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JAEA Reports

Strategic roadmap for back-end technology development

Nakazawa, Osamu; Takiya, Hiroaki; Murakami, Masashi; Donomae, Yasushi; Meguro, Yoshihiro

JAEA-Review 2023-012, 6 Pages, 2023/08

JAEA-Review-2023-012.pdf:0.93MB

The selection of back-end technology development issues to be prioritized and their schedule of the Japan Atomic Energy Agency (JAEA) have been put together as the "Strategic Roadmap for Back-end Technology Development." The results of questionnaires on development technologies (seeds) and technical issues (needs) within JAEA conducted in FY2022 were reflected in the selection. The issues were extracted from among those that match the seeds and needs, from the perspective of early implementation in the work front and the perspective of common issues, and nine themes were selected. We will build a cross-organizational implementation framework within JAEA and aim to implement the development results in the work front as well as social implementation.

Journal Articles

Fundamental research of X-ray absorption imaging for elemental identification using a secondary target

Nakae, Masanori*; Matsuyama, Tsugufumi*; Murakami, Masashi; Yoshida, Yukihiko; Machida, Masahiko; Tsuji, Koichi*

Advances in X-Ray Chemical Analysis, Japan, 54, p.89 - 99, 2023/03

Fundamental research on X-ray absorption imaging for elemental identification was studied. A secondary target was applied to obtain X-ray absorption images above and below the X-ray absorption edge of the target element. X-rays from an X-ray tube were irradiated to the secondary target, where the characteristic X-rays were emitted that were irradiated to the sample. X-ray absorption images were acquired with an exposure time of a few seconds with an X-ray camera. In this technique, it is difficult to change the energy of X-rays as we want, however we can apply this technique for imaging the specific element. Metal foil sample composed of Al, Cu, and Ni was analyzed. To obtain an X-ray elemental image of Ni, two X-ray absorption images were taken using the X-rays above and below the Ni K-edge. X-rays of Cu K$$alpha$$ and Zn K$$alpha$$ were prepared by using Cu and Zn plates as the secondary target. Finally, the Ni elemental image was obtained by subtracting two images. Furthermore, the X-ray camera had a function of setting critical energies for imaging, thus it was demonstrated that an X-ray elemental image of Ni was obtained using a single secondary target without changing the secondary target.

Journal Articles

Spectrum prediction in X-ray fluorescence analysis using Bayesian estimation

Matsuyama, Tsugufumi*; Nakae, Masanori*; Murakami, Masashi; Yoshida, Yukihiko; Machida, Masahiko; Tsuji, Koichi*

Spectrochimica Acta, Part B, 199, p.106593_1 - 106593_6, 2023/01

 Times Cited Count:2 Percentile:45.92(Spectroscopy)

JAEA Reports

Common evaluation procedure radioactivity concentration by theoretical calculation for radioactive waste generated from the decommissioning of research reactors

Okada, Shota; Murakami, Masashi; Kochiyama, Mami; Izumo, Sari; Sakai, Akihiro

JAEA-Testing 2022-002, 66 Pages, 2022/08

JAEA-Testing-2022-002.pdf:2.46MB

Japan Atomic Energy Agency is an implementing organization of burial disposal for low-level radioactive waste generated from research, industrial and medical facilities in Japan. Radioactivity concentrations of the waste are essential information for design of the disposal facility and for licensing process. A lot of the waste subjected to the burial disposal is arising from dismantling of nuclear facilities. Radioactive Wastes Disposal enter has therefore discussed a procedure to evaluate the radioactivity concentrations by theoretical calculation for waste arising from the dismantling of the research reactors facilities and summarized the common procedure. The procedure includes evaluation of radioactive inventory by activation calculation, validation of the calculation results, and determination of the disposal classification as well as organization of the data on total radioactivity and maximum radioactivity concentration for each classification. For the evaluation of radioactive inventory, neutron flux and energy spectra are calculated at each region in the reactor facility using two- or three-dimensional neutron transport code. The activation calculation is then conducted for 140 nuclides using the results of neutron transport calculation and an activation calculation code. The recommended codes in this report for neutron transport calculation are two-dimensional discrete ordinate code DORT, three-dimensional discrete ordinate code TORT, or Monte Carlo codes MCNP and PHITS, and for activation calculation is ORIGEN-S. Other recommendation of cross-section libraries and calculation conditions are also indicated in this report. In the course of the establishment of the procedure, Radioactive Wastes Disposal Center has discussed the commonly available procedure at meetings. It has periodically held to exchange information with external operators which have research reactor facilities. The procedure will properly be reviewed and be revised by reflecting future situ

