Stabilization of post-experiment nuclear materials in Plutonium Fuel Research Facility

Sato, Takumi; Otobe, Haruyoshi; Morishita, Kazuki; Marufuji, Takato; Ishikawa, Takashi; Fujishima, Tadatsune; Nakano, Tomoyuki

JAEA-Technology 2023-016, 41 Pages, 2023/09

JAEA-Technology-2023-016.pdf:2.74MB

This report summarizes the results of the stabilization treatments of post-experiment nuclear materials in Plutonium Fuel Research Facility (PFRF) from August 2018 to March 2021. Based on the management standards for nuclear materials enacted after the contamination accident that occurred at PFRF on June 6, 2017, the post-experiment nuclear materials containing plutonium (Pu): samples mixed with organic substances that cause an increase in internal pressure due to radiolysis (including X-ray diffraction samples mixed with epoxy resin and plutonium powder which caused contamination accidents), carbides and nitrides samples which is reactive in air, and chloride samples which may cause corrosion of storage containers, were selected as targets of the stabilization. The samples containing organic materials, carbides and nitrides were heated in an air flow at 650 C and 950 C for 2 hours respectively to remove organic materials and convert uranium (U) and Pu into oxides. U and Pu chlorides in LiCl-KCl eutectic melt were reduced and extracted into liquid Cd metal by a reaction with lithium (Li) -cadmium (Cd) alloy and converted to U-Pu-Cd alloy at 500 C or higher. All of the samples were stabilized and stored at PFRF. We hope that the contents of this report will be utilized to consider methods for stabilizing post experiment nuclear materials at other nuclear fuel material usage facilities.

Formation of MPd (M = Gd, Np) by the reaction of MN with Pd and chlorination of MPd using cadmium chloride

Hayashi, Hirokazu; Shibata, Hiroki; Sato, Takumi; Otobe, Haruyoshi

Journal of Radioanalytical and Nuclear Chemistry, 332(2), p.503 - 510, 2023/02

https://doi.org/10.1007/s10967-023-08760-4

The formation of MPd (M = Gd, Np) by the reaction of MN with Pd at 1323 K in Ar gas flow was observed. Cubic AuCu-type GdPd ( = 0.4081 0.0001 nm) and NpPd ( = 0.4081 0.0001 nm) were identified, respectively. The product obtained from the reaction of NpN with Pd contained additional phases including the hexagonal TiNi-type NpPd. Chlorination of the MPd (M = Gd, Np) samples was accomplished by the solid-state reaction using cadmium chloride at 673 K in a dynamic vacuum. Pd-rich solid solution phase saturated with Cd and an intermetallic compound PdCd were obtained as by-products of MCl formation.

The Chemistry of thorium, plutonium and MA

Sato, Nobuaki*; Kirishima, Akira*; Watanabe, Masayuki; Sasaki, Takayuki*; Uehara, Akihiro*; Takeda, Shino*; Kitatsuji, Yoshihiro; Otobe, Haruyoshi; Kobayashi, Taishi*

The Chemistry of Thorium, Plutonium and MA, 254 Pages, 2022/03

The chemistry of nuclear materials such as Thorium (Part 1) and Plutonium (Part 2) was described in relation from the fundamentals on solid chemistry and solution chemistry to the practicals on the experiment and evaluation method in detail. Minor actinides such as Neptunium, Americium, Curium and Protoactinium, was introduced the basics on the solid and solution chemistry.

Measurement of plutonium spectrum using laser induced breakdown spectroscopy; High resolution spectroscopy (350-670nm)

Akaoka, Katsuaki; Oba, Masaki; Miyabe, Masabumi; Otobe, Haruyoshi; Wakaida, Ikuo

JAEA-Research 2020-001, 142 Pages, 2020/03

JAEA-Research-2020-001.pdf:4.0MB

Laser Induced Breakdown Spectroscopy (LIBS) method is an attractive technique because real-time, in-situ and remote elemental analysis is possible without any sample preparation. The LIBS technique can be applied for analyzing elemental composition of samples under severe environments such as the estimation of impurities in the next generation nuclear fuel material containing minor actinide (MA) and the detection of fuel debris in the post-accident nuclear core reactor of TEPCO's Fukushima Daiichi Nuclear Power Station. For applying LIBS to the analysis of nuclear fuel materials, it is indispensable to identify the emission spectrum and its intensity on impurities intermingled within complex emission spectra of matrix elements such as uranium (U) and plutonium (Pu). In the present study, an echelle spectrometer with a resolving power of 50,000 was employed to identify spectra of plutonium of wavelength ranging from 350 to 670nm. The 465 atomic spectra and 341 ionic spectra can be identified. We have confirmed that the measured wavelength of spectra is consistent with published values.

Preliminary missions for the decommissioning of the laboratory building No.1 for the plutonium research program

Segawa, Yukari; Horita, Takuma; Kitatsuji, Yoshihiro; Kumagai, Yuta; Aoyagi, Noboru; Nakada, Masami; Otobe, Haruyoshi; Tamura, Yukito*; Okamoto, Hisato; Otomo, Takashi; et al.

JAEA-Technology 2016-039, 64 Pages, 2017/03

JAEA-Technology-2016-039.pdf:5.24MB

The laboratory building No.1 for the plutonium research program (Bldg. Pu1) was chosen as one of the facilities to decommission by Japan Atomic Energy Agency Reform in September, 2013. The research groups, users of Bldg. Pu1, were driven by necessity to remove used equipment and transport nuclear fuel to other facilities from Bldg. Pu1. Research Group for Radiochemistry proactively established the Used Equipment Removal Team for the smooth operation of the removal in April, 2015. The team classified six types of work into the nature of the operation, removal of used equipment, disposal of chemicals, stabilization of mercury, stabilization of nuclear fuel, transportation of nuclear fuel and radioisotope, and survey of contamination status inside the glove boxes. These works were completed in December, 2015. This report circumstantially shows six works process, with the exception of the approval of the changes on the usage of nuclear fuel in Bldg. Pu1 to help prospective decommission.

