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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

Study on the mechanism of radiolytic degradation of an extractant for minor actinides separation

Toigawa, Tomohiro; Murayama, Rin*; Kumagai, Yuta; Yamashita, Shinichi*; Suzuki, Hideya; Ban, Yasutoshi; Matsumura, Tatsuro

UTNL-R-0501, p.24 - 25, 2020/12

This report summarizes the results obtained in FY2019 at Electron Linac Facility of University of Tokyo. The radiolysis process of a diglycolamide extractant, which is expected to be used in the separation process of minor actinides (MA), in dodecane and octanol solutions was investigated by pulse radiolysis. As a result, it was suggested that by adding alcohol, the decomposition process of the diglycolamide extractant was different from the decomposition processes in the single solvent of dodecane considered that the decomposition occurred via a radical cation species of the extractant.

JAEA Reports

Critical mass evaluation of minor actinides in aqueous solution; Data for criticality safety assessment of separation process

Morita, Yasuji; Fukushima, Masahiro; Kashima, Takao*; Tsubata, Yasuhiro

JAEA-Data/Code 2020-013, 38 Pages, 2020/09

JAEA-Data-Code-2020-013.pdf:1.94MB

Critical Masses of Cm, Am and the mixture were calculated in metal-water mixtures with water reflector as a basic data for criticality safety assessment of minor actinide separation process. In the mixture of Cm-244 and Cm-245, higher ratio of Cm-245 gives smaller critical mass, but the amount of Cm-245 in the critical mass can be obtained by concentration of Cm-245 in the Cm mixture without depending on the Cm-245 ratio. Critical mass of Cm isotope mixture with 30% Cm-245 was smaller than that of Pu isotope mixture in the practical reprocessing (71% Pu-239 + 17% Pu-240 + 12% Pu-241). When Cm is separated from other element including Am and the solution is concentrated, measure for the critical accident has to be taken. Critical mass of Am-242m is smaller than that of Cm-245, but the ratio of Am-242m in the Am contained in practical spent fuel is small enough, about several percent, and therefore the critical accident by Am does not have to be considered. That by the mixture of Am and Cm does not either.

Journal Articles

Improvement in flow-sheet of extraction chromatography for trivalent minor actinides recovery

Watanabe, So; Senzaki, Tatsuya; Shibata, Atsuhiro; Nomura, Kazunori; Takeuchi, Masayuki; Nakatani, Kiyoharu*; Matsuura, Haruaki*; Horiuchi, Yusuke*; Arai, Tsuyoshi*

Journal of Radioanalytical and Nuclear Chemistry, 322(3), p.1273 - 1277, 2019/12

 Times Cited Count:4 Percentile:40.00(Chemistry, Analytical)

Journal Articles

Characteristics of TPDN/SiO$$_{2}$$-P adsorbent for MA(III) recovery

Kofuji, Hirohide; Watanabe, So; Takeuchi, Masayuki; Suzuki, Hideya; Matsumura, Tatsuro; Shiwaku, Hideaki; Yaita, Tsuyoshi

Progress in Nuclear Science and Technology (Internet), 5, p.61 - 65, 2018/11

Journal Articles

Research and development for accuracy improvement of neutron nuclear data on minor actinides

Harada, Hideo; Iwamoto, Osamu; Iwamoto, Nobuyuki; Kimura, Atsushi; Terada, Kazushi; Nakao, Taro; Nakamura, Shoji; Mizuyama, Kazuhito; Igashira, Masayuki*; Katabuchi, Tatsuya*; et al.

EPJ Web of Conferences, 146, p.11001_1 - 11001_6, 2017/09

 Times Cited Count:2 Percentile:77.79(Nuclear Science & Technology)

Journal Articles

Minor actinides recovery from irradiated fuel for SmART cycle test

Takeuchi, Masayuki; Sano, Yuichi; Watanabe, So; Nakahara, Masaumi; Aihara, Haruka; Kofuji, Hirohide; Koizumi, Tsutomu; Mizuno, Tomoyasu

Proceedings of 2017 International Congress on Advances in Nuclear Power Plants (ICAPP 2017) (CD-ROM), 6 Pages, 2017/04

Journal Articles

Application of FE-SEM to the measurement of U, Pu, Am in the irradiated MA-MOX fuel