JAEA Reports

Survey on the planning process for waste characterization with statistical methods; Data quality objectives process

Murakami, Masashi; Sasaki, Toshiki

JAEA-Review 2022-004, 106 Pages, 2022/06

JAEA-Review-2022-004.pdf:3.95MB

A numerous analytical data will be required for the characterization of the radioactive waste stored in Japan Atomic Energy Agency toward their processing and disposal. A "Data Quality Objectives (DQO) Process" is widely applied as a tool for the development of a cost-effective characterization plan in the overseas nuclear sites. The DQO Process is a multi-step planning process developed by the United States Environmental Protection Agency (EPA), and can be used for the planning of a scientifically rigorous and cost-effective data collection program for the various projects involving the collection of the environmental data. We have considered to reduce the cost required for the future characterization of the stored waste by applying the statistical methods and have performed a literature survey on the DQO Process. The survey effort was focused on the guidance documents of the DQO Process published by the EPA and was also spent for the related matters such as a quality system of the EPA and the activities beyond the DQO Process as well as the examples of the application at the nuclear sites. In this report, the details on the planning procedure using the DQO Process are reviewed together with the background information such as why DQO Process was developed, what kind of transition was occurred, and how it is currently used in the EPA. The examples on the application for various objects at Hanford Site in the United States, where has the various legacy waste generated in the past activities and has the big environmental problems, are also reviewed. This report summarizes the important matters and methodology on the planning with the statistical sampling methods. It also provides the examples of the approaches for the complex objects, and will therefore be helpful in the future planning for the various kind of the waste characterization.

Journal Articles

Development and evaluation of XRF imaging instrument for moving objects

Fuchita, Tomoki*; Urata, Taisei*; Matsuyama, Tsugufumi*; Murakami, Masashi; Yoshida, Yukihiko; Ueda, Akihiko; Machida, Masahiko; Sasaki, Toshiki; Tsuji, Koichi*

Advances in X-Ray Chemical Analysis, Japan, 53, p.77 - 87, 2022/03

X-ray fluorescence (XRF) analysis is an analytical method to obtain elemental information by detecting fluorescence X-rays emitted from a sample irradiated with X-rays. It is possible to obtain two-dimensional elemental distribution images by scanning a sample with micro X-ray beam. In this study, we developed an XRF analytical instrument to rapidly obtain the elemental distributions for moving samples on a belt conveyor by applying the micro XRF technique. X-rays were widely irradiated to the belt conveyor. The elemental distributions were measured by scanning an X-ray detector, crossing above the belt conveyor. A collimator was attached to the top of the detector to limit the analyzing area. Both detection limit and spatial resolutions for moving directions of the detector and the belt conveyor were evaluated. Finally, it was demonstrated that the multi-elemental imaging was possible with the developed XRF instrument.

JAEA Reports

Basic policy for rational measures of radioactive waste processing and disposal; Results of studies for acceleration of waste processing

Nakagawa, Akinori; Oyokawa, Atsushi; Murakami, Masashi; Yoshida, Yukihiko; Sasaki, Toshiki; Okada, Shota; Nakata, Hisakazu; Sugaya, Toshikatsu; Sakai, Akihiro; Sakamoto, Yoshiaki

