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Journal Articles

Kinetic and thermodynamic controls on CsI-Mo gas-phase reactions under varying oxygen potentials

Shiotsu, Hiroyuki

Progress in Nuclear Energy, 195, p.106300_1 - 106300_11, 2026/05

 Times Cited Count:0 Percentile:0.00(Nuclear Science & Technology)

Journal Articles

DECOVALEX-2023: An International collaboration for advancing the understanding and modeling of coupled thermo-hydro-mechanical-chemical (THMC) processes in geological systems

Birkholzer, J. T.*; Graupner, B. J.*; Harrington, J.*; Jayne, R.*; Kolditz, O.*; Kuhlman, K. L.*; LaForce, T.*; Leone, R. C.*; Mariner, P. E.*; McDermott, C.*; et al.

Geomechanics for Energy and the Environment, 42, p.100685_1 - 100685_17, 2025/06

 Times Cited Count:7 Percentile:87.84(Energy & Fuels)

Journal Articles

Development of corrosion-stable dual-Si-layered membranes for hydrogen production via thermochemical iodine-sulfur process

Myagmarjav, O.; Tanaka, Nobuyuki; Noguchi, Hiroki; Kamiji, Yu; Ono, Masato; Nomura, Mikihiro*; Takegami, Hiroaki

Progress in Nuclear Science and Technology (Internet), 7, p.235 - 242, 2025/03

JAEA Reports

Trial analysis of chemical behavior in high-level radioactive liquid waste tank at accident of evaporation to dryness by boiling of reprocessing plant

Yoshida, Kazuo; Hiyama, Mina*; Tamaki, Hitoshi

JAEA-Research 2024-007, 24 Pages, 2024/08

JAEA-Research-2024-007.pdf:2.1MB

An accident of evaporation to dryness by boiling of high-level radioactive liquid waste (HLLW) is postulated as one of the severe accidents caused by the loss of cooling function at a fuel reprocessing plant. In this case, volatile radioactive materials, such as ruthenium (Ru) are released from the tanks with water and nitric-acid mixed vapor into the atmosphere. Accurate quantitative estimation of released Ru is one of the important issues for risk assessment of those facilities. It has been observed experimentally that volatility of RuO$$_{4}$$ is suppressed by HNO$$_{2}$$ generated by HNO$$_{3}$$ radiolysis. The analysis of chemical reactions of NO$$_{x}$$ including HNO$$_{3}$$ and HNO$$_{2}$$ in the waste tank is essential to simulate of these phenomena. To resolve this issue, an analytical approach has been attempted to couple dynamically two computer codes SHAWED and SCHERN. The simulation of boiling behavior in the tank is conducted with SHAWED. SCHERN simulates chemical behaviors of HNO$$_{3}$$, HNO$$_{2}$$ and NO$$_{x}$$ in the tank. A programmatic coupling algorithm and a trial simulation of the accident are presented in this report.

JAEA Reports

Development of analytical approach of source term for accident of evaporation to dryness by boiling of reprocessed high level liquid waste

Yoshida, Kazuo; Tamaki, Hitoshi; Hiyama, Mina*

JAEA-Research 2023-001, 26 Pages, 2023/05

JAEA-Research-2023-001.pdf:1.61MB

An accident of evaporation to dryness by boiling of high-level radioactive liquid waste (HLLW) is postulated as one of the severe accidents caused by the loss of cooling function at a fuel reprocessing plant. In this case, volatile radioactive materials, such as ruthenium (Ru) are released from the tanks with water and nitric-acid mixed vapor into the atmosphere. Accurate quantitative estimation of released Ru is one of the important issues for risk assessment of those facilities. To resolve this issue, an analytical approach has been developed using computer simulation programs to assess the radioactive source term from those facilities. The proposed approach consists analyses with three computer programs. At first, the simulation of boiling behavior in the HLLW tank is conducted with SHAWED code. Next step, the thermal-hydraulic behavior in the facility building is simulated with MELCOR code based on the results at the first step simulation such as flowed out mixed steam flow rate, temperature and volatilized Ru from the tank. The final analysis step is carried out for estimating amount of released radioactive materials with SCHERN computer code which simulates chemical behaviors of nitric acid, nitrogen oxide and Ru based on the condition also simulated MELCOR. Series of sample simulations of the accident at a hypothetical typical facility are presented with the data transfer between those codes in this report.

