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JAEA Reports

Development of tailor-made adsorbents for uranium recovery from seawater on the basis of uranyl coordination chemistry (Contract research); FY2021 Nuclear Energy Science & Technology and Human Resource Development Project

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

JAEA-Review 2022-028, 54 Pages, 2022/11

JAEA-Review-2022-028.pdf:2.97MB

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 …

JAEA Reports

Identification of altered phases of fuel debris by laser fluorescence spectroscopy (Contract research); FY2020 Nuclear Energy Science & Technology and Human Resource Development Project

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

JAEA-Review 2022-007, 59 Pages, 2022/06

JAEA-Review-2022-007.pdf:2.09MB

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 "Identification of altered phases of fuel debris by laser fluorescence spectroscopy" conducted from FY2018 to FY2021 (this contract was extended to FY2021). Since the final year of this proposal was FY2021, the results for four fiscal years were summarized. The present study aims to identify alteration phases occurring on the surface fuel debris at various conditions, using time-resolved laser fluorescence spectroscopy (TRLFS), which is a selective analytical technique for U(VI), a major constituent of fuel debris and stable in oxidizing conditions.

JAEA Reports

Development of tailor-made adsorbents for uranium recovery from seawater on the basis of uranyl coordination chemistry (Contract research); FY2020 Nuclear Energy Science & Technology and Human Resource Development Project

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

JAEA-Review 2021-041, 42 Pages, 2022/01

JAEA-Review-2021-041.pdf:2.03MB

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.

JAEA Reports

Identification of altered phases of fuel debris by laser fluorescence spectroscopy (Contract research); FY2019 Nuclear Energy Science & Technology and Human Resource Development Project

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

JAEA-Review 2020-053, 64 Pages, 2021/01

JAEA-Review-2020-053.pdf:3.58MB

JAEA/CLADS had been conducting the Nuclear Energy Science & Technology and Human Resource Development Project in FY2019. Among the adopted proposals in FY2019, this report summarizes the research results of the "Identification of Altered Phases of Fuel Debris by Laser Fluorescence Spectroscopy" conducted in FY2019.

JAEA Reports

Development of tailor-made adsorbents for uranium recovery from seawater on the basis of uranyl coordination chemistry (Contract research); FY2019 Nuclear Energy Science & Technology and Human Resource Development Project

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

JAEA-Review 2020-026, 41 Pages, 2020/12

JAEA-Review-2020-026.pdf:3.25MB

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.

JAEA Reports

Identification of altered phases of fuel debris by laser fluorescence spectroscopy (Contract research) FY2018 Center of World Intelligence Project for Nuclear Science/Technology and Human Resource Development

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

JAEA-Review 2019-030, 66 Pages, 2020/03

JAEA-Review-2019-030.pdf:7.11MB

JAEA/CLADS, had been conducting the Center of World Intelligence Project for Nuclear Science/Technology and Human Resource Development (hereafter referred to "the Project") in FY2018. The Project aims to contribute to solving problems in nuclear energy field represented by the decommissioning of the Fukushima Daiichi Nuclear Power Station, Tokyo Electric Power Company Holdings, Inc. 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. Among the adopted proposals in FY2018, this report summarizes the research results of the "Identification of Altered Phases of Fuel Debris by Laser Fluorescence Spectroscopy". In the present study, we focus on uranium that is the main component element in debris, and identify the altered phase produced on the debris surface under various conditions by time-resolved laser fluorescence spectroscopy (TRLFS) with high sensitivity to hexavalent uranium (U(VI)) that is stable in oxidation environment. In particular, further high-sensitive and high-resolution measurements are implemented by improving the fluorescence yields and suppressing the broadening of the peaks through the measurements at ultra-low temperature. In addition, with the supports by quantum chemical calculations, multivariate analysis, and machine learning, the method will lead to the identification of multicomponent and heterogeneous altered phase of fuel debris.

Journal Articles

Estimation of hydrogen gas production at transient criticality in uranyl nitrate solution

Yoshida, Ryoichiro; Yamane, Yuichi; Abe, Hitoshi

Proceedings of International Nuclear Fuel Cycle Conference / Light Water Reactor Fuel Performance Conference (Global/Top Fuel 2019) (USB Flash Drive), p.408 - 414, 2019/09

In a criticality accident, it is known that some kinds of radiolysis gases are generated mainly due to kinetic energy of fission fragments. Hydrogen gas (H$$_{2}$$) is one of them, which is able to initiate explosion. The rate of H$$_{2}$$ generation and its total amount can be estimated from the number of fission per second if its G value is known. In this study, it was tried to estimate G value of hydrogen gas (G(H$$_{2}$$)) by using the H$$_{2}$$ concentration measured as time-series data in Transient Experiment Critical Facility (TRACY) which was carried out by Japan Atomic Energy Agency. There was time lag in the measured H$$_{2}$$ concentration from its generation. To overcome those problems, measured profile of H$$_{2}$$ concentration was reproduced based on a hypothetical model and its total amount was evaluated. Based on the model, the obtained G(H$$_{2}$$) was 1.2.