JAEA-Technology 2021-006, 186 Pages, 2021/06

JAEA-Technology-2021-006.pdf:54.45MB

Radioactive wastes generated from R&D activities have been stored in Japan Atomic Energy Agency. In order to reduce the risk of taking long time to process legacy wastes, countermeasures for acceleration of waste processing and disposal were studied. Work analysis of waste processing showed bottleneck processes, such as evaluation of radioactivity concentration, segregation of hazardous and combustibles materials. Concerning evaluation of radioactivity concentration, a radiological characterization method using a scaling factor and a nondestructive gamma-ray measurement should be developed. The number of radionuclides that are to be selected for the safety assessment of the trench type disposal facility can decrease using artificial barriers. Hazardous materials, will be identified using records and nondestructive inspection. The waste identified as hazardous will be unpacked and segregated. Preliminary calculations of waste acceptance criteria of hazardous material concentrations were conducted based on environmental standards in groundwater. The total volume of the combustibles will be evaluated using nondestructive inspection. The waste that does not comply with the waste acceptance criteria should be mixed with low combustible material waste such as dismantling concrete waste in order to satisfy the waste acceptance criteria on a disposal facility average. It was estimated that segregation throughput of compressed waste should be increased about 5 times more than conventional method by applying the countermeasures. Further study and technology development will be conducted to realize the plan.

Journal Articles

Production of $$^{266}$$Bh in the $$^{248}$$Cm($$^{23}$$Na,5$$n$$)$$^{266}$$Bh reaction and its decay properties

Haba, Hiromitsu*; Fan, F.*; Kaji, Daiya*; Kasamatsu, Yoshitaka*; Kikunaga, Hidetoshi*; Komori, Yukiko*; Kondo, Narumi*; Kudo, Hisaaki*; Morimoto, Koji*; Morita, Kosuke*; et al.

Physical Review C, 102(2), p.024625_1 - 024625_12, 2020/08

 Times Cited Count:6 Percentile:59.56(Physics, Nuclear)

JAEA Reports

Study on the evaluation method to determine the radioactivity concentration in radioactive waste generated from the dismantling of research reactors

Murakami, Masashi; Hoshino, Yuzuru; Nakatani, Takayoshi; Sugaya, Toshikatsu; Fukumura, Nobuo*; Sanda, Toshio*; Sakai, Akihiro

JAEA-Technology 2019-003, 50 Pages, 2019/06

JAEA-Technology-2019-003.pdf:4.42MB

Toward the establishment of a common approach to determine the radioactivity concentrations in dismantling wastes arising from research reactors, radionuclide concentrations in the reactor structure materials of aluminum, carbon steel, shield concrete, and graphite of TRIGA Mark II reactor at Rikkyo University, Japan, were evaluated with both radiochemical analysis and theoretical calculation. The measured nuclides by the radiochemical analysis were $$^{3}$$H, $$^{60}$$Co, and $$^{63}$$Ni in aluminum, $$^{3}$$H, $$^{60}$$Co, $$^{63}$$Ni, and $$^{152}$$Eu in carbon steel, $$^{3}$$H, $$^{60}$$Co, and $$^{152}$$Eu in shield concrete, and $$^{3}$$H, $$^{14}$$C, $$^{60}$$Co, $$^{63}$$Ni, and $$^{152}$$Eu in graphite. Neutron-flux distributions and neutron-induced activities were computed with DORT and ORIGEN-ARP codes, respectively. Using the results of material composition analysis, radioactivity concentrations were conservatively predicted with good accuracy except for graphite material.

Journal Articles

Extraction behavior of rutherfordium as a cationic fluoride complex with a TTA chelate extractant from HF/HNO $$_{3}$$ acidic solutions

Yokoyama, Akihiko*; Kitayama, Yuta*; Fukuda, Yoshiki*; Kikunaga, Hidetoshi*; Murakami, Masashi*; Komori, Yukiko*; Yano, Shinya*; Haba, Hiromitsu*; Tsukada, Kazuaki; Toyoshima, Atsushi*

Radiochimica Acta, 107(1), p.27 - 32, 2019/01

 Times Cited Count:1 Percentile:11.15(Chemistry, Inorganic & Nuclear)

Journal Articles

Extraction behavior of Mo and W from H$$_{2}$$SO$$_{4}$$ and HF/HCl solutions into toluene with Aliquat336; Sulfate and fluoride complex formation of Mo and W towards chemical studies of seaborgium (Sg)

Toyoshima, Atsushi; Mitsukai, Akina; Tsukada, Kazuaki; Oe, Kazuhiro*; Haba, Hiromitsu*; Komori, Yukiko*; Murakami, Masashi; Kaneya, Yusuke*; Sato, Daisuke*; Asai, Masato; et al.