JAEA Reports

Analysis of risk reduction effect of supposed steam condenser implementation as accident measure for accident of evaporation to dryness by boiling of reprocessed high level liquid waste

Yoshida, Kazuo; Tamaki, Hitoshi; Hiyama, Mina*

JAEA-Research 2021-013, 20 Pages, 2022/01

JAEA-Research-2021-013.pdf:2.35MB

An accident of evaporation to dryness by boiling of high level liquid waste (HLLW) is postulated as one of the severe accidents caused by the loss of cooling function at a fuel reprocessing plant. In this case, volatile radioactive materials, such as ruthenium (Ru) are released from the tanks with water and nitric-acid mixed vapor into atmosphere. An idea has been proposed to implement a steam condenser as an accident countermeasure. This measure is expected to prevent nitric acid steam diffusing in facility building and to increase gaseous Ru trapping ratio into condensed water. A simulation study has been carried out with a hypothetical typical facility building to analyze the efficiency of steam condenser. In this study, SCHERN computer code simulates chemical behaviors of Ru in nitrogen oxide, nitric acid and water mixed vapor based on the conditions obtained from simulation with thermal-hydraulic computer code MELCOR. The effectiveness of steam condenser has been analyzed quantitively in preventing mixed vapor diffusion and gaseous Ru trapping effect. Some issues to be solved in analytical model has been also clarified in this study.

Journal Articles

Development of a membrane reactor with a closed-end silica membrane for nuclear-heated hydrogen production

Myagmarjav, O.; Tanaka, Nobuyuki; Nomura, Mikihiro*; Noguchi, Hiroki; Imai, Yoshiyuki; Kamiji, Yu; Kubo, Shinji; Takegami, Hiroaki

Progress in Nuclear Energy, 137, p.103772_1 - 103772_7, 2021/07

 Times Cited Count:9 Percentile:61.47(Nuclear Science & Technology)

JAEA Reports

JAEA-TDB-RN in 2020; Update of JAEA's thermodynamic database for solubility and speciation of radionuclides for performance assessment of geological disposal of high-level and TRU wastes

Kitamura, Akira

JAEA-Data/Code 2020-020, 164 Pages, 2021/03

JAEA-Data-Code-2020-020.pdf:3.11MB
JAEA-Data-Code-2020-020-appendix(DVD-ROM).zip:0.56MB

Part of JAEA's Thermodynamic Database (JAEA-TDB) for solubility and speciation of radionuclides (JAEA-TDB-RN) for performance assessment of geological disposal of high-level radioactive and TRU wastes has been updated with subsuming the database for geochemical calculations (JAEA-TDB-GC). This report has focused to update JAEA-TDB-RN after selecting change in standard Gibbs free energy of formation ($$Delta_{rm r}$$$$G^{circ}_{rm m}$$), change in standard enthalpy change of formation ($$Delta$$$$H$$$$^{circ}$$$$_{rm m}$$), standard molar entropy ($$S^{circ}$$$$_{rm m}$$) and, heat capacity ($$C^{circ}_{rm p}$$), change in standard Gibbs free energy of reaction ($$Delta_{rm r}G^{circ}$$$$_{rm m}$$), change in standard enthalpy change of reaction ($$Delta$$$$_{rm r}$$$$H$$$$^{circ}$$$$_{rm m}$$) and standard entropy change of reaction ($$Delta_{rm r}S^{circ}_{rm m}$$) as well as logarithm of equilibrium constant (log$$_{10}$$$$K^{circ}$$) at standard state. The extent of selection of these thermodynamic data enables to evaluate solubility and speciation of radionuclides at temperatures other than 298.15 K. Furthermore, the latest thermodynamic data for iron which have been critically reviewed, selected and compiled by the Nuclear Energy Agency within Organisation for Economic Co-operation and Development (OECD/NEA) have been accepted. Most of previously selected log$$_{10}$$$$K^{circ}$$ have been refined to confirm internal consistency with JAEA-TDB-GC. Text files of the updated JAEA-TDB have been provided for geochemical calculation programs of PHREEQC and Geochemist's Workbench.

