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JAEA Reports

Development of technology for separating Am-241 in aged plutonium

Emori, Tatsuya; Kitatsuji, Yoshihiro; Ban, Yasutoshi

JAEA-Technology 2024-025, 20 Pages, 2025/03

JAEA-Technology-2024-025.pdf:1.65MB

Radioisotope Thermoelectric Generators (RTGs) using the decay heat of Pu-238 has been applied for outer planet missions far from Jupiter, where solar power is limited. However, no facilities are available to produce Pu-238 for space probes in Japan. Moreover, the use of nuclear materials for the space exploration is difficult in term of the regulation. Thus, we focused on Am-241 whose half-life is around 432 years as an alternative heat source for RTGs. This report describes the procedure of separating Am-241 decayed from Pu-241 in aged plutonium oxide. Two experiments were performed: one using solid-liquid extraction and the other combining liquid-liquid extraction and solid-liquid extraction. Packed columns were used in the experiments, with their number reduced by less than one-fifth in the latter experiment compared to the former. Furthermore, the time required for separation in the latter experiment was less than half that of the former. We performed the separation experiments six times, collecting a total of approximately 0.43 g of Am-241 as an oxalate salt.

JAEA Reports

Annual report of Nuclear Science Research Institute, JFY 2023

Nuclear Science Research Institute

JAEA-Review 2024-058, 179 Pages, 2025/03

JAEA-Review-2024-058.pdf:7.42MB

Nuclear Science Research Institute (NSRI) is composed of Planning and Management Department and six departments, namely Department of Operational Safety Administration, Department of Radiation Protection, Engineering Services Department, Department of Research Reactor and Tandem Accelerator, Department of Criticality and Hot Examination Technology and Department of Decommissioning and Waste Management, and each department manages facilities and develops related technologies to achieve the "Medium- to Long-term Plan" successfully and effectively. And, four research centers which are Advanced Science Research Center, Nuclear Science and Engineering Center, Nuclear Engineering Research Collaboration Center and Materials Sciences Research Center, belong to NSRI. In order to contribute the future research and development and to promote management business, this annual report summarizes information on the activities of NSRI of JFY 2023 as well as the activity on research and development carried out by Collaborative Laboratories for Advanced Decommissioning Science, Nuclear Safety Research Center and activities of Nuclear Human Resource Development Center, using facilities of NSRI.

JAEA Reports

Annual report of Nuclear Science Research Institute, JFY 2022

Nuclear Science Research Institute

JAEA-Review 2024-057, 178 Pages, 2025/03

JAEA-Review-2024-057.pdf:8.51MB

Nuclear Science Research Institute (NSRI) is composed of Planning and Management Department and six departments, namely Department of Operational Safety Administration, Department of Radiation Protection, Engineering Services Department, Department of Research Reactor and Tandem Accelerator, Department of Criticality and Hot Examination Technology and Department of Decommissioning and Waste Management, and each department manages facilities and develops related technologies to achieve the "Medium- to Long-term Plan" successfully and effectively. And, four research centers which are Advanced Science Research Center, Nuclear Science and Engineering Center, Nuclear Engineering Research Collaboration Center and Materials Sciences Research Center, belong to NSRI. In order to contribute the future research and development and to promote management business, this annual report summarizes information on the activities of NSRI of JFY 2022 as well as the activity on research and development carried out by Collaborative Laboratories for Advanced Decommissioning Science, Nuclear Safety Research Center and activities of Nuclear Human Resource Development Center, using facilities of NSRI.