Journal of Radioanalytical and Nuclear Chemistry, 317(1), p.421 - 430, 2018/07

 Times Cited Count:2 Percentile:20.93(Chemistry, Analytical)

We have studied extraction behavior of group-6 elements Mo and W to search for suitable conditions for an on-line extraction experiment of their heavier homolog, seaborgium (Sg). Batch-wise extraction of carrier-free radiotracers $$^{93m}$$Mo and $$^{177,179,181}$$W were carried out from 0.10 - 8.6 M H$$_{2}$$SO$$_{4}$$ and 1.0$$times$$10$$^{-4}$$ - 5.0 M HF/1.0 M HCl into toluene with a quaternary ammonium compound, Aliquat336. Anionic sulfate complexes of Mo and W with charge - 2 were extracted with Aliquat336 from H$$_{2}$$SO$$_{4}$$ solutions with concentrations of [H$$_{2}$$SO$$_{4}$$] $$>$$ 2 M. In HF/1.0 M HCl, oxyfluoro complexes of Mo and W with charge - 1 were interpreted to be formed and extracted with Aliquat336. From these results, favorable conditions for the extraction of Sg are discussed.

Journal Articles

Determination of fusion barrier distributions from quasielastic scattering cross sections towards superheavy nuclei synthesis

Tanaka, Taiki*; Narikiyo, Yoshihiro*; Morita, Kosuke*; Fujita, Kunihiro*; Kaji, Daiya*; Morimoto, Koji*; Yamaki, Sayaka*; Wakabayashi, Yasuo*; Tanaka, Kengo*; Takeyama, Mirei*; et al.

Journal of the Physical Society of Japan, 87(1), p.014201_1 - 014201_9, 2018/01

 Times Cited Count:18 Percentile:74.47(Physics, Multidisciplinary)

Excitation functions of quasielastic scattering cross sections for the $$^{48}$$Ca + $$^{208}$$Pb, $$^{50}$$Ti + $$^{208}$$Pb, and $$^{48}$$Ca + $$^{248}$$Cm reactions were successfully measured by using the gas-filled recoil-ion separator GARIS. Fusion barrier distributions were extracted from these data, and compared with the coupled-channels calculations. It was found that the peak energies of the barrier distributions for the $$^{48}$$Ca + $$^{208}$$Pb and $$^{50}$$Ti + $$^{208}$$Pb systems coincide with those of the 2n evaporation channel cross sections for the systems, while that of the $$^{48}$$Ca + $$^{248}$$Cm is located slightly below the 4n evaporation ones. This results provide us helpful information to predict the optimum beam energy to synthesize superheavy nuclei.

Journal Articles

$$beta$$-delayed fission of $$^{230}$$Am

Wilson, G. L.*; Takeyama, Mirei*; Andreyev, A. N.; Andel, B.*; Antalic, S.*; Catford, W. N.*; Ghys, L.*; Haba, Hiromitsu*; He${ss}$berger, F. P.*; Huang, M.*; et al.

Physical Review C, 96(4), p.044315_1 - 044315_7, 2017/10

 Times Cited Count:6 Percentile:47.01(Physics, Nuclear)

Journal Articles

Study of the reaction $$^{48}$$Ca + $$^{248}$$Cm $$rightarrow$$ $$^{296}$$Lv$$^{ast}$$ at RIKEN-GARIS

Kaji, Daiya*; Morita, Kosuke*; Morimoto, Koji*; Haba, Hiromitsu*; Asai, Masato; Fujita, Kunihiro*; Gan, Z.*; Geissel, H.*; Hasebe, Hiroo*; Hofmann, S.*; et al.