Sasaki, Shinji; Tanno, Takashi; Maeda, Koji

Proceedings of 54th Annual Meeting of Hot Laboratories and Remote Handling (HOTLAB 2017) (Internet), 6 Pages, 2017/00

During irradiation in a fast reactor, the microstructure change of the mixed oxide fuels and the changes of element distributions occur because of a radial temperature gradient. Therefore, it is important to study the irradiation behavior of MA-MOX for advancement of fast reactor fuels. In order to make detailed observations of microstructure and elemental analyses of MA-MOX, irradiated MA-MOX specimens were carried out PIE by using a FE-SEM equipped with WDX. Because fuel samples have high radio activities and emit alpha-particles, the instrument was modified. the instrument was installed in a lead shield box and the control unit was separately located outside the box. The microstructure changes were observed in irradiated MA-MOX specimen. The characteristic X-rays peaks were detected successfully. By measuring the intensities of characteristic X-rays, it was tried quantitative analysis of U, Pu, Am along radial direction of irradiated specimen.

Journal Articles

Flow-sheet study of MA recovery by extraction chromatography for SmART cycle project

Watanabe, So; Nomura, Kazunori; Kitawaki, Shinichi; Shibata, Atsuhiro; Kofuji, Hirohide; Sano, Yuichi; Takeuchi, Masayuki

Procedia Chemistry, 21, p.101 - 108, 2016/12

BB2015-3215.pdf:0.34MB

 Times Cited Count:14 Percentile:99.14(Chemistry, Inorganic & Nuclear)

Journal Articles

Development of nitride fuel cycle technology for transmutation of minor actinides

Hayashi, Hirokazu; Nishi, Tsuyoshi*; Sato, Takumi; Kurata, Masaki

Proceedings of 21st International Conference & Exhibition; Nuclear Fuel Cycle for a Low-Carbon Future (GLOBAL 2015) (USB Flash Drive), p.1811 - 1817, 2015/09

Transmutation of long-lived radioactive nuclides including minor actinides (MA: Np, Am, Cm) has been studied in Japan Atomic Energy Agency (JAEA). Accelerator-driven system (ADS) is regarded as one of the powerful tools for transmutation of MA under the double strata fuel cycle concept. Uranium-free nitride fuel was chosen as the first candidate fuel for MA transmutation using ADS. To improve the transmutation ratio of MA, reprocessing of spent fuel and reusing MA recovered from the spent fuels is necessary. Our target is to transmute 99% of MA arisen from commercial power reactor fuel cycle, with which the period until the radiotoxicity drops below that of natural uranium can be shorten from about 5000 years to about 300 years. A pyrochemical process has been proposed as the first candidate for reprocessing of the spent nitride fuel. This paper overviews the current status of the nitride fuel cycle technology. Our recent study on fuel fabrication, fuel property measurements, reprocessing of spent fuel, development of the property database of MA nitride fuel, and fuel behavior simulation code are introduced. Our research and development (R&D) plan based on the roadmap of the development is also introduced.

Journal Articles

Extraction separation of Am(III) and Eu(III) with TPEN isomers and decanoic acid

Matsumura, Tatsuro; Takeshita, Kenji*

ACS Symposium Series, 933, p.261 - 273, 2006/07

Three TPEN isomers with different positon of nitrogen donor in pyridyl groups, t2pen, t3pen and t4pen, were synthesized and the extraction separation of Am(III) and Eu(III) with these ligands and a fatty acid, decanoic acid, was investigated. All isomers were similar in the complexation in the aqueous phase, such as the protonation and the formation of metal complex, however, they showed different extraction behavior of Am and Eu. The synergistic extraction effect for Am was observed for t2pen and the high separation factor about 100 was measured, when 1:2. The value is comparable to that for the extraction system with a famous nitrogen-donor extractant, BTP. On the other hand, the extractability of other isomers was very low and no separation of Am and Eu was observed. Only t2pen, in which nitrogen donor in pyridyl groups is positioned in the vicinity of the skeletal structure (N-C-C-N structure) of ligand, is available for the extraction separation of Am.