Journal Articles

Extraction behaviors of minor actinides and rare earth elements with NTA amide extractants

Suzuki, Hideya*; Ban, Yasutoshi

Journal of Nuclear Science and Technology, 62(2), p.157 - 166, 2025/02

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

Journal Articles

Solvent extraction of tin in nitric acids; Evaluation of multiple extractants

Ito, Kengo*; Takahashi, Shin*; Kato, Chizu*; Fukutani, Satoshi*; Matsumura, Tatsuro; Fujii, Toshiyuki*

Journal of Radioanalytical and Nuclear Chemistry, 334, p.2467 - 2475, 2025/02

 Times Cited Count:0 Percentile:0.00(Chemistry, Analytical)

In this study, the solvent extraction behavior of tin (Sn), specifically $$^{126}$$Sn, from high-level radioactive waste was evaluated using six different extractants in a HNO$$_{3}$$ system. Among the tested extractants, N,N-Didodecyl-2-hydroxyacetoamide (HAA) exhibited higher efficiency, still not sufficient for industrial implementation. In systems where HCl was added to HNO$$_{3}$$, both tributyl phosphate (TBP) and N,N,N,N'-tetra-2-ethylhexyl diglycolamide (TEHDGA) achieved D$$_{Sn}$$ values greater than 1 at $$>$$ 1 M HCl. However, due to practical challenges in industrial applications, HAA extraction in HNO$$_{3}$$ systems, particularly at low Sn concentrations (0.0008 M), may provide a more effective solution for Sn recovery.

Journal Articles

Development of a dissolution method for analyzing the elemental composition of fuel debris using sodium peroxide fusion technique

Nakamura, Satoshi; Ishii, Sho*; Kato, Hitoshi*; Ban, Yasutoshi; Hiruta, Kenta; Yoshida, Takuya; Uehara, Hiroyuki; Obata, Hiroki; Kimura, Yasuhiko; Takano, Masahide

Journal of Nuclear Science and Technology, 62(1), p.56 - 64, 2025/01

 Times Cited Count:1 Percentile:51.66(Nuclear Science & Technology)

A dissolution method for analyzing the elemental composition of fuel debris using the sodium peroxide (Na$$_{2}$$O$$_{2}$$) fusion technique has been developed. Herein, two different types of simulated debris materials (such as solid solution of (Zr,RE)O$$_{2}$$ and molten core-concrete interaction products (MCCI)) were taken. At various temperatures, these debris materials were subsequently fused with Na$$_{2}$$O$$_{2}$$ in crucibles, which are made of different materials, such as Ni, Al$$_{2}$$O$$_{3}$$, Fe, and Zr. Then, the fused samples are dissolved in nitric acid. Furthermore, the effects of the experimental conditions on the elemental composition analysis were evaluated using inductively coupled plasma-atomic emission spectroscopy (ICP-AES), which suggested the use of a Ni crucible at 923 K as an optimum testing condition. The optimum testing condition was then applied to the demonstration tests with Three Mile Island unit-2 (TMI-2) debris in a shielded concrete cell, thereby achieving complete dissolution of the debris. The elemental composition of TMI-2 debris revealed by the proposed dissolution method has good reproducibility and has an insignificant contradiction in the mass balance of the sample. Therefore, this newly developed reproducible dissolution method can be effectively utilized in practical applications by dissolving fuel debris and estimating its elemental composition.

Journal Articles

Solvent extraction behaviors of rhodium and palladium in nitric acid solutions using amide extractants

Ito, Kengo*; Morita, Misaki*; Araki, Yuta*; Kato, Chizu*; Fukutani, Satoshi*; Matsumura, Tatsuro; Fujii, Toshiyuki*

Solvent Extraction Research and Development, Japan, 32(1), p.53 - 62, 2025/00

Rhodium (Rh) and Palladium (Pd) in high-level radioactive waste are primarily fission products. This Study focused on understanding the extraction behavior of these platinum group elements (PGEs) using the novel extractants ${it N,N,N',N',N'',N''}$-hexaoctylnitriloacetamide (HONTA) and alkyl diamideamine (ADAAM). Both extractants showed affinity for Pd, with distribution coefficients significantly exceeding 1, demonstrating their effectiveness in Pd separation. In contrast, the distribution coefficients for Rh were consistently below 10 $$^{-1}$$, indicating low extraction efficiency from nitric acid. However, by leveraging the salting-out effect with calcium nitrate hydrate, a distribution coefficient of $$sim$$570 for Rh was achieved using HONTA. To overcome the difficult back-extraction of PGEs with HONTA, experiments were conducted using HEDTA and thiourea. Back-extraction with HEDTA in high-concentration nitric acid ($$>$$2M) resulted in $$sim$$90% extraction of Pd, while thiourea-based back-extraction with nitric acid yielded over 40% extraction for Rh, with the maximum of 62.7% achieved using hydrochloric acid.

