Saito, Tatsuo; Sato, Kazuhiko; Yamazawa, Hiromi*
Journal of Environmental Radioactivity, 237, p.106708_1 - 106708_9, 2021/10
We succeeded at numerical reproduction of dissolved U concentrations from column experiments with PO-treated Hanford 300 Area sediment. The time-series curves of dissolved U concentrations under various Darcy flow rate conditions were reproduced by the numerical model in the present study through optimization of the following parameters:(i) the mass of U in mobile domain (on surface soil connected to the stream) and the rest of the total U left as precipitation in immobile domain (isolated in deep soil);(ii) the mixing ratio between immobile and mobile domains, to fit the final recovering curve of concentration; and (iii) the cation exchange capacity (CEC) and equilibrium constant (k) of the exchange reaction of UO and H on simulated soil surface (), to fit the transient equilibrium concentration, forming the bed of the bathtub curve.
Fichter, S.*; Radoske, T.*; Ikeda, Atsushi
Acta Crystallographica Section E; Crystallographic Communications (Internet), 77(8), p.847 - 852, 2021/08
Yasuda, Hiroshi*; Fumoto, Hiromichi*; Saito, Tatsuo
Nihon Genshiryoku Gakkai-Shi ATOMO, 63(8), p.610 - 614, 2021/08
Regarding the handling of uranium bearing waste, which is contaminated with uranium, which is a naturally occurring radionuclide, and its descendant nuclides, in recent years, the Japan Nuclear Regulatory Commission, etc. have been carefully and actively deliberated based on the knowledge of natural science and safety engineering. It was carried out, and as of March 2021, a certain policy has been shown. On the other hand, when disposing of uranium waste, which may cause dose exposure to future generations, the authors consider not only the science and engineering perspectives that have been conducted so far, but also the humanities and social science perspectives. We have been discussing with experts in related fields, thinking that it is necessary. In this report, we will introduce the background that brought about such an idea and the direction of future discussions.
Matsumoto, Yuji*; Haga, Yoshinori; Yamamoto, Etsuji; Takeuchi, Tetsuya*; Miyake, Atsushi*; Tokunaga, Masashi*
Journal of the Physical Society of Japan, 90(7), p.074707_1 - 074707_6, 2021/07
Miyajima, Yusuke*; Saito, Ayaka*; Kagi, Hiroyuki*; Yokoyama, Tatsunori; Takahashi, Yoshio*; Hirata, Takafumi*
Geostandards and Geoanalytical Research, 45(1), p.189 - 205, 2021/03
Uncertainty for elemental and isotopic analyses of calcite by LA-ICP-MS is largely controlled by the homogeneity of the reference materials (RMs) used for normalization and validation. In order to produce calcite RMs with homogeneous elemental and isotopic compositions, we incorporated elements including U, Pb, and rare earth elements into calcite through heat- and pressure-induced crystallization from amorphous calcium carbonate that was precipitated from element-doped reagent solution. X-ray absorption spectra showed that U was present as U(VI) in the synthesized calcite, probably with a different local structure from that of aqueous uranyl ions. The uptake rate of U by our calcite was higher in comparison to synthetic calcite of previous studies. Variations of element mass fractions in the calcite were better than 12% 2RSD, mostly within 7%. The Pb/Pb ratio in the calcite showed 1% variations, while the U/Pb ratio showed 3-24% variations depending on element mass fractions. Using the synthetic calcite as primary RMs, we could date a natural calcite RM, WC-1, with analytical uncertainty as low as 3%. The method presented can be useful to produce calcite with controlled and homogeneous element mass fractions, and is a promising alternative to natural calcite RMs for U-Pb geochronology.
Nagaoka, Mika; Fujita, Hiroki; Aida, Taku*; Guo, H.*; Smith, R. L. Jr.*
Applied Radiation and Isotopes, 168, p.109465_1 - 109465_6, 2021/02
The radioactivities in the environmental samples are analyzed to monitor the nuclear power facilities. The pretreatment of radioactive nuclides of alpha and beta emitters in the environmental samples is performed with acid to decompose organic matter and extract object nuclide such as Sr, U and Pu. However, the pretreatment methods are time-consuming and used many concentrated acid solutions that are unsafe and hazardous. Therefore, we develop to the new pretreatment method using supercritical water instead of acid. Hydrothermal pretreatment of soils (Andosols) from Ibaraki prefecture (Japan) was used to improve methods for monitoring radioactive Sr and U. Calcined samples were pretreated with subcritical or supercritical water (SCW) followed by extraction with 0.5 M HNO solutions. With SCW pretreatment, recoveries of Sr and U were 70% and 40%, respectively. Experimental recoveries obtained can be described by a linear relationship in water density. The proposed method is robust and can lower environmental burden of routine analytical protocols.
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.