Journal of the Physical Society of Japan, 86(3), p.034201_1 - 034201_7, 2017/03

 Times Cited Count:28 Percentile:81.43(Physics, Multidisciplinary)

The fusion reaction of $$^{48}$$Ca + $$^{248}$$Cm $$rightarrow$$ $$^{296}$$Lv$$^{ast}$$ was studied using the gas-filled recoil-ion separator GARIS at RIKEN. A total of seven $$alpha$$ and spontaneous-fission decay chains were observed, which would originate from the reaction products of the element 116, $$^{292}$$Lv and $$^{293}$$Lv. Decay properties observed in the chains are in good agreement with the previously published ones. However, one of the chains showed a discrepancy, indicating the new spontaneous-fission branch in $$^{285}$$Cn or the production of the new isotope $$^{294}$$Lv.

Journal Articles

Complex chemistry with complex compounds

Eichler, R.*; Asai, Masato; Brand, H.*; Chiera, N. M.*; Di Nitto, A.*; Dressler, R.*; D$"u$llmann, Ch. E.*; Even, J.*; Fangli, F.*; Goetz, M.*; et al.

EPJ Web of Conferences, 131, p.07005_1 - 07005_7, 2016/12

 Times Cited Count:3 Percentile:72.98(Chemistry, Inorganic & Nuclear)

In recent years gas-phase chemical studies assisted by physical pre-separation allowed for the productions and investigations of fragile single molecular species of superheavy elements. The latest highlight is the formation of very volatile hexacarbonyl compound of element 106, Sg(CO)$$_{6}$$. Following this success, second-generation experiments were performed to measure the first bond dissociation energy between the central metal atom and the surrounding ligand. The method using a tubular decomposition reactor was developed and successfully applied to short-lived Mo(CO)$$_{6}$$, W(CO)$$_{6}$$, and Sg(CO)$$_{6}$$.

Journal Articles

Decomposition studies of group 6 hexacarbonyl complexes, 1; Production and decomposition of Mo(CO)$$_6$$ and W(CO)$$_6$$

Usoltsev, I.*; Eichler, R.*; Wang, Y.*; Even, J.*; Yakushev, A.*; Haba, Hiromitsu*; Asai, Masato; Brand, H.*; Di Nitto, A.*; D$"u$llmann, Ch. E.*; et al.

Radiochimica Acta, 104(3), p.141 - 151, 2016/03

 Times Cited Count:31 Percentile:95.03(Chemistry, Inorganic & Nuclear)

Conditions of the production and decomposition of hexacarbonyl complexes of short-lived Mo and W isotopes were investigated to study thermal stability of the heaviest group 6 hexacarbonyl complex Sg(CO)$$_6$$. A tubular flow reactor was tested to decompose the hexacarbonyl complexes and to extract the first bond dissociation energies. A silver was found to be the most appropriate reaction surface to study the decomposition of the group 6 hexacarbonyl. It was found that the surface temperature at which the decomposition occurred was correlated to the first bond dissociation energy of Mo(CO)$$_6$$ and W(CO)$$_6$$, indicating that the first bond dissociation energy of Sg(CO)$$_6$$ could be determined with this technique.

Journal Articles

Performance of new gas-filled recoil ion separator GARIS-II for asymmetric fusion reaction

Kaji, Daiya*; Morimoto, Koji*; Wakabayashi, Yasuo*; Takeyama, Mirei*; Yamaki, Sayaka*; Tanaka, Kengo*; Haba, Hiromitsu*; Huang, M.*; Murakami, Masashi*; Kanaya, Jumpei*; et al.

JPS Conference Proceedings (Internet), 6, p.030107_1 - 030107_4, 2015/06

Performance of the new gas-filled recoil ion separator GARIS-II was investigated using asymmetric $$^{22}$$Ne-induced fusion reactions. The use of He-H$$_{2}$$ mixture gas for the gas-filled magnet significantly reduced background scattered particles detected at the focal-plane Si detector, and increased a transmission of the asymmetric reaction products. A target-identification system was newly installed for efficient measurements of excitation functions without changing beam energy nor target.

