Effect of decay heat on pyrochemical reprocessing of minor actinide transmutation nitride fuels

Hayashi, Hirokazu; Tsubata, Yasuhiro; Sato, Takumi

Nihon Genshiryoku Gakkai Wabun Rombunshi (Internet), 22(3), p.97 - 107, 2023/08

https://doi.org/10.3327/taesj.J22.009

The Japan Atomic Energy Agency has chosen nitride fuel as the first candidate for the transmutation of long-lived minor actinides (MA) using accelerator-driven systems (ADS). The pyrochemical method has been considered for reprocessing spent MA nitride fuels, because their decay heat should be very large for aqueous reprocessing. This study was conducted to investigate the effect of decay heat on the pyrochemical reprocessing of MA nitride fuels. On the basis of the estimated decay heats and the temperature limits of the materials that are to be handled in pyrochemical reprocessing, quantities adequate for handling in argon gas atmosphere were evaluated. From these considerations, we proposed that an electrorefiner with a diameter of 26 cm comprising 12 cadmium (Cd) cathodes with a diameter of 4 cm is suitable. On the basis of the size of the electrorefiner, the number necessary to reprocess spent MA fuels from 1 ADS in 200 days was evaluated to be 25. Furthermore, the amount of Cd-actinides (An) alloy to produce An nitrides by the nitridation-distillation combined reaction process was proposed to be about one-quarter that of Cd-An cathode material. The evaluated sizes and required numbers of equipment support the feasibility of pyrochemical reprocessing for MA nitride fuels.

Evaluation of the mass transfer coefficients for the minor actinide separation; Evaluation by the single drop method

Sakamoto, Atsushi; Kibe, Satoshi*; Kawanobe, Kazunori*; Fujisaku, Kazuhiko*; Sano, Yuichi; Takeuchi, Masayuki; Suzuki, Hideya*; Tsubata, Yasuhiro; Ban, Yasutoshi; Matsumura, Tatsuro

JAEA-Research 2021-003, 30 Pages, 2021/06

JAEA-Research-2021-003.pdf:1.81MB

Japan Atomic Energy Agency has been developing a solvent extraction process called SELECT to recover minor actinides (MA) from spent nuclear fuel. In the SELECT process, TDdDGA, HONTA, and ADAAM are used as the extractants for MA + Ln corecovery, MA/Ln separation and Am/Cm separation, respectively. These extractants do not contain phosphorus (P), and consist of carbon (C), hydrogen (H), oxygen (O), and nitrogen (N). In this study, in order to give beneficial information for designing flowsheet, the mass transfer coefficients of Ln between HNO solution and TDdDGA or HONTA / n-dodecane solvent were evaluated by the single drop technique. Prior to the evaluation of mass transfer coefficient, we had optimized the structure of the single drop apparatus to improve accuracy of the measurement. Based on the mass transfer coefficients obtained in HNO / TDdDGA-n-dodecane system, Ln behaviors in the counter-current extraction and back-extraction using mixer-settlers and centrifugal contactors were estimated by simple calculation, and they had a good agreement with our previous experimental results. We also confirmed the mass transfer coefficients of Ln in HNO / HONTA - n-dodecane system are under 10 m/s.

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.

Material balance evaluation of pyroprocessing for minor actinide transmutation nitride fuel

Tateno, Haruka; Sato, Takumi; Tsubata, Yasuhiro; Hayashi, Hirokazu

Journal of Nuclear Science and Technology, 57(3), p.224 - 235, 2020/03

https://doi.org/10.1080/00223131.2019.1666056

Fuel cycle technology for the transmutation of long-lived minor actinides (MAs) using an accelerator-driven system has been developed using the double-strata fuel cycle concept. A mononitride solid solution of MAs and Pu diluted with ZrN is a prime fuel candidate for the accelerator-driven transmutation of MAs. Pyro-reprocessing is suitable for recycling the residual MAs in irradiated nitride fuel with high radiation doses and decay heat. Spent nitride fuel is anodically dissolved, and the actinides are recovered simultaneously into a liquid cadmium cathode via molten salt electrorefining. The process should be designed to achieve the target recovery yield of MAs and the acceptable impurity level of rare earths in the recovered material. We evaluated the material balance during the pyro-reprocessing of spent nitride fuel to gain important insight on the design process. We examined the effects of changing processing conditions on material flow and quantity of waste.