Journal Articles

Solvent extraction of selenium in nitric acid; Evaluation of multiple extractants and proposal of a novel separation process

Ito, Kengo*; Kawakami, Takahiro*; Kato, Chizu*; Fukutani, Satoshi*; Matsumura, Tatsuro; Fujii, Toshiyuki*

Journal of Radioanalytical and Nuclear Chemistry, 333(10), p.5183 - 5189, 2024/10

 Times Cited Count:1 Percentile:51.66(Chemistry, Analytical)

Solvent extraction behaviors of Se (VI) from nitric acid solutions were investigated with multiple extractants used for uranium, plutonium, minor actinides, and rare earthelements separation processes from high-level liquid waste. During the processes, Se remained in the residual aqueous solutions, as all extractants showed distributionratios $$<$$ 1. In contrast, Se showed distribution ratios $$>$$ 1 with $$o$$-phenylenediamine in dilute nitric acid ($$<$$ 2 M HNO$$_{3}$$), octanol as the organic phase, and concentrated nitric acid (8 M HNO$$_{3}$$) for back extraction, suggesting a potential new single separation process and recovery of Se.

Journal Articles

Recovery of minor actinides from HLW using Hexaoctyl nitrilotriacetamide (HONTA) by mixer-settler extractors

Ban, Yasutoshi; Suzuki, Hideya*; Hotoku, Shinobu; Tsubata, Yasuhiro

Proceedings of International Conference on Nuclear Fuel Cycle (GLOBAL2024) (Internet), 4 Pages, 2024/10

A continuous counter-current extraction experiment was performed by mixer-settler extractors to recover minor actinides (MA; Am and Cm) from high-level liquid waste. Using hexaoctyl nitrilotriacetamide (HONTA) as an extractant, 0.17 g of MA was recovered in a MA fraction.

Journal Articles

Electrochemical behavior of neptunium in NaCl-2CsCl melt

Hayashi, Hirokazu; Minato, Kazuo*

Electrochemistry (Internet), 92(4), p.043020_1 - 043020_5, 2024/04

 Times Cited Count:0 Percentile:0.00(Electrochemistry)

The electrochemical behavior of neptunium in NaCl-2CsCl melt at 823-923 K was investigated by cyclic voltammetry, differential pulse voltammetry, and open-circuit chronopotentiometry after polarization. The results show that Np$$^{4+}$$ ions are reduced to Np metal by a two-step mechanism via Np$$^{3+}$$ ions in NaCl-2CsCl melt. The diffusion coefficients of Np$$^{3+}$$ and Np$$^{4+}$$ ions were determined from cyclic voltammograms. The apparent standard potentials of Np$$^{3+}$$/Np$$^{0}$$ and Np$$^{4+}$$/Np$$^{3+}$$ redox couples have been determined to be E$$^*$$(Np$$^{3+}$$/Np$$^0$$) = -3.353 + 7.67$$times$$10$$^{-4}$$T, and E$$^*$$(Np$$^{4+}$$/Np$$^{3+}$$) = -1.175 + 4.99$$times$$10$$^{-4}$$ T vs. Cl$$_2$$/Cl$$^-$$ (V), respectively. The activity coefficients of Np$$^{3+}$$ and Np$$^{4+}$$ ions were also determined using the reported data on the Gibbs free energy of formation for NpCl$$_3$$ and NpCl$$_4$$ in supercooled liquid state.