Journal Articles

Investigation of high-temperature chemical interaction of calcium silicate insulation and cesium hydroxide

Rizaal, M.; Nakajima, Kunihisa; Saito, Takumi*; Osaka, Masahiko; Okamoto, Koji*

Journal of Nuclear Science and Technology, 57(9), p.1062 - 1073, 2020/09

 Times Cited Count:10 Percentile:61.75(Nuclear Science & Technology)

The interaction of cesium hydroxide and a calcium silicate insulation material was experimentally investigated at high temperature conditions. A thermogravimetry equipped with differential thermal analysis was used to analyze thermal events in the samples of mixed calcium silicate and cesium hydroxide under Ar-5%H$$_{2}$$ and Ar-4%H$$_{2}$$-20%H$$_{2}$$0 with maximum temperature of 1100$$^{circ}$$C. Prior being mixed with cesium hydroxide, a part of calcium silicate was pretreated at high temperature to evaluate the effect of possible structural changes of this material due to a preceding thermal history and also the sake of thermodynamic evaluation to those available ones. Based upon the initial condition (preliminary heat treatment) of calcium silicate, it was found that if the original material consisted of xonotlite (Ca$$_{6}$$Si$$_{6}$$0$$_{17}$$(0H)$$_{2}$$), the endothermic reaction with cesium hydroxide occurred over the temperature range 575-730$$^{circ}$$C meanwhile if the crystal phase of original material was changed to wollastonite (CaSi0$$_{3}$$), the interaction occurred over temperature range 700-1100$$^{circ}$$C. Furthermore, the X-ray diffraction analyses have indicated on both type of pretreated calsils that regardless of Ar-5%H$$_{2}$$ and Ar-4%H$$_{2}$$-20%H$$_{2}$$0 atmosphere, cesium aluminum silicate, CsAlSi0$$_{4}$$ was formed with aluminum in the samples as an impurity or adduct.

Journal Articles

Chemical forms of uranium evaluated by thermodynamic calculation associated with distribution of core materials in the damaged reactor pressure vessel

Ikeuchi, Hirotomo; Yano, Kimihiko; Washiya, Tadahiro

Journal of Nuclear Science and Technology, 57(6), p.704 - 718, 2020/06

 Times Cited Count:8 Percentile:53.05(Nuclear Science & Technology)

To suggest efficient process of the fuel debris treatment after the retrieval from the Fukushima Daiichi Nuclear Power Plant (1F), thorough investigation is indispensable on potential source of U in the fuel debris. Estimation on the fuel debris accumulated in the reactor pressure vessel is specifically important due to its limited accessibility. The present study aims to estimate the chemical forms of U in the in-vessel fuel debris, especially in the minor phases such as metallic phases, by performing the thermodynamic calculation considering the material relocation and changing environment during the accident progression in the 1F Unit 2. Input conditions for the thermodynamic calculation such as composition, temperature, and oxygen amount were assumed mainly based on the results of severe accident analysis. The chemical form of U varied depending on the local amount of Fe and O. In regions of low steel content, the U-containing metallic phase was dominated by $$alpha$$-(Zr,U)(O), while regions of high steel content were dominated by Fe$$_{2}$$(Zr,U) (Laves phase). A few percent of U was transferred to the metallic phases under reducing conditions, raising challenging issues on the chemical removal of nuclear material from fuel debris.

Journal Articles

Comparison of experimental and simulation results on catalytic HI decomposition in a silica-based ceramic membrane reactor

Myagmarjav, O.; Tanaka, Nobuyuki; Nomura, Mikihiro*; Kubo, Shinji

International Journal of Hydrogen Energy, 44(59), p.30832 - 30839, 2019/11

 Times Cited Count:14 Percentile:33.06(Chemistry, Physical)

Journal Articles

The Analytical study of inventories and physicochemical configuration of spallation products produced in Lead-Bismuth Eutectic of Accelerator Driven System

Miyahara, Shinya*; Ohdaira, Naoya*; Arita, Yuji*; Maekawa, Fujio; Matsuda, Hiroki; Sasa, Toshinobu; Meigo, Shinichiro

Nuclear Engineering and Design, 352, p.110192_1 - 110192_8, 2019/10

 Times Cited Count:6 Percentile:42.01(Nuclear Science & Technology)