Kokusen, Junya; Akasaka, Shingo*; Shimizu, Osamu; Kanazawa, Hiroyuki; Honda, Junichi; Harada, Katsuya; Okamoto, Hisato
JAEA-Technology 2020-011, 70 Pages, 2020/10
The Uranium Enrichment Laboratory in the Japan Atomic Energy Agency (JAEA) was constructed in 1972 for the purpose of uranium enrichment research. The smoke emitting accident on 1989 and the fire accident on 1997 had been happened in this facility. The research on uranium enrichment was completed in JFY1998. The decommissioning work was started including the transfer of the nuclear fuel material to the other facility in JFY2012. The decommissioning work was completed in JFY2019 which are consisting of removing the hood, dismantlement of wall and ceiling with contamination caused by fire accident. The releasing the controlled area was performed after the confirmation of any contamination is not remained in the target area. The radioactive waste was generated while decommissioning, burnable and non-flammable are 1.7t and 69.5t respectively. The Laboratory will be used as a general facility for cold experiments.
Task Force on Writing Textbook of Nuclear Fuel Materials
JAEA-Review 2020-007, 165 Pages, 2020/07
The present textbook was written by Task Force on Writing Textbook of Nuclear Fuel Materials at the Nuclear Science Research Institute in order to improve technological abilities of engineers and researchers who handle nuclear fuel materials. The taskforce consists of young and middle class engineers each having certification for chief engineer of nuclear fuel. The present textbook mainly deals with uranium and plutonium, and shows their nuclear properties, physical and chemical properties, and radiation effects on materials and human body. It also presents basic matters for safety handling of nuclear fuel materials, such as handling of nuclear fuel materials with hood and glovebox, important points in storage and transportation of nuclear fuel materials, radioactive waste management, radiation safety management, and emergency management. Furthermore, incident cases at domestic and foreign nuclear fuel materials facilities are compiled to learn from the past.
Yokoyama, Kaoru; Ohashi, Yusuke
Annals of Nuclear Energy, 141, p.107299_1 - 107299_5, 2020/06
A large amount of general steel waste is generated during decommissioning and dismantling of nuclear facilities. Very low-contaminated radioactive waste, whose radioactivity is below clearance level, generated from the demolition process may be reused for general use. We examined the feasibility of the clearance verification system for uranium waste. The relative error of uranium determination was within 30% for 1 g of uranium when measuring steel materials (angle bar, channel steel, pipe steel, square steel tube, fragments of metal tube).
Saito, Tatsuo; Kobayashi, Shinichi*; Zaitsu, Tomohisa*; Shimo, Michikuni*; Fumoto, Hiromichi*
Hoken Butsuri (Internet), 55(2), p.86 - 91, 2020/06
Safety cases for disposal of uranium bearing waste and NORM with uranium has not yet been fully developed in Japan, because of safety assessment of extraordinary long timespan and uncertainty in unexpected incidents with uncompleted radon impact evaluation measures arising from uranium waste disposal facility in far future. Our task group of radiation protection for wastes with natural radioactive nuclides studied some safety cases with disposal of uranium bearing waste and NORM in terms of nuclides, U-235, U-238 and their progenies, and comprehensively discussed the current state of their disposal in comparison to the ideas of international organizations such as ICRP and IAEA. We developed our ideas for long term uncertainty and radon with the knowledge of experts in each related area of direction, repeating discussions, focusing out the orientation of each directions, and outlined the recommendations with our suggestions of solving important issues in the future to be addressed.
Ikeuchi, Hirotomo; Yano, Kimihiko; Washiya, Tadahiro
Journal of Nuclear Science and Technology, 57(6), p.704 - 718, 2020/06
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 -(Zr,U)(O), while regions of high steel content were dominated by Fe(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.
Haga, Yoshinori; Sugai, Takashi*; Matsumoto, Yuji*; Yamamoto, Etsuji
JPS Conference Proceedings (Internet), 29, p.013003_1 - 013003_5, 2020/02
Fukushima, Masahiro; Goda, J.*; Oizumi, Akito; Bounds, J.*; Cutler, T.*; Grove, T.*; Hayes, D.*; Hutchinson, J.*; McKenzie, G.*; McSpaden, A.*; et al.