JAEA Reports

Annual report of Nuclear Science Research Institute, JFY2021

Nuclear Science Research Institute, Sector of Nuclear Science Research

JAEA-Review 2023-050, 178 Pages, 2024/03

JAEA-Review-2023-050.pdf:7.06MB

Nuclear Science Research Institute (NSRI) is composed of Planning and Management Department and six departments, namely Department of Operational Safety Administration, Department of Radiation Protection, Engineering Services Department, Department of Research Reactor and Tandem Accelerator, Department of Criticality and Hot Examination Technology and Department of Decommissioning and Waste Management, and each department manages facilities and develops related technologies to achieve the "Medium- to Long- term Plan" successfully and effectively. And, four research centers which are Advanced Science Research Center, Nuclear Science and Engineering Center, Nuclear Engineering Research Collaboration Center and Materials Sciences Research Center, belong to NSRI. In order to contribute the future research and development and to promote management business, this annual report summarizes information on the activities of NSRI of JFY 2021 as well as the activity on research and development carried out by Collaborative Laboratories for Advanced Decommissioning Science, Nuclear Safety Research Center and activities of Nuclear Human Resource Development Center, using facilities of NSRI.

Journal Articles

Flexible waste management system for the future application of MA P&T technology to the current high-level liquid waste

Fukasawa, Tetsuo*; Suzuki, Akihiro*; Endo, Yoichi*; Inagaki, Yaohiro*; Arima, Tatsumi*; Muroya, Yusa*; Endo, Keita*; Watanabe, Daisuke*; Matsumura, Tatsuro; Ishii, Katsunori; et al.

Journal of Nuclear Science and Technology, 61(3), p.307 - 317, 2024/03

 Times Cited Count:2 Percentile:43.92(Nuclear Science & Technology)

A flexible waste management system (FWM) is being developed to apply future MA partitioning and transmutation (P&T) technology to current HLLW. This FWM system will store high-level waste (HLLW) in granular form until MA partitioning and transmutation technology is realized. The feasibility of the main process was essentially confirmed by basic experiments and preliminary thermal analysis for granule production by rotary kiln from simulated HLLW and for temporary storage (50 years) of HLW granules at the HLW storage facility, respectively. The granule production experiments revealed that relatively large particles can be produced by the rotary kiln. The results of the thermal analysis showed that the small diameter canisters could be used to safely store the granules at a higher storage density than vitrified HLW. The effectiveness of the FWM system in terms of potential radiotoxicity and repository area was also evaluated, and it was shown that FWM can reduce these factors and has significant advantages in the disposal of HLW generated in current reprocessing plants. Since LWR fuel is stored for a long period of time in Japan and the operation of a reprocessing plant is expected to start soon, the FWM system is considered to be an effective system for reducing the environmental burden of HLW disposal.

Journal Articles

A Demonstration test to separate minor actinides in high-level liquid waste by ${it N,N,N',N',N'',N''}$-hexaoctyl nitrilotriacetamide (HONTA) using mixer-settler extractors in a hot cell

Ban, Yasutoshi; Suzuki, Hideya*; Hotoku, Shinobu; Tsubata, Yasuhiro

Solvent Extraction Research and Development, Japan, 31(1), p.1 - 11, 2024/00

A demonstration test was performed to separate minor actinides (MA; Am and Cm) by ${it N,N,N',N',N'',N''}$-hexaoctyl nitrilotriacetamide (HONTA) as an extractant using mixer-settler extractors installed in a hot cell. A high-level liquid waste containing MA, and rare earths (RE; Y, La, Nd, and Eu) was used as the feed. HONTA diluted to 0.05 mol/dm$$^{3}$$ in ${it n}$-dodecane was fed as the organic phase, and a part of the organic phase was reused without solvent regeneration. HONTA effectively extracted MA, whereas RE were less extractable. Consequently, the Y, La, Nd, and Eu ratios distributed to a RE fraction were $$>$$ 99.9%, 99.2%, 61.8%, and 81.4%, respectively. The Am and Cm ratios distributed to an MA fraction were 86.8% and 74.7%, respectively, and a substantial amount of MA (0.12 g) was recovered in the MA fraction by the end of the cumulative duration of 40 h.