Lead-Bismuth Eutectic (LBE) is used as a spallation neutron target and coolant materials of Accelerator Driven System (ADS), and many kinds of elements are produced as spallation products. It is important to evaluate the release and transport behavior of the spallation products in the LBE. The inventories and the physicochemical composition of the spallation products produced in LBE have been investigated for an LBE loop in the ADS Target Test Facility (TEF-T) in J-PARC. The inventories of the spallation products in the LBE were estimated using the PHITS code. The physicochemical composition of the spallation products in the LBE was calculated using the Thermo-Calc code under the conditions of the operation temperatures of LBE from 350$$^{circ}$$C to 500$$^{circ}$$C and the oxygen concentrations in LBE from 10 ppb to 1 ppm. The calculation showed that the 5 elements of Rb, Tl, Tc, Os, Ir, Pt, Au and Hg were soluble in LBE under the all given conditions and any kinds of compound were not formed in LBE. It was suggested that the oxides of Ce, Sr, Zr and Y were stable as CeO$$_{2}$$, SrO, ZrO$$_{2}$$ and Y$$_{2}$$O$$_{3}$$ in the LBE.

Journal Articles

Research and development on membrane IS process for hydrogen production using solar heat

Myagmarjav, O.; Iwatsuki, Jin; Tanaka, Nobuyuki; Noguchi, Hiroki; Kamiji, Yu; Ioka, Ikuo; Kubo, Shinji; Nomura, Mikihiro*; Yamaki, Tetsuya*; Sawada, Shinichi*; et al.

International Journal of Hydrogen Energy, 44(35), p.19141 - 19152, 2019/07

 Times Cited Count:20 Percentile:45.27(Chemistry, Physical)

JAEA Reports

Update of JAEA-TDB; Update of thermodynamic data for zirconium and those for isosaccahrinate, tentative selection of thermodynamic data for ternary M$$^{2+}$$-UO$$_{2}$$$$^{2+}$$-CO$$_{3}$$$$^{2-}$$ system and integration with JAEA's thermodynamic database for geochemical calculations

Kitamura, Akira

JAEA-Data/Code 2018-018, 103 Pages, 2019/03

JAEA-Data-Code-2018-018.pdf:5.66MB
JAEA-Data-Code-2018-018-appendix1(DVD-ROM).zip:0.14MB
JAEA-Data-Code-2018-018-appendix2(DVD-ROM).zip:0.15MB
JAEA-Data-Code-2018-018-appendix3(DVD-ROM).zip:0.19MB

The latest available thermodynamic data were critically reviewed and the selected values were included into the JAEA-TDB for performance assessment of geological disposal of high-level radioactive and TRU wastes. This critical review specifically addressed thermodynamic data for (1) a zirconium-hydroxide system through comparison of thermodynamic data selected by the Nuclear Energy Agency within the Organisation for Economic Co-operation and Development (OECD/NEA), (2) complexation of metal ions with isosaccharinic acid based on the latest review papers. Furthermore, the author performed (3) tentative selection of thermodynamic data on ternary complexes among alkaline-earth metal, uranyl and carbonate ions, and (4) integration with the latest version of JAEA's thermodynamic database for geochemical calculations. The internal consistency of the selected data was checked by the author. Text files of the updated and integrated thermodynamic database have been prepared for geochemical calculation programs of PHREEQC and Geochemist's Workbench.

Journal Articles

R&D status in thermochemical water-splitting hydrogen production iodine-sulfur process at JAEA

Noguchi, Hiroki; Takegami, Hiroaki; Kasahara, Seiji; Tanaka, Nobuyuki; Kamiji, Yu; Iwatsuki, Jin; Aita, Hideki; Kubo, Shinji

Energy Procedia, 131, p.113 - 118, 2017/12

 Times Cited Count:25 Percentile:99.62(Energy & Fuels)

The IS process is the most deeply investigated thermochemical water-splitting hydrogen production cycle. It is in a process engineering stage in JAEA to use industrial materials for components. Important engineering tasks are verification of integrity of the total process and stability of hydrogen production in harsh environment. A test facility using corrosion-resistant materials was constructed. The hydrogen production ability was 100 L/h. Operation tests of each section were conducted to confirm basic functions of reactors and separators, etc. Then, a trial operation for integration of the sections was successfully conducted to produce hydrogen of about 10 L/h for 8 hours.