Journal Articles

Production of $$^{88}$$Nb and $$^{170}$$Ta for chemical studies of element 105, Db, using the GARIS gas-jet system

Huang, M.*; Haba, Hiromitsu*; Murakami, Masashi*; Asai, Masato; Kaji, Daiya*; Kanaya, Jumpei*; Kasamatsu, Yoshitaka*; Kikunaga, Hidetoshi*; Kikutani, Yuki*; Komori, Yukiko*; et al.

Journal of Radioanalytical and Nuclear Chemistry, 304(2), p.845 - 849, 2015/05

 Times Cited Count:3 Percentile:25.85(Chemistry, Analytical)

A technique to utilize radioisotopes of Nb and Ta was developed for chemical studies of element 105, Db, by coupling a gas-jet transport system to the RIKEN gas-filled recoil ion separator (GARIS). The short-lived $$^{88}$$Nb and $$^{170}$$Ta were produced with nuclear reactions using a $$^{19}$$F beam whose energy was the same as that to produce $$^{262}$$Db. Then, they were separated with GARIS and extracted to a chemistry laboratory with the gas-jet transport system. By changing only magnetic field of GARIS and inserting an energy degrader and a shutter for recoil ions, we could deliver the $$^{88}$$Nb and $$^{170}$$Ta to a chemistry device for $$^{262}$$Db without changing other experimental conditions.

Journal Articles

In situ synthesis of volatile carbonyl complexes with short-lived nuclides

Even, J.*; Ackermann, D.*; Asai, Masato; Block, M.*; Brand, H.*; Di Nitto, A.*; D$"u$llmann, Ch. E.*; Eichler, R.*; Fan, F.*; Haba, Hiromitsu*; et al.

Journal of Radioanalytical and Nuclear Chemistry, 303(3), p.2457 - 2466, 2015/03

 Times Cited Count:15 Percentile:77.56(Chemistry, Analytical)

Rapid In situ synthesis of metal carbonyl complexes has been demonstrated using short-lived isotopes produced in nuclear fission and fusion reactions. The short-lived isotopes with high recoil energy directly react with carbon-monoxides and form carbonyl complexes. Only highly volatile complexes were fast transported in a gas stream to counting and chemistry devices. Short-lived Mo, Tc, Ru, Rh, W, Re, Os, and Ir were found to form volatile carbonyl complexes, while no volataile complex of Hf and Ta were detected. This technique has been applied to a chemical investigation of the superheavy element Sg (atomic number 106), and will be applicable to various fields of nuclear science with short-lived transition metal isotopes.

Journal Articles

Synthesis and detection of a Seaborgium carbonyl complex

Even, J.*; Yakushev, A.*; D$"u$llmann, Ch. E.*; Haba, Hiromitsu*; Asai, Masato; Sato, Tetsuya; Brand, H.*; Di Nitto, A.*; Eichler, R.*; Fan, F. L.*; et al.

Science, 345(6203), p.1491 - 1493, 2014/09

 Times Cited Count:63 Percentile:83.28(Multidisciplinary Sciences)

A new superheavy element complex, a seaborgium carbonyl, has been successfully synthesized, and its adsorption property has been studied using a cryo-thermochromatography and $$alpha$$-detection apparatus COMPACT. Nuclear reaction products of short-lived $$^{265}$$Sg preseparated with a gas-filled recoil ion separator GARIS at RIKEN were directly injected into a gas cell filled with He/CO mixture gas, and chemical reaction products of volatile carbonyl complexes were trasported to COMPACT. The Sg carbonyl complex detected with COMPACT was found to be very volatile with adsorption enthalpy of $$-$$50 kJ/mol, from which we have concluded that this complex should be a Sg hexacarbonyl Sg(CO)$$_{6}$$. This is the first synthesis of organometallic compounds of transactinide elements for which only simple inorganic comounds have been synthesized so far.

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