Journal Articles

Development of an integrated non-destructive analysis system, Active-N

Tsuchiya, Harufumi; Toh, Yosuke; Ozu, Akira; Furutaka, Kazuyoshi; Kitatani, Fumito; Maeda, Makoto; Komeda, Masao

Journal of Nuclear Science and Technology, 60(11), p.1301 - 1312, 2023/11

 Times Cited Count:3 Percentile:59.85(Nuclear Science & Technology)

Journal Articles

Development of a DDA+PGA-combined non-destructive active interrogation system in "Active-N"

Furutaka, Kazuyoshi; Ozu, Akira; Toh, Yosuke

Nuclear Engineering and Technology, 55(11), p.4002 - 4018, 2023/11

 Times Cited Count:1 Percentile:23.64(Nuclear Science & Technology)

Journal Articles

Planning of the debris-simulated critical experiments on the new STACY

Gunji, Satoshi; Araki, Shohei; Arakaki, Yu; Izawa, Kazuhiko; Suyama, Kenya

Proceedings of 12th International Conference on Nuclear Criticality Safety (ICNC2023) (Internet), 9 Pages, 2023/10

JAEA has been modifying a critical assembly called STACY from a solution system to a light-water moderated heterogeneous system to validate computation results of criticality characteristics of fuel debris generated in the accident at TEPCO's Fukushima Daiichi Nuclear Power Station. To experimentally simulate the composition and characteristics of fuel debris, we will prepare several grid plates which make particular neutron moderation conditions and a number of rod-shaped concrete and stainless-steel materials. Experiments to evaluate fuel debris's criticality characteristics are scheduled using these devices and materials. This series of STACY experiments are planned to measure the reactivity of fuel debris-simulated samples, measure the critical mass of core configurations containing structural materials such as concrete and stainless steels, and the change in critical mass when their arrangement becomes non-uniform. Furthermore, two divided cores experiments are scheduled that statically simulate fuel debris falling, and also scheduled that subcriticality measurement experiments with partially different neutron moderation conditions. The experimental plans have been considered taking into account some experimental constraints. This paper shows the schedule of these experiments, as well as the computation results of the optimized core configurations and expected results for each experiment.

Journal Articles

Status on the development of the fabrication and analysis equipment of the pseudo fuel debris

Kobayashi, Fuyumi; Fukaya, Hiroyuki; Izawa, Kazuhiko; Kida, Takashi; Sono, Hiroki; Suyama, Kenya

Proceedings of 12th International Conference on Nuclear Criticality Safety (ICNC2023) (Internet), 7 Pages, 2023/10

In the criticality experiment in the new STACY, pseudo fuel debris samples are used to acquire data for validation of the system used for 1F debris criticality safety assessment. The pseudo fuel debris is a pellet with a diameter of 8 mm and a height of 10 mm containing uranium oxide and structural materials (iron, silicon, zirconium, etc.). The pellets are made by mixing, pressing and sintering uranium dioxide powder and structural materials powder. The UO$$_{2}$$ powder uses the same composition of uranium as the STACY driver fuel rods, in order to reduce the errors in fuel composition. The pseudo fuel debris fabrication devices and analysis equipment are installed at the BECKY in order to evaluate the critical properties of fuel debris with high accuracy in dimension and analysis. This equipment is located in the same laboratory and can quickly respond to experimental needs such as preparation of the pseudo fuel debris and analysis before and after irradiation.

Journal Articles

Study on criticality safety control of fuel debris for validation of methodology applied to the safety regulation

Suyama, Kenya; Ueki, Taro; Gunji, Satoshi; Watanabe, Tomoaki; Araki, Shohei; Fukuda, Kodai; Yamane, Yuichi; Izawa, Kazuhiko; Nagaya, Yasunobu; Kikuchi, Takeo; et al.

Proceedings of 12th International Conference on Nuclear Criticality Safety (ICNC2023) (Internet), 6 Pages, 2023/10

