicon-bearing compounds globally. Experimental log10 equilbrium constant, K values describing the formation reactions of the hydrated and dehydrated monomeric silicon species were therefore compiled from the literature, extrapolated to zero ionic strength by specific ion interaction theory as required and used to derive their thermodynamic properties and r-H-K-F EoS parameters. Consideration of all formation reactions in the same study provides a collective, internally consistent update to the thermodynamic properties and r-H-K-F EoS parameters of the monomeric silicon species that can provide a satisfactory match to the experimental log10 K values at
= 0.01-600
C,
= 1-3000 bars, 
= 0.35-1.1 g cm
, and zero ionic strength. These temperature and pressure limits comfortably bracket t=0.01-100
C and P =1-270 bars relecant to the geological disposal of radioactive wastes at depths of up to 1 km.
-CsOHRizaal, M.; Luu, V. N.; Nakajima, Kunihisa; Miwa, Shuhei
Proceedings of International Topical Workshop on Fukushima Decommissioning Research 2024 (FDR2024) (Internet), 4 Pages, 2024/10
Toigawa, Tomohiro; Kai, Takeshi; Kumagai, Yuta; Yokoya, Akinari*
Journal of Chemical Physics, 160(21), p.214119_1 - 214119_9, 2024/06
Times Cited Count:4 Percentile:50.47(Chemistry, Physical)The spur reaction is crucial for determining radiolysis or photolysis in liquid, but the spur expansion process has yet to be elucidated. One reason is the need to understand the role of the dielectric response of the solvating molecules surrounding the charged species generated by ionization. The dielectric response corresponds to the time evolution of the permittivity and might affect the chemical reaction-diffusion of the species in a spur expansion process. This study examined the competitive relationship between reaction-diffusion kinetics and the dielectric response by solving the Debye-Smoluchowski equation while considering the dielectric response. The Coulomb force between the charged species gradually decreases with the dielectric response. Our calculation results found a condition where fast recombination occurs before the dielectric response is complete. Although it has been reported that the primary G-values of free electrons depend on the static dielectric constant under low-linear-energy transfer radiation-induced ionization, we propose that considering the dielectric response can provide a deeper insight into fast recombination reactions under high-linear-energy transfer radiation- or photo-induced ionization. Our simulation method enables the understanding of fast radiation-induced phenomena in liquids.
Hayashi, Hirokazu; Minato, Kazuo*
Electrochemistry (Internet), 92(4), p.043020_1 - 043020_5, 2024/04
Times Cited Count:1 Percentile:4.77(Electrochemistry)The electrochemical behavior of neptunium in NaCl-2CsCl melt at 823-923 K was investigated by cyclic voltammetry, differential pulse voltammetry, and open-circuit chronopotentiometry after polarization. The results show that Np
ions are reduced to Np metal by a two-step mechanism via Np
ions in NaCl-2CsCl melt. The diffusion coefficients of Np
and Np
ions were determined from cyclic voltammograms. The apparent standard potentials of Np
/Np
and Np
/Np
redox couples have been determined to be E
(Np
/Np
) = -3.353 + 7.67
10
T, and E
(Np
/Np
) = -1.175 + 4.99
10
T vs. Cl
/Cl
(V), respectively. The activity coefficients of Np
and Np
ions were also determined using the reported data on the Gibbs free energy of formation for NpCl
and NpCl
in supercooled liquid state.
Zablackaite, G.; Shiotsu, Hiroyuki; Kido, Kentaro; Sugiyama, Tomoyuki
Nuclear Engineering and Technology, 56(2), p.536 - 545, 2024/02
Times Cited Count:2 Percentile:40.43(Nuclear Science & Technology)Yamada, Raiki; Takahashi, Toshiro*; Ogita, Yasuhiro
Journal of Mineralogical and Petrological Sciences (Internet), 118(1), p.221219a_1 - 221219a_26, 2023/11
Times Cited Count:6 Percentile:53.12(Mineralogy)Oligocene to Miocene volcanic rocks from the Toyama basin of the SW Japan arc, that were formed during back-arc spreading in the Japan Sea, were examined to reveal their petrogeneses and temporal change of arc volcanism during the Japan Sea opening. We reported whole-rock major and trace element and Sr-Nd isotopic compositions of andesites and rhyolites (23-16 Ma) and quantitatively discussed their petrogenesis, based on comparison with the results of model calculations, in this paper. Main concluding remarks are as follows: (1) Rhyolite magmas were generated by crustal assimilation of basaltic to andesitic magmas. (2) Andesites consist of high-Mg andesite, high-Sr, and tholeiitic andesite, generated by interaction among slab fluid, slab melt, and crustal material. (3) Upwelling of the asthenospheric mantle into the mantle wedge caused melting of the subducting Pacific plate, and andesitic magmatism induced rhyolitic magmatism.