Journal Articles

Preparation of an H$$_{2}$$-permselective silica membrane for the separation of H$$_{2}$$ from the hydrogen iodide decomposition reaction in the iodine-sulfur process

Myagmarjav, O.; Ikeda, Ayumi*; Tanaka, Nobuyuki; Kubo, Shinji; Nomura, Mikihiro*

International Journal of Hydrogen Energy, 42(9), p.6012 - 6023, 2017/03

 Times Cited Count:24 Percentile:49.96(Chemistry, Physical)

Journal Articles

IS process hydrogen production test for components and system made of industrial structural material, 1; Bunsen and HI concentration section

Tanaka, Nobuyuki; Takegami, Hiroaki; Noguchi, Hiroki; Kamiji, Yu; Iwatsuki, Jin; Aita, Hideki; Kasahara, Seiji; Kubo, Shinji

Proceedings of 8th International Topical Meeting on High Temperature Reactor Technology (HTR 2016) (CD-ROM), p.1022 - 1028, 2016/11

Japan Atomic Energy Agency (JAEA) has manufactured 100 NL/h-H$$_2$$-scale hydrogen test apparatus. In advance to conduct the continuous operation, we investigated performance of the components in each section of the IS process. In this paper, the results of test of Bunsen and HI concentration sections was shown. In Bunsen reaction, section, we confirmed that outlet gas flow rate included no SO$$_{2}$$ gas, indicating that all the feed SO$$_{2}$$ gas was absorbed to the solution in the Bunsen reactor for the Bunsen reaction. On the basis of these results, we evaluated that Bunsen reactor was workable. In HI concentration section, HI concentration was conducted by EED stack. As a result, it can concentrate HI in HIx solution as theoretically predicted on the basis of the previous paper. Based on the results added to that shown in Series II, we have conducted a trial continuous operation and succeeded it for 8 hours.

Journal Articles

IS process hydrogen production test for components and system made of industrial structural material, 2; H$$_{2}$$SO$$_{4}$$ decomposition, HI distillation, and HI decomposition section

Noguchi, Hiroki; Takegami, Hiroaki; Kamiji, Yu; Tanaka, Nobuyuki; Iwatsuki, Jin; Kasahara, Seiji; Kubo, Shinji

Proceedings of 8th International Topical Meeting on High Temperature Reactor Technology (HTR 2016) (CD-ROM), p.1029 - 1038, 2016/11

JAEA has been conducting R&D on the IS process for nuclear-powered hydrogen production. We have constructed a 100 NL/h-H$$_2$$-scale test apparatus made of industrial materials. At first, we investigated performance of components in this apparatus. In this paper, the test results of H$$_2$$SO$$_4$$ decomposition, HI distillation, and HI decomposition were shown. In the H$$_2$$SO$$_4$$ section, O$$_2$$ production rate is proportional to H$$_2$$SO$$_4$$ feed rate and SO$$_3$$ decomposition ratio was estimated about 80%. In HI distillation section, we confirmed to acquire a concentrated HI solution over azeotropic HI composition in the condenser. In HI decomposition section, H$$_2$$ could be produced stably by HI decomposer and decomposition ratio was about 18%. The H$$_2$$SO$$_4$$ decomposer, the HI distillation column, and the HI decomposer were workable. Based on the results added to that shown in Series I, we conducted a trial continuous operation and succeeded it for 8 hours.

Journal Articles

Flowsheet study of the thermochemical water-splitting IS process for effective hydrogen production

Kasahara, Seiji; Kubo, Shinji; Hino, Ryutaro; Onuki, Kaoru; Nomura, Mikihiro*; Nakao, Shinichi*

Proceedings of AIChE 2005 Spring National Meeting (CD-ROM), 8 Pages, 2005/04

Japan Atomic Energy Research Institute (JAERI) has been conducting the research and development on the thermochemical water-splitting IS process for effective hydrogen production using nuclear heat of close to 1000 $$^{circ}$$C that can be supplied from High Temperature Gas-cooled Reactor (HTGR). The activity covers the studies on the process control for the continuous hydrogen production, the process improvements in the HI decomposition procedure and the preliminary screening of corrosion resistant materials of construction. Present status of the study is presented, especially, focusing on the process flowsheeting study concerning the application of membrane process for the HI processing.

Journal Articles

A Pilot test plan of the thermochemical water-splitting iodine-sulfur process

Kubo, Shinji; Kasahara, Seiji; Okuda, Hiroyuki; Terada, Atsuhiko; Tanaka, Nobuyuki; Inaba, Yoshitomo; Ohashi, Hirofumi; Inagaki, Yoshiyuki; Onuki, Kaoru; Hino, Ryutaro

Nuclear Engineering and Design, 233(1-3), p.355 - 362, 2004/10

 Times Cited Count:65 Percentile:95.48(Nuclear Science & Technology)

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