JAEA Reports

Research and development on partitioning in JAERI; Review of the research activities until the development of 4-group partitioning process

Morita, Yasuji; Kubota, Masumitsu*

JAERI-Review 2005-041, 35 Pages, 2005/09

JAERI-Review-2005-041.pdf:2.24MB

Research and development on Partitioning in JAERI are reviewed in the present report from the beginning to the development of the 4-Group Partitioning Process and its test with real high-level liquid waste (HLLW). In the 3-Group Partitioning Process established in around 1980, elements in HLLW are separated into 3 groups of transuranium element group, Sr-Cs group and the other element group. The 4-Group Partitioning Process subsequently developed contains the separation of Tc-platinum group metals additionally. The process was tested to demonstrate its performance with real concentrated HLLW. Until then, various separation methods for various elements were studied and selection and optimization of the separation methods were carried out to establish the process. Review of the experience, findings and results is very important and valuable for future study on partitioning. The present report is prepared from this point of view.

Journal Articles

Selective separation of Am(III) from Ln(III) with a novel synergistic extraction system, N,N,N',N'-tetrakis(2-methylpyridyl)ethylenediamine (TPEN) and carboxylic acid in 1-octanol

Mirvaliev, R.*; Watanabe, Masayuki; Matsumura, Tatsuro; Tachimori, Shoichi*; Takeshita, Kenji*

Journal of Nuclear Science and Technology, 41(11), p.1122 - 1124, 2004/11

 Times Cited Count:21 Percentile:77.73(Nuclear Science & Technology)

Transmutation is a technology aimed to reduce HLW from reprocessing process. Minor actinides in the HLW will be converted to short-lived nuclides. However, lanthanides in HLW adversely affects on the efficiency of the transmutation. It is well known that separating An(III) and Ln(III) is very difficult because of their similarity of chemical properties. Therefore, the separation is one of the essential subjects to establish the transmutation technology. Considerable efforts have been devoted to the development of new extractants for the separation. N,N,N',N'-tetrakis(2-methylpyridyl)ethylenediamine (TPEN) demonstrates 100-fold preference for Am(III) over Ln(III) between stability constants with the ions in the aqueous phase. We have reported that Am(III) was selectively extracted from the aqueous phase containing Ln(III) by TPEN in nitrobenzene system and synergistic system with TPEN and D2EHPA in octanol. This work presents our recent results that Am(III) is separated from Eu(III) by a synergistic extraction system with TPEN and decanoic acid diluted with 1-octanol.

Journal Articles

Fabrication of nitride fuels for transmutation of minor actinides

Minato, Kazuo; Akabori, Mitsuo; Takano, Masahide; Arai, Yasuo; Nakajima, Kunihisa; Ito, Akinori; Ogawa, Toru

Journal of Nuclear Materials, 320(1-2), p.18 - 24, 2003/09

 Times Cited Count:53 Percentile:94.49(Materials Science, Multidisciplinary)

In the Japan Atomic Energy Research Institute, the concept of the transmutation of minor actinides (MA: Np, Am and Cm) with accelerator-driven systems is being studied. The MA nitride fuel has been chosen as a candidate because of the possible mutual solubility among the actinide mononitrides and excellent thermal properties besides supporting hard neutron spectrum. MA nitrides of AmN, (Am,Y)N, (Am,Zr)N and (Cm0.4Pu0.6)N were prepared from the oxides by the carbothermic reduction method. The prepared MA nitrides were examined by X-ray diffraction and the contents of impurities of oxygen and carbon were measured. The fabrication conditions for MA nitrides were improved so as to reduce the impurity contents. For an irradiation test of U-free nitride fuels, pellets of (Pu,Zr)N and PuN+TiN were prepared and a He-bonded fuel pin was fabricated. The irradiation test started in May 2002 and will go on for two years in the Japan Materials Testing Reactor.

Journal Articles

Research and development on nuclear transmutation, B; Transmutation fuel and reprocessing

Minato, Kazuo; Arai, Yasuo

Genshikaku Kenkyu, 47(6), p.31 - 38, 2003/06

no abstracts in English

Journal Articles

Validation of minor actinide cross sections by studying samples irradiated for 492 days at the dounreay prototype fast reactor, 1; Radiochemical analysis

Shinohara, Nobuo; Kono, Nobuaki; Nakahara, Yoshinori; Tsujimoto, Kazufumi; Sakurai, Takeshi; Mukaiyama, Takehiko*; Raman, S.*