Measurement of uranium spectrum using laser induced breakdown spectroscopy; High resolution spectroscopy (470-670 nm)

Akaoka, Katsuaki; Oba, Masaki; Miyabe, Masabumi; Otobe, Haruyoshi; Wakaida, Ikuo

JAEA-Research 2016-005, 40 Pages, 2016/05

JAEA-Research-2016-005.pdf:1.82MB

Laser Induced Breakdown Spectroscopy (LIBS) method is an attractive technique because real-time, in-situ and remote elemental analysis is possible without any sample preparation. The LIBS technique can be applied for analyzing elemental composition of samples under severe environments such as the estimation of impurities in the next generation nuclear fuel material containing minor actinide (MA) and the detection of fuel debris in the post-accident nuclear core reactor of TEPCO Fukushima Daiichi Nuclear Power Plant. For applying LIBS to the analysis of nuclear fuel materials, it is indispensable to identify the emission spectrum and its intensity on impurities intermingled within complex emission spectra of matrix elements such as uranium (U) and plutonium (Pu). In the present study, an echelle spectrometer with a resolving power of 50,000 was employed to identify spectra of natural uranium of wavelength ranging from 470 to 670 nm. The 173 atomic spectra and 119 ionic spectra can be identified. We have confirmed that the measured wavelength and oscillator strength of spectra are consistent with published values.

Laser-induced breakdown spectroscopy for nuclear fuel material

Akaoka, Katsuaki; Miyabe, Masabumi; Otobe, Haruyoshi; Wakaida, Ikuo

Reza Kenkyu, 42(12), p.918 - 922, 2014/12

For the remote analysis of the next generation nuclear fuel material containing minor actinide (MA), Laser Induced Breakdown Spectroscopy (LIBS) was applied to uranium oxide (UO) including a small amount of neodymium oxide (NdO) as a simulated sample of MA. By using deconvolution technique for the spectra of Nd in U, the complex, overlapped and confused spectra were separated and their actual intensities were determined. As a result, the calibration curve with good linearity and the detection limit of less than 700 ppm were demonstrated.

Propagation of U(V)-reduction in the presence of U(IV) aggregate in a weakly acidic solution

Kitatsuji, Yoshihiro; Otobe, Haruyoshi; Kimura, Takaumi; Kihara, Sorin*

Electrochimica Acta, 141, p.6 - 12, 2014/09

https://doi.org/10.1016/j.electacta.2014.07.012

Reduction processes of U(VI) in weakly acidic solutions were investigated based on electrochemical and spectrophotometric measurements. A reversible one-electron reduction of U(VI) to U(V) and a further irreversible reduction of U(V) were observed voltammetrically at a gold microdisk electrode in solutions of pH from 2.0 to 3.5. Aggregates of U(IV) were formed as a deposit on the electrode and a colloid in the bulk solution, when the electrolysis was carried out at a gold gauze electrode, even though the potential applied was that available for the first one-electron reduction wave of U(VI) observed. It was elucidated that the aggregate was produced by the combination of the one-electron reduction to U(V) and the disproportionation of U(V) producing U(IV) and U(VI). The aggregate enhanced the rate of the disproportionation of U(V), and hence the reduction current of U(VI) increased abruptly when a definite amount of aggregate was formed on the electrode, in the solution, or both.

Syntheses and thermal analyses of curium trichloride

Hayashi, Hirokazu; Takano, Masahide; Otobe, Haruyoshi; Koyama, Tadafumi*

Journal of Radioanalytical and Nuclear Chemistry, 297(1), p.139 - 144, 2013/07

https://doi.org/10.1007/s10967-012-2413-7

Curium trichloride was synthesized by the solid state reaction of curium nitride with cadmium chloride heated from room temperature to 748K in a dynamic vacuum. The product was hexagonal CmCl, of which lattice parameters were determined to be a= 0.73850.0005 and c= 0.42010.0005 nm. The melting temperature of the CmCl sample was determined to be 9703 K by differential thermal analyses using a gold crucible. These values are close to those reported in literatures. The results show that mg-scale CmCl samples for thermochemical measurements were prepared from the purified oxide sample without the use of corrosive reagents.

Maintenance of Module for TRU High Temperature Chemistry

Tagami, Susumu; Sano, Naruto; Otobe, Haruyoshi; Akabori, Mitsuo; Kurobane, Shiro

JAEA-Technology 2010-034, 65 Pages, 2010/10

JAEA-Technology-2010-034.pdf:3.56MB

An experimental facility called the Module for TRU High Temperature Chemistry (TRU-HITEC) was installed in the Back-end Cycle Key Elements Research Facility (BECKY) of the Nuclear Fuel Cycle Safety Engineering Research Facility (NUCEF) in February, 2003. The main purpose of this facility is to perform the basic studies of the behavior the transuranium elements (TRU) in pyrochemical reprocessing and oxide fuels. Hot-experiment started in December, 2004. TRU-HITEC consists of three / cells and a glove box. This is the only facility in the country as large-scale facilities maintained a high purity argon gas atmosphere. The experience gained through the maintenance and improvement is useful also for the maintenance of similar designed facility. This report describes the maintenance method and improvement for the purpose of keeping the performance of TRU-HITEC.