Minor actinides separation by -hexaoctyl nitrilotriacetamide (HONTA) using mixer-settler extractors in a hot cell

Ban, Yasutoshi; Suzuki, Hideya*; Hotoku, Shinobu; Tsutsui, Nao; Tsubata, Yasuhiro; Matsumura, Tatsuro

Solvent Extraction and Ion Exchange, 37(7), p.489 - 499, 2019/11

https://doi.org/10.1080/07366299.2019.1693486

A continuous counter-current experiment to separate minor actinides (MAs: Am and Cm) was performed with -hexaochyl nitrilotriacetamide (HONTA) as an extractant. Nitric acid of 0.08 M (mol/dm) containing MAs and rare earths (REs) recovered from high-level waste was used as the Feed, and the experiment was conducted for 14 h. The ratios of Am and Cm recovered into the MA fraction measured 94.9% and 78.9%, respectively. HONTA hardly extracted Y, La, and Eu in the Feed (99.9% for Y, 99.9% for La, and 96.7% for Eu), most of which were distributed to the RE fraction. A portion of Nd was extracted by HONTA, and consequently the ratio of Nd in the RE fraction was 83.5%. The concentrations of MAs and some REs in each stage were calculated using a simulation code, and the results are consistent with the experimental values. This code indicates that the ratios of MAs in the MA fraction and REs in the RE fraction could be 99% by optimizing separation conditions.

Uranium-based TRU multi-recycling with thermal neutron HTGR to reduce environmental burden and threat of nuclear proliferation

Fukaya, Yuji; Goto, Minoru; Ohashi, Hirofumi; Yan, X.; Nishihara, Tetsuo; Tsubata, Yasuhiro; Matsumura, Tatsuro

Journal of Nuclear Science and Technology, 55(11), p.1275 - 1290, 2018/11

AA2017-0752.pdf:1.25MB

https://doi.org/10.1080/00223131.2018.1492983

To reduce environmental burden and thread of nuclear proliferation, multi-recycling fuel cycle with High Temperature Gas-cooled Reactor (HTGR) has been investigated. Those problems are solved by incinerating TRans Uranium (TRU) nuclides, which is composed of plutonium and Minor Actinoide (MA), and there is concept to realize TRU incineration by multi-recycling with Fast Breeder Reactor (FBR). In this study, multi-recycling is realized even with thermal reactor by feeding fissile uranium from outside of the fuel cycle instead of breeding fissile nuclide. In this fuel cycle, recovered uranium by reprocessing and natural uranium are enriched and mixed with recovered TRU by reprocessing and partitioning to fabricate fresh fuels. The fuel cycle was designed for a Gas Turbine High Temperature Reactor (GTHTR300), whose thermal power is 600 MW, including conceptual design of uranium enrichment facility. Reprocessing is assumed as existing Plutonium Uranium Redox EXtraction (PUREX) with four-group partitioning technology. As a result, it was found that the TRU nuclides excluding neptunium can be recycled by the proposed cycle. The duration of potential toxicity decaying to natural uranium level can be reduced to approximately 300 years, and the footprint of repository for High Level Waste (HLW) can be reduced by 99.7% compared with GTHTR300 using existing reprocessing and disposal technology. Suppress plutonium is not generated from this cycle. Moreover, incineration of TRU from Light Water Reactor (LWR) cycle can be performed in this cycle.