Miyakawa, Kazuya; Nakata, Kotaro*
JAEA-Data/Code 2022-013, 19 Pages, 2023/03
In the Horonobe Underground Research Laboratory (URL) project, groundwater chemistry was analyzed to investigate changes due to the excavation of the underground facility and to review geochemical models until the fiscal year 2019. From the fiscal year 2020, to proceed remaining important issues deduced from the conclusion of the investigations during the fiscal year 2015-2019, primary data such as groundwater chemistry need to be successively acquired. Here, the chemical analysis of 54 groundwater samples in 2022 from boreholes drilled in the 140 m, 250 m, 350 m gallery in the Horonobe URL, and water rings settled in three vertical shafts is presented. Analytical results include groundwater chemistry such as pH, electrical conductivity, dissolved components (Na
, K
, Ca
, Mg
, Li
, NH
, F
, Cl
, Br
, NO
, NO
, PO
, SO
, Total-Mn, Total-Fe, Al, B, Sr, Ba, I, alkalinity, dissolved organic carbon, dissolved inorganic carbon, CO
, HCO
, Fe
, sulfide), and 
O,
D along with a detailed description of analytical methods.
Collaborative Laboratories for Advanced Decommissioning Science; Tokyo Institute of Technology*
JAEA-Review 2022-028, 54 Pages, 2022/11
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 FY2019, this report summarizes the research results of the "Development of Tailor-made Adsorbents for Uranium Recovery from Seawater on the Basis of Uranyl Coordination Chemistry" conducted from FY2019 to FY2021. Since the final year of this proposal was FY2021, the results for three fiscal years were summarized. The present study aims to develop a new ligand class for efficient and selective capture of uranium from seawater. On the basis of deep understanding on uranyl coordination chemistry, we design molecular structures of pentadentate ligands as functional moieties for uranium adsorption from seawater and study fundamental coordination chemistry of uranyl ion with those ligands in order to resolve current problems in uranium recovery technology …
Osaka, Masahiko; Gou
llo, M.*; Nakajima, Kunihisa
Journal of Nuclear Science and Technology, 59(3), p.292 - 305, 2022/03
Times Cited Count:12 Percentile:72.76(Nuclear Science & Technology)Research on the fission product chemistry made after the severe accident of the Fukushima Daiichi Nuclear Power Station were reviewed with focus on the Cesium chemistry in terms of two regimes, namely the accidental source term and the long-term source term via aqueous phase towards the decommissioning. For the accidental source term, Cs chemical interaction with Mo, B and Si were reviewed. Regarding the unique issue of long-term source term via aqueous phase, Cs penetration into concrete and fuel debris leaching were mentioned as the main sources of FPs. Efforts on the preparation of thermodynamic data for the Cs complex oxides were described. All these Cs chemical behaviors should be modelled and validated/verified through the analysis and evaluation of the actual samples including fuel debris that would be taken from the Fukushima Daiichi Nuclear Power Station in near future.
Collaborative Laboratories for Advanced Decommissioning Science; Tokyo Institute of Technology*
JAEA-Review 2021-041, 42 Pages, 2022/01
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 FY2019, this report summarizes the research results of the "Development of tailor-made adsorbents for uranium recovery from seawater on the basis of uranyl coordination chemistry" conducted in FY2020. On the basis of deep understanding on uranyl coordination chemistry, we design molecular structures of pentadentate ligands as functional moieties for uranium adsorption from seawater and study coordination chemistry of uranyl ion with those ligands in order to resolve current problems in uranium recovery technology from seawater and to develop novel selective and efficient adsorbents for this purpose.
Rizaal, M.; Miwa, Shuhei; Suzuki, Eriko; Imoto, Jumpei; Osaka, Masahiko; Gou
llo, M.*
ACS Omega (Internet), 6(48), p.32695 - 32708, 2021/12
Times Cited Count:6 Percentile:23.78(Chemistry, Multidisciplinary)Miwa, Shuhei; Miyahara, Naoya*; Nakajima, Kunihisa; Imoto, Jumpei; Suzuki, Eriko
Nihon Genshiryoku Gakkai-Shi ATOMO
, 63(12), p.825 - 829, 2021/12
In the BWR severe accident, it was indicated that the control material boron significantly influences chemical behavior and transition behavior of cesium, which is important from the viewpoint of exposure, and it causes great uncertainty in the prediction of environmental release and distribution in the reactor. Therefore, in order to elucidate the important chemistry to be considered in severe accident analysis, we have developed the experimental setup that enables the evaluation of chemistry during transportation in the reactor, and evaluated cesium chemistry. Based on the results, we developed the chemistry database named ECUME composed of datasets and models that are the basis of chemical reaction analysis so that chemical behavior could be evaluated by severe accident analysis code.