JAEA Reports

Stabilization of MOX dissolving solution at STACY

Kobayashi, Fuyumi; Sumiya, Masato; Kida, Takashi; Kokusen, Junya; Uchida, Shoji; Kaminaga, Jota; Oki, Keiichi; Fukaya, Hiroyuki; Sono, Hiroki

JAEA-Technology 2016-025, 42 Pages, 2016/11

JAEA-Technology-2016-025.pdf:17.88MB

A preliminary test on MOX fuel dissolution for the STACY critical experiments had been conducted in 2000 through 2003 at Nuclear Science Research Institute of JAEA. Accordingly, the uranyl / plutonium nitrate solution should be reconverted into oxide powder to store the fuel for a long period. For this storage, the moisture content in the oxide powder should be controlled from the viewpoint of criticality safety. The stabilization of uranium / plutonium solution was carried out under a precipitation process using ammonia or oxalic acid solution, and a calcination process using a sintering furnace. As a result of the stabilization operation, recovery rate was 95.6% for uranium and 95.0% for plutonium. Further, the recovered oxide powder was calcined again in nitrogen atmosphere and sealed immediately with a plastic bag to keep its moisture content low and to prevent from reabsorbing atmospheric moisture.

Journal Articles

Diffusion and adsorption of uranyl ion in clays; Molecular dynamics study

Arima, Tatsumi*; Idemitsu, Kazuya*; Inagaki, Yaohiro*; Kawamura, Katsuyuki*; Tachi, Yukio; Yotsuji, Kenji

Progress in Nuclear Energy, 92, p.286 - 297, 2016/09

 Times Cited Count:12 Percentile:71.23(Nuclear Science & Technology)

Diffusion and adsorption behavior of uranyl (UO$$_2^{2+}$$) species is important for the performance assessment of radioactive waste disposal. The diffusion behaviors of UO$$_2^{2+}$$, K$$^{+}$$, CO$$_3^{2-}$$ and Cl$$^{-}$$ and H$$_{2}$$O in the aqueous solutions were evaluated by molecular dynamics (MD) calculations. The diffusion coefficient (De) of UO$$_2^{2+}$$ is the smallest and is 26% less than the self-diffusion coefficient of H$$_{2}$$O. For the aqueous solution with high concentration of carbonate ions, uranyl carbonate complexes: UO$$_{2}$$CO$$_{3}$$ and UO$$_{2}$$(CO$$_{3}$$)$$^{2-}$$ can be observed. For the clay (montmorillonite or illite)-aqueous solution systems, the adsorption and diffusion behaviors of UO$$_2^{2+}$$ and K$$^{+}$$ were evaluated by MD calculations. The distribution coefficients (Kd) increase with the layer charge of clay, and Kd of UO$$_2^{2+}$$ might be smaller than that of K$$^{+}$$. Further, their two-dimensional diffusion coefficients were relatively small in the adsorption layer and were extremely small for illite with higher layer charge.

Journal Articles

Electrochemical properties of uranium(VI) complexes with multidentate ligands in $$N,N$$-dimethylformamide

Kim, S.-Y.; Asakura, Toshihide; Morita, Yasuji; Ikeda, Yasuhisa*

Journal of Alloys and Compounds, 408-412, p.1291 - 1295, 2006/02

 Times Cited Count:10 Percentile:54.57(Chemistry, Physical)

The electrochemical reactions of UO$$_{2}$$($$beta$$-diketonato)$$_{2}$$DMF, UO$$_{2}$$(trop)$$_{2}$$DMF and UO$$_{2}$$(sap)(DMF)$$_{2}$$, (DMF = N,N-dimethylformamide, $$beta$$-diketonate = thenoyltrifluoroacetonate (ttfa), benzoyltrifluoroacetonate (btfa), and dibenzoylmethanate(dbm), trop = tropolonate, and sap = 2-salicylidenaminophenolate) complexes in DMF solution containing tetrabutyl ammonium perchlorate as a supporting electrolyte have been studied with cyclic voltammetry. These uranyl(VI) complexes were found to be quasi-reversibly reduced to U(V) species. The formal redox potentials (E$$^{o}$$, ${it vs}$. ferrocene/ferrocenium) for U(VI)/U(V) couples were determined to be -1.18 V for UO$$_{2}$$(ttfa)$$_{2}$$DMF, -1.18 V for UO$$_{2}$$(btfa)$$_{2}$$DMF, -1.46 V for UO$$_{2}$$ (dbm)$$_{2}$$DMF, -1.46 V for UO$$_{2}$$(trop)$$_{2}$$DMF, and -1.59 V for UO$$_{2}$$(sap)(DMF)$$_{2}$$.