Nuclear Science and Engineering, 194(2), p.138 - 153, 2020/02
To validate lead (Pb) nuclear cross sections, a series of integral experiments to measure lead void reactivity worth was conducted systematically in three fast spectra with different fuel compositions on the Comet critical assembly of the National Criticality Experiments Research Center. Previous experiments in a high-enriched uranium (HEU)/Pb and a low-enriched uranium (LEU)/Pb systems had been performed in 2016 and 2017, respectively. A follow-on experiment in a plutonium (Pu)/Pb system has been completed. The Pu/Pb system was constructed using lead plates and weapons grade plutonium plates that had been used in the Zero Power Physics Reactor (ZPPR) of Argonne National Laboratory until the 1990s. Furthermore, the HEU/Pb system was re-examined on the Comet critical assembly installed newly with a device that can guarantee the gap reproducibility with a higher accuracy and precision, and then the experimental data was re evaluated. Using the lead void reactivity worth measured in these three cores with different fuel compositions, the latest nuclear data libraries, JENDL 4.0 and ENDF/B VIII.0, were tested with the Monte Carlo calculation code MCNP version 6.1. As a result, the calculations by ENDF/B-VIII.0 were confirmed to agree with lead void reactivity worth measured in all the cores. It was furthermore found that the calculations by JENDL 4.0 overestimate by more than 20% for the Pu/Pb core while being in good agreements for the HEU/Pb and LEU/Pb cores.
Sato, Yoshiyuki; Aono, Ryuji; Haraga, Tomoko; Ishimori, Kenichiro; Kameo, Yutaka
JAEA-Testing 2019-003, 20 Pages, 2019/12
In the Radioactive Waste Management Technology Section, the radioactive liquid waste generated in the test using natural uranium in the past has been stored based on the contents of permission. Although we decided to perform solidification treatment in order to reduce the risk in storage, no rational treatment method has been established so far. Therefore, we examined adsorption treatment of natural uranium using uranium adsorbent (Tannix), and finally stabilized treatment by cement solidification. The treatment methods and findings obtained for a series of operations in waste liquid treatment are summarized in this report for reference when treating similar liquid waste.
Kobayashi, Taishi*; Sasaki, Takayuki*; Kitamura, Akira
Journal of Chemical Thermodynamics, 138, p.151 - 158, 2019/11
The effect of -isosaccharinic acid (ISA) on the solubility and redox of tetravalent and hexavalent uranium (U(IV), U(VI)) was investigated in the hydrogen ion concentration (pH) range of 613 and at total ISA concentration ([ISA]) = 1010 mol/dm. The dependence of U(IV) solubility on pH and [ISA] suggested the existence of U(OH)(ISA) as a dominant species within the investigated pH range of 612. For the U(VI)-ISA system, UO(OH)(ISA) was suggested as a dominant species at pH 713. The formation constants of the U(IV)-ISA and U(VI)-ISA complexes were determined by least-squares fitting of the solubility data. The solubility of U(IV) and U(VI) in the presence of ISA and its effect on the redox behavior were thermodynamically interpreted based on the obtained constants.
Umezawa, Katsuhiro; Morimoto, Yasuyuki; Nakayama, Takuya; Nakagiri, Toshio
Proceedings of 27th International Conference on Nuclear Engineering (ICONE-27) (Internet), 6 Pages, 2019/05
In December 2016, the Ningyo-toge Environmental Engineering Center of Japan Atomic Energy Agency (JAEA Ningyo-toge) announced new concept of "Uranium and Environmental Research Platform". As part of the concept, uranium waste engineering research are now undergoing. The objective of the research is to establish the processing technology for safely and reasonable disposal of uranium waste. In particular, estimation of the amount of uranium and harmful substances and development of technologies to reduce their concentration in the waste to the permissive level for the disposal in shallow ground disposal are needed. We are now developing the technologies to reduce the concentration of uranium and harmful substances shown below. (1) Survey on uranium inventory. Uranium waste is now stored in 10-odd thousands of 200 L drums. We are surveying amount and chemical form of uranium in the drums. (2) Development of decontamination technology of metal and concrete waste. We are investigating decontamination methods for metals and concrete contaminated with uranium. (3) Development of technologies to remove, detoxify and fix the harmful substances. We are surveying the types and amounts of harmful substances in waste. In addition, we are investigating the method to remove, detoxify, and fix harmful substances. (4) Measurement technology of uranium radioactivity. We are investigating and examining ways to improve the quantitative accuracy of measurement and shorten the measurement time. (5) Development of uranium removal technology from sludge. We are investigating new processing method to remove uranium from sludge which is applicable for several kind of sludge. The results of these technological developments and environmental research will be reflected to "small-scale field test" and "disposal demonstration test" which are planned for demonstration of the uranium waste disposal technology.
Takahatake, Yoko; Koma, Yoshikazu
Proceedings of International Topical Workshop on Fukushima Decommissioning Research (FDR 2019) (Internet), 4 Pages, 2019/05
JAEA-Data/Code 2018-018, 103 Pages, 2019/03
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.
Li, D. X.*; Honda, Fuminori*; Miyake, Atsushi*; Homma, Yoshiya*; Haga, Yoshinori; Nakamura, Ai*; Shimizu, Yusei*; Maurya, A.*; Sato, Yoshiki*; Tokunaga, Masashi*; et al.
Physical Review B, 99(5), p.054408_1 - 054408_9, 2019/02