Miyakawa, Kazuya
JAEA-Data/Code 2021-003, 25 Pages, 2021/05
Development of technologies to investigate properties of deep geological environment and model development of geological environment have been pursued in "Geoscientific Research" in the Horonobe Underground Research Laboratory (HURL) project. In the fiscal year 2020, to proceed remaining important issues which were deduced from the conclusion of the investigations during the fiscal year 2015-2019, basic data such as groundwater chemistry need to be successively acquired. In the fiscal year 2020, groundwater was sampled from boreholes drilled in the 140 m, 250 m, 350 m gallery in the HURL, and water rings settled in three each vertical shaft, and groundwater chemistries of 41 samples were analyzed. Here, analytical results of groundwater chemistry such as physicochemical parameters, dissolved ions, oxygen and hydrogen isotope ratios, and tritium content, which were obtained in the fiscal year 2020, were reported along with a detailed description of analytical methods.
-octylnitrilo-triacetamide (HONTA) complexes of americium and europiumToigawa, Tomohiro; Peterman, D. R.*; Meeker, D. S.*; Grimes, T. S.*; Zalupski, P. R.*; Mezyk, S. P.*; Cook, A. R.*; Yamashita, Shinichi*; Kumagai, Yuta; Matsumura, Tatsuro; et al.
Physical Chemistry Chemical Physics, 23(2), p.1343 - 1351, 2021/01
Times Cited Count:26 Percentile:83.13(Chemistry, Physical)The candidate An(III)/Ln(III) separation ligand hexa-
-octylnitrilo-triacetamide (HONTA) was irradiated under envisioned SELECT (Solvent Extraction from Liquid waste using Extractants of CHON-type for Transmutation) process conditions using a solvent test loop in conjunction with cobalt-60 gamma irradiation. We demonstrate that HONTA undergoes exponential decay with increasing gamma dose to produce a range of degradation products which have been identified and quantified by HPLC-ESI-MS/MS techniques. The combination of HONTA destruction and degradation product ingrowth, particularly dioctylamine, negatively impacts the extraction and back-extraction of both americium and europium ions. The loss of HONTA was attributed to its reaction with the solvent (
-dodecane) radical cation of
(HONTA + R
) = (7.61
0.82)
10
M
s
obtained by pulse radiolysis techniques. However, when this ligand is bound to either americium or europium ions, the observed
-dodecane radical cation kinetics increase by over an order of magnitude. This large reactivity increase to additional reaction pathways occurring upon metal-ion binding. Lastly nanosecond time-resolved measurements showed that both direct and indirect HONTA radiolysis yielded the short-lived (
100 ns) HONTA radical cation as well as a longer-lived (
s) HONTA triplet excited state. These HONTA species are important precursors to the suite of HONTA degradation products observed.
Collaborative Laboratories for Advanced Decommissioning Science; Tokyo Institute of Technology*
JAEA-Review 2020-026, 41 Pages, 2020/12
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 FY2019. 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 FY2019, this report summarizes the research results of the "Development of Tailor-Made Adsorbents for Uranium Recovery from Seawater on the Basis of Uranyl Coordination Chemistry". On the basis of deep understanding on uranyl coordination chemistry, we design molecular structures of pentadentate ligands as functional moieties for uranium adsorption from seawater and study coordination chemistry of uranyl ion with those ligands in order to resolve current problems in uranium recovery technology from seawater and to develop novel selective and efficient adsorbents for this purpose.
Miwa, Shuhei; Nakajima, Kunihisa; Suzuki, Chikashi; Rizaal, M.; Suzuki, Eriko; Horiguchi, Naoki; Osaka, Masahiko
Proceedings of Joint International Conference on Supercomputing in Nuclear Applications + Monte Carlo 2020 (SNA + MC 2020), p.253 - 260, 2020/12
We have proceeded the fundamental study for the improvement of the evaluation of fission product (FP) chemistry and the treatment of fine space resolution which are main issues for the evaluation of FP behaviors in a severe accident (SA). We have been developing FP chemistry database named ECUME for the improvement of SA analysis codes. We prepared thermodynamic data for Cs compounds which is no experimental data available by computational approach. Regarding the space resolution issue, we have been developing analysis tool named CHASER based on 3D-CFD code with the model for FP chemistry. More accurate evaluation of FP behavior can be achieved by incorporating ECUME to the CHASER.
Fukuda, Kenji; Watanabe, Yusuke; Murakami, Hiroaki; Amano, Yuki; Aosai, Daisuke*; Hara, Naohiro*
JAEA-Data/Code 2020-012, 80 Pages, 2020/10
Japan Atomic Energy Agency has been investigating groundwater chemistry to understand the influence of excavation and maintenance of underground facilities as part of the Mizunami Underground Research Laboratory (MIU) Project in Mizunami, Gifu, Japan. In this report, we compiled data of groundwater chemistry and microbiology obtained at the MIU in the fiscal year 2019. In terms of ensuring traceability of data, basic information (e.g. sampling location, sampling time, sampling method and analytical method) and methodology for quality control are described.