JAEA Reports

Report on the fuel treatment facility operation

Kokusen, Junya; Seki, Masakazu; Abe, Masayuki; Nakazaki, Masato; Kida, Takashi; Umeda, Miki; Kihara, Takehiro; Sugikawa, Susumu

JAERI-Tech 2005-004, 53 Pages, 2005/03

JAERI-Tech-2005-004.pdf:5.92MB

This report presents operating records of dissolution of uranium dioxide and concentration of uranyl nitrate solution and acid removal, which have been performed from 1994 through 2003, for the purpose of feeding 10% and 6% enriched uranyl nitrate solution fuel to Static Experimental Critical Facility(STACY) and Transient Experimental Critical Facility(TRACY) in Nuclear Fuel Safety Engineering Facility(NUCEF).

Journal Articles

Electrochemical redox reactions of uranium(VI) complexes with multidentate ligands in dimethyl sulfoxide

Kim, S.-Y.; Asakura, Toshihide; Morita, Yasuji; Uchiyama, Gunzo*; Ikeda, Yasuhisa*

Radiochimica Acta, 93(2), p.75 - 81, 2005/02

 Times Cited Count:9 Percentile:53.1(Chemistry, Inorganic & Nuclear)

no abstracts in English

Journal Articles

Measurement of temperature effect on low enrichment STACY heterogeneous core

Watanabe, Shoichi; Yamamoto, Toshihiro; Miyoshi, Yoshinori

Transactions of the American Nuclear Society, 91, p.431 - 432, 2004/11

Temperature effect is a main factor which affects the transient characteristics at a criticality accident. A series of reactivity effects due to changes in fuel temperatures were measured for two kinds of STACY heterogeneous lattice configurations. The core was composed of LWR-type fuel rod array and low-enriched uranyl-nitrate-solution concerning the dissolver of the reprocessing facility for LWR spent fuel. The critical solution heights at various solution temperatures were measured. From the change of the critical water height with fuel temperature, the reactivity effect was evaluated by a critical-solution-level worth method. The temperature effect was also calculated by using SRAC and the transport calculation code TWODANT. The experimental value was estimated to be -2.0 cent/$$^{circ}$$C for the case "2.1cm-pitch", and -2.5 cent/$$^{circ}$$C for the case "1.5cm-pitch". The calculated results gave agreement with the experiments within $$sim$$10%.

JAEA Reports

Present status of chemical analysis of uranyl nitrate solution used for the criticality experiments in NUCEF

Haga, Takahisa*; Gunji, Kazuhiko; Fukaya, Hiroyuki; Sonoda, Takashi; Sakazume, Yoshinori; Sakai, Yutaka; Niitsuma, Yasushi; Togashi, Yoshihiro; Miyauchi, Masakatsu; Sato, Takeshi; et al.

JAERI-Tech 2004-005, 54 Pages, 2004/02

JAERI-Tech-2004-005.pdf:2.06MB

Criticality experiments using uranyl nitrate solution fuel are being conducted at STACY (the Static Experiment Critical Facility) and TRACY (the Transient Experiment Critical Facility) in NUCEF (the Nuclear Fuel Cycle Safety Engineering Research Facility). Chemical analyses of the solution have been carried out to take necessary data for criticality experiments, for treatment and control of the fuel, and for safeguards purpose at the analytical laboratory placed in NUCEF. About 300 samples are analyzed annually that provide various kinds of data, such as uranium concentration, isolation acid concentration, uranium isotopic composition, concentration of fission product (FP) nuclides, tri-butyl phosphoric acid (TBP) concentration, impurities in the solution fuel and so on. This report summarizes the analytical methods and quality management of the analysis for uranyl nitrate solution relating to the criticality experiments.