Nuclear Science and Engineering, 144(2), p.115 - 128, 2003/06

 Times Cited Count:12 Percentile:62.06(Nuclear Science & Technology)

no abstracts in English

Journal Articles

Validation of minor actinide cross sections by studying samples irradiated for 492 days at the dounreay prototype fast reactor, 1; Radiochemical analysis

Shinohara, Nobuo; Kono, Nobuaki; Nakahara, Yoshinori; Tsujimoto, Kazufumi; Sakurai, Takeshi; Mukaiyama, Takehiko*; Raman, S.*

Nuclear Science and Engineering, 144(2), p.115 - 128, 2003/06

no abstracts in English

Journal Articles

Validation of minor actinide cross sections by studying samples irradiated for 492 days at the dounreay prototype fast reactor, 2; Burnup calculations

Tsujimoto, Kazufumi; Kono, Nobuaki; Shinohara, Nobuo; Sakurai, Takeshi; Nakahara, Yoshinori; Mukaiyama, Takehiko; Raman, S.*

Nuclear Science and Engineering, 144(2), p.129 - 141, 2003/06

To evaluate neutron cross-section data of minor actinides, separated actinide samples and dosimetry samples were irradiated at the Dounreay Prototype Fast Reactor for 492 effective full power days. Based on the burnup calculations of major actinide and dosimetry samples, the neutron flux distribution and the flux level were adjusted at the locations where minor actinide samples were irradiated. The burnup calculations were carried out for minor actinides using the determined flux distribution and flux level. This paper discusses the burnup calculations and the validation of minor actinide cross-section data in evaluated nuclear data libraries. We find that we can obtain reliable FIMA (fission per initial metallic atom) values by using the $$^{148}$$Nd method except that the uncertainties in the FIMA values are large for $$^{234}$$U, $$^{238}$$Pu, Am isotopes, and Cm isotopes because the $$^{148}$$Nd yields are known poorly for these isotopes and are probably overestimated. For these isotopes, measurements to improve the fission-yield data are needed. We also find that, in general, the JENDL-3.2 nuclear data for the minor actinides are adequate for the conceptual design study of transmutation systems. But, there are some nuclides (especially $$^{238}$$Pu and $$^{242}$$Pu) for which new measurements are needed particulary if the minor actinides constitute a major part of the nuclear fuel.

Journal Articles

Validation of minor actinide cross sections by studying samples irradiated for 492 days at the dounreay prototype fast reactor, 2; Burnup calculations

Tsujimoto, Kazufumi; Kono, Nobuaki; Shinohara, Nobuo; Sakurai, Takeshi; Nakahara, Yoshinori; Mukaiyama, Takehiko*; Raman, S.*

Nuclear Science and Engineering, 144(2), p.129 - 141, 2003/06

 Times Cited Count:11 Percentile:59.22(Nuclear Science & Technology)

no abstracts in English

Journal Articles

Preparation of novel silica-based R-BTP extraction-resins and their application to trivalent actinides and lanthanides separation

Wei, Y.*; Hoshi, Harutaka*; Kumagai, Mikio*; Asakura, Toshihide; Uchiyama, Gunzo*

Journal of Nuclear Science and Technology, 39(Suppl.3), p.761 - 764, 2002/11

To separate long-lived minor actinides and specific fission products such as Zr and Mo from nitrate acidic high-level liquid waste, we studied an advanced partitioning process by extraction chromatography using minimal organic solvent and compact equipment. In this work, we synthesized several new type of nitrogen donor ligands, 2,6-bi-(5,6-dialkyl-1,2,4-triazine-3-yl)-pyridine (R-BTP) with different alkyl groups and prepared novel silica-based extraction-resins by impregnating these ligands into the SiO$$_{2}$$-P support with a diameter of 50 $$mu$$m. The adsorption performance of $$^{243}$$Am and Ln (III) from nitrate solution was investigated. It was found that the adsorption behavior depends strongly on the alkyl group in R-BTP. ${it n}$Bu-BTP/SiO$$_{2}$$-P and ${it n}$Hex-BTP/SiO$$_{2}$$-P showed high absorbability and selectivity for Am (III) over Ln (III). The separation factor is about 10$$^{4}$$ for Am/Ce and near 10$$^{2}$$ for Am/Eu-Gd, respectively. Effective Am (III) separation form Ln (III) by extraction chromatography using R-BTP/SiO$$_{2}$$-P extraction-resins is expected.

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