Research on neutron capture cross sections at J-PARC in ImPACT Project

Nakamura, Shoji; Kimura, Atsushi; Hales, B. P.; Iwamoto, Osamu; Tsubata, Yasuhiro; Matsumura, Tatsuro; Shibahara, Yuji*; Uehara, Akihiro*; Fujii, Toshiyuki*

JAEA-Conf 2017-001, p.15 - 22, 2018/01

https://doi.org/10.11484/jaea-conf-2017-001

Neutron nuclear data of long lived fission products (LLFPs) have been required as basic data for the technology of reduce environmental impact involved in high level radioactive wastes (HLW). The innovative large project called by "Impusing Paradigm Change through Disruptive Technologies Program: ImPACT" have been started from October, 2014. In the ImPACT project, some research groups of JAEA engaged in the Project No.2 (Nuclear Reaction Data Measurements), and have started measurements of neutron capture cross-section at J-PARC/MLF/ANNRI. In our research, we selected cesium-135 (Cs) nuclide (half life: 2.310 yr.) among LLFPs in the HLW, and decided to measure the neutron capture cross-sections of Cs. When measurement, the Cs sample might contained cecium-137 (Cs) as impurities because it's impossible to chemically separate each other. To measure the cross-sections of Cs, there should be also needed to know the cross-sections of Cs. In this work, sample maintenance also has been examined especially for selen-79 (Se) nuclide among LLFPs having difficulty in sample preparations. In this oral session, the outline of our research project will be presented together with a research motivation, situations of past reported data, total schedules, progress, future plans, and some of high light data for neutron capture cross-section measurements.

Research and development on pyrochemical treatment of spent nitride fuels for MA transmutation in JAEA

Hayashi, Hirokazu; Sato, Takumi; Shibata, Hiroki; Tsubata, Yasuhiro

NEA/NSC/R(2017)3, p.427 - 432, 2017/11

Transmutation of long-lived radioactive nuclides including minor actinides (MA: Np, Am, Cm) has been studied in Japan Atomic Energy Agency (JAEA). Pb-Bi cooled sub-critical 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 MA-Pu nitride fuel was chosen as the first candidate for MA transmutation. Reprocessing of spent ADS fuel and reusing MA recovered from the spent ADS fuels is necessary to improve the transmutation ratio. A pyrochemical process has been proposed as the first candidate for reprocessing of the spent nitride fuel for MA transmutation, because this technique has some advantages over aqueous process, such as the resistance to radiation damage, which is an important issue for the fuels containing large amounts of highly radioactive MA, and feasibility for recovering expensive N-15 in the spent fuels to be reused. This paper overviews the current status of the technology development, including our recent study. Development of the anode suitable for electro-refining of nitride fuels and that of the apparatus for renitridation of the metals recovered in Cd cathode for 100g-Cd scale cold tests are main topics. Evaluation of the batch sizes of each process, which is necessary for estimating the scale of the engineering-apparatus, with considering the decay heat of MA and FP, will also be introduced.

High-performance alkyl diamide amine and water-soluble diamide ligand for separating of Am(III) from Cm(III)

Suzuki, Hideya; Tsubata, Yasuhiro; Matsumura, Tatsuro

Analytical Sciences, 33(2), p.239 - 242, 2017/02

https://doi.org/10.2116/analsci.33.239

Alkyl diamide amine (ADAAM), a new high-performance reagent with a simple structure, was examined for the mutual separation of Am(III) and Cu(III). The combination of ADAAM and Tetraethyldiglycolamide (TEDGA) as a masking agent shows selectivity for Am(III) over Cm(III) in highly acidic media with separation factors up to 41.

Spent fuel test equipment for research and development activities at NUCEF-BECKY

Suzuki, Asuka; Hotoku, Shinobu; Ban, Yasutoshi; Tsutsui, Nao; Tsubata, Yasuhiro; Matsumura, Tatsuro

Proceedings of 5th International Conference on Asian Nuclear Prospects 2016 (ANUP 2016) (CD-ROM), 2 Pages, 2016/10

The Japan Atomic Energy Agency (JAEA) conducts extensive research and development (R&D) activities toward the development of aqueous separation processes for spent nuclear fuel at the Nuclear Fuel Cycle Safety Engineering Research Facility-Back-end Fuel Cycle Key Element Research Facility (NUCEF-BECKY). BECKY is equipped with three hot cells, several glove boxes, and fume hoods. One of the hot cells, called the process cell, contains bench scale spent fuel test equipment used for U, Pu, and other spent fuel material. In this study, we describe an equipment used for aqueous separation processes in the process cell.