Journal Articles

The Resonance Raman effect of uranyl formate in dimethyl sulfoxide

Soga, Takeshi

Spectrochimica Acta, Part A, 59(11), p.2497 - 2510, 2003/09

no abstracts in English

Journal Articles

Reactivity effect measurement of neutron interaction between two slab cores containing 10% enriched uranyl nitrate solution without neutron isolater

Tonoike, Kotaro; Miyoshi, Yoshinori; Okubo, Kiyoshi

Journal of Nuclear Science and Technology, 40(4), p.238 - 245, 2003/04

 Times Cited Count:2 Percentile:18.9(Nuclear Science & Technology)

The reactivity effect of neutron interaction between two identical units containing low enriched (10% $$^{235}$$ enrichment) uranyl nitrate solution was measured in the STACY. The unit has 350mm of thickness and 690mm of width and distance between those two units was adjustable from 0mm to 1450mm. Condition of the solution was about 290gU/L in uranium concentration, about 0.8N in free nitric acid molarity, 24$$sim$$27$$^{circ}$$C in temperature and about 1.4g/cm$$^{3}$$ in solution density. The reactivity effect was estimated from variation of critical solution level from 495mm to 763mm depending on the core distance. The reactivity effect was also evaluated by the solid angle method and a computational method using the continuous energy Monte Carlo code MCNP-4C and the nuclear data library JENDL3.2. Comparison of those estimations is presented.

JAEA Reports

Cation-cation interaction in neptunyl(V) compounds

Krot, N. N.*; Saeki, Masakatsu

JAERI-Review 2003-005, 37 Pages, 2003/03

JAERI-Review-2003-005.pdf:2.12MB

The original manuscript was prepared by Professor N. N. Krot of Institute of Physical Chemistry, Russian Academy of sciences, in 1997. Saeki tried to translate that into Japanese and to add some new data since 1997. The contents include the whole picture of cation-cation interactions mainly on 5-valence neptunium compounds. Firstly, characteristic structures are summarized for the cation-cation bonding in compounds of neptunium. Secondly, it is introduced how the cation-cation bonding affects physical and chemical properties of the compounds. Then, detection-methods are shown for the cation-cation bonding in the compounds. Besides, the cation-cation interaction are shortly reviewed for compounds of other actinide-ions.

Journal Articles

Critical experiments on 10% enriched uranyl nitrate solution using an 80-cm-diameter cylindrical core

Yamane, Yuichi; Miyoshi, Yoshinori; Watanabe, Shoichi; Yamamoto, Toshihiro

Nuclear Technology, 141(3), p.221 - 232, 2003/03

 Times Cited Count:5 Percentile:36.77(Nuclear Science & Technology)

no abstracts in English

Journal Articles

Kinetic parameter $$beta_{rm eff}/ell$$ measurement on low enriched uranyl nitrate solution with single unit cores (600$$phi$$, 280T, 800$$phi$$) of STACY

Tonoike, Kotaro; Miyoshi, Yoshinori; Kikuchi, Tsukasa*; Yamamoto, Toshihiro

Journal of Nuclear Science and Technology, 39(11), p.1227 - 1236, 2002/11

 Times Cited Count:21 Percentile:77.32(Nuclear Science & Technology)

Kinetic parameter $$beta_{rm eff}/ell$$ of low enriched uranyl nitrate solution was measured by the pulsed neutron source method in the STACY. This measurement was repeated systematically over several uranium concentrations from 193.7 gU/$$ell$$ to 432.1 gU/$$ell$$. Used core tanks were two cylindrical tanks whose diameters are 600 mm and 800 mm and one slab tank which has 280 mm thickness and 700 mm width. In this report, experimental data such as solution conditions, critical solution level for each solution condition, subcritical solution levels where measurements were conducted, measured decay time constants of prompt neutron and extrapolated $$beta_{rm eff}/ell$$ values are described as well as basic principle of the pulsed neutron source method. $$beta_{rm eff}/ell$$ values were evaluated also by computation with the diffusion code CITATION in SRAC and the nuclear data library JENDL 3.2. Both experimental and computational $$beta_{rm eff}/ell$$ values show good agreement.

JAEA Reports

Report of TRACY operation

Aizawa, Eiju; Ogawa, Kazuhiko; Sakuraba, Koichi; Tsukamoto, Michio; Sugawara, Susumu; Takeuchi, Masaki*; Miyauchi, Masakatsu; Yanagisawa, Hiroshi; Ono, Akio

JAERI-Tech 2002-031, 120 Pages, 2002/03

JAERI-Tech-2002-031.pdf:4.32MB

TRACY (Transient Experiment Critical Facility) in NUCEF (Nuclear Safety Research Facility) is the pulse-type critical facility using uranyl nitrate solution which can carry out various supercritical experiments changing reactivity addition up to 3$.TRACY achieved its first criticality on 20th December 1995,and transient operations have been conducted Since1996.This report summarizes the operation data of 176 experiments from the first criticality to FY2000.

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