To remove and store safely the fuel debris generated by the severe accident of the Fukushima Daiichi Nuclear Power Station in 2011 is one of the most important and challenging topics for decommissioning of the damaged reactors in Fukushima. To validate the adopted method for the evaluation of criticality safety control of the fuel debris through comparison with the experimental data obtained by the criticality experiments, the Nuclear Regulation Authority (NRA) of Japan funds a research and development project which was entrusted to the Nuclear Safety Research Center (NSRC) of Japan Atomic Energy Agency (JAEA) from 2014. In this project, JAEA has been conducting such activities as i) comprehensive computation of the criticality characteristics of the fuel debris and making database (criticality map of the fuel debris), ii) development of new continuous energy Monte Carlo code, iii) evaluation of criticality accident and iv) modification of the critical assembly STACY for the experiments for validation of criticality safety control methodology. After the last ICNC2019, the project has the substantial progress in the modification of STACY which will start officially operation from May 2024 and the development of the Monte Carlo Code "Solomon" suitable for the criticality calculation for materials having spatially random distribution complies with the power spectrum. We present the whole picture of this research and development project and status of each technical topics in the session.

Journal Articles

Efficient separation of americium by a mixed solvent of two extractants, a diamideamine and a nitrilotriacetamide

Suzuki, Hideya*; Ban, Yasutoshi

Analytical Sciences, 39(8), p.1341 - 1348, 2023/08

 Times Cited Count:4 Percentile:46.80(Chemistry, Analytical)

The Japan Atomic Energy Agency (JAEA) has proposed the Solvent Extraction from Liquid waste using Extractants of CHON-type for Transmutation (SELECT) process by solvent extraction as a new separation technology to recover minor actinides (MA) from high-level liquid waste (HLLW) produced by spent fuel reprocessing. The MA separation in the SELECT process comprises the batch recovery of MA and rare earths (RE) from HLLW, MA/RE separation, and Am/Cm separation. Three highly practical extractants are used in the MA separation. Furthermore, this flow configuration facilitates the preparation of nitric acid concentrations in the aqueous phase. However, the separation factor between Cm and Nd in the MA/RE separation is small ($$SF$$$$_{rm Cm/Nd}$$ = 2.5), requiring many extraction stages for continuous extraction in a mixer-settler. Therefore, this study investigated the separation of only Am from an aqueous nitric acid solution containing MA (Am and Cm) and RE using an organic phase mixed with two extractants alkyl diamideamine with 2-ethylhexyl alkyl chains (ADAAM(EH)) and hexa-n-octylnitrilotriacetamide (HONTA) used in the SELECT process. Under high-concentration nitric acid conditions, Am and La, Ce, Pr, Nd (light lanthanides) were extracted in the ADAAM(EH) + HONTA mixed solvent, whereas Cm, medium, and heavy lanthanides, and Y were partitioned in the aqueous phase. Subsequently, only light lanthanides could be back extracted from the ADAAM(EH) + HONTA mixture solvent containing Am and light lanthanides in low nitric acid concentrations. Furthermore, Am could be easily stripped with 0.2 M or 5 M nitric acid. This method does not require the mutual separation of Cm and Nd, which have low separation factors. Am can be efficiently separated by one extraction and two back-extractions, reducing the number of steps in the SELECT process.

Journal Articles

Effect of calcium on niobium solubility in alkaline solutions

Ohira, Saki; Abe, Takeyasu; Iida, Yoshihisa

Radiochimica Acta, 111(7), p.525 - 531, 2023/07

 Times Cited Count:0 Percentile:0.00(Chemistry, Inorganic & Nuclear)

The solubility of $$^{94}$$Nb in calcium alkaline solutions is one of the important parameters in safety assessment of intermediate-depth disposal which are assumed to use cementitious materials. Nb solubility and solubility-limiting solid phases of Nb in these systems remain unclear. The oversaturation solubility experiments were performed systematically in the 0.001-0.1 M CaCl$$_{2}$$ solutions under alkali conditions, and the characterization of precipitated solid phase controlling Nb solubility was conducted. The negative dependence of Nb solubilities on pH and Ca concentration was observed in solubility experiments, the molar ratio of Nb to Ca of precipitated solid phase was 0.66. The pH and Ca dependence of Nb solubilities was reproduced by the reaction with Nb aqueous species Nb(OH)$$_{6}$$$$^{-}$$ and Ca-Nb oxide with the molar ratio of Nb to Ca 0.66, e.g., Ca$$_{4}$$Nb$$_{6}$$O$$_{19}$$(am).

212 (Records 1-20 displayed on this page)