Evaluation report for sludge measurement by nondestructive assay (Plutonium Scrap Multiplicity Counter)(Joint research)

Tanigawa, Masafumi; Seya, Kazuhito*; Asakawa, Naoya*; Hayashi, Hiroyuki*; Horigome, Kazushi; Mukai, Yasunobu; Kitao, Takahiko; Nakamura, Hironobu; Henzlova, D.*; Swinhoe, M. T.*; et al.

JAEA-Technology 2024-014, 63 Pages, 2025/02

JAEA-Technology-2024-014.pdf:3.02MB

The liquid waste treatment process generated sludge items at the plutonium conversion development facility. They are highly heterogeneous and contain large amounts of impurities (Na, Fe, Ni etc.). Therefore, the sludge items have very large sampling uncertainty and so the total measurement uncertainty is very large (approximately 24%). The plutonium scrap multiplicity counter (PSMC) measurement technique for sludge items was developed by joint research between the Japan Atomic Energy Agency (JAEA) and Los Alamos National Laboratory (LANL). The technical validity for sludge items using the PSMC was evaluated using various types of sample measurements and Monte Carlo N-Particle transport code calculations. The PSMC measurement parameters were found to be valid for use with sludge items and the validity of multiplicity analysis was confirmed and demonstrated through comparisons with standard MOX powder and a standard sludge. As a result, the PSMC measurement values were shown to be consistent and reasonable and the large amount of impurity (Fe, Ni etc.) did not impact the results. Therefore, the measurement uncertainty of the improved nuclear material accountancy (NMA) procedure by combined PSMC and high-resolution gamma spectrometry was shown to be 6.5%. In addition, an acceptance test was conducted using PSMC/HRGS and IAEA benchmark equipment. Measured Pu mass by both equipment agrees within the measurement uncertainty of each method, and so the validity for Pu mass measurement by PSMC/HRGS was confirmed. The above results confirm the applicability of PSMC/HRGS as an additional NMA method for sludge and a newly designed NDA procedure based on this study is applied to sludge for NMA in PCDF.

High temperature nanoindentation of (U,Ce)O compounds

Frazer, D.*; Saleh, T. A.*; Matsumoto, Taku; Hirooka, Shun; Kato, Masato; McClellan, K.*; White, J. T.*

Nuclear Engineering and Design, 423, p.113136_1 - 113136_7, 2024/07

https://doi.org/10.1016/j.nucengdes.2024.113136

Nanoindentation based techniques can be employed on minute volumes of material to measure mechanical properties, including Young's modulus, hardness, and creep stress exponents. In this study, (U,Ce)O solid solutions samples are used to develop elevated temperature nanoindentation and nanoindentation creep testing methods for use on mixed oxide fuels. Nanoindentation testing was performed on 3 separate (Ux-1,Cex)O compounds ranging from x equals 0.1 to 0.3 at up to 800 C: their Young's modulus, hardness, and creep stress exponents were evaluated. The Young's modulus decreases in the expected linear manner while the hardness decreases in the expected exponential manner. The nanoindentation creep experiments at 800 C give stress exponent values, n=4.7-6.9, that suggests dislocation motion as the deformation mechanism.

Nanoscale heterogeneity induced by nonmagnetic Zn dopants in the quantum critical metal CeCoIn; In NQR/NMR and Co NMR study

Sakai, Hironori; Tokunaga, Yo; Kambe, Shinsaku; Zhu, J.-X.*; Ronning, F.*; Thompson, J. D.*; Ramakrishna, S. K.*; Reyes, A. P.*; Suzuki, Kohei*; Oshima, Yoshiki*; et al.

Physical Review B, 104(8), p.085106_1 - 085106_12, 2021/08

https://doi.org/10.1103/PhysRevB.104.085106

Antiferromagnetism in a prototypical quantum critical metal CeCoIn is known to be induced by slight substitutions of non-magnetic Zn atoms for In. In nominally 7% Zn substituted CeCoIn, an antiferromagnetic (AFM) state coexists with heavy fermion superconductivity. Heterogeneity of the electronic states is investigated in Zn doped CeCoIn by means of nuclear quadrupole and magnetic resonances (NQR and NMR). Site-dependent NQR relaxation rates indicate that the AFM state is locally nucleated around Zn substituents in the matrix of a heavy fermion state, and percolates through the bulk at the AFM transition temperature . At lower temperatures, an anisotropic superconducting (SC) gap below the SC transition temperature , and the SC state permeates through the AFM regions via a SC proximity effect. Applying an external magnetic field induces a spin-flop transition near 5 T, reducing the volume of the AFM regions. Consequently, a short ranged inhomogeneous AFM state survives and coexists with a paramagnetic Fermi liquid state at high fields.

Final report on feasibility study of Pu monitoring and solution measurement of high active liquid waste containing fission product at Reprocessing Facility

Sekine, Megumi; Matsuki, Takuya; Suzuki, Satoshi*; Tsutagi, Koichi; Nishida, Naoki; Kitao, Takahiko; Tomikawa, Hirofumi; Nakamura, Hironobu; LaFleur, A.*; Browne, M.*

JAEA-Technology 2019-023, 160 Pages, 2020/03

JAEA-Technology-2019-023.pdf:9.43MB

The International Atomic Energy Agency (IAEA) has proposed in its Research and Development plan (STR-385), the development of technology to enable real-time flow measurement of nuclear material as a part of an advanced approach to effective and efficient safeguards for reprocessing facilities. To address this, Japan Atomic Energy Agency (JAEA) has been tackling development of a new detector to enable monitoring of Pu in solutions with numerous FPs as a joint research program with U.S. DOE to cover whole reprocessing process. In this study, High Active Liquid Waste (HALW) Storage Facility in Tokai Reprocessing Plant was used as the test field. At first, the design information of HALW storage tank and radiation (type and intensity) were investigated to develop a Monte Carlo N-Particle Transport Code (MCNP) model. And then, dose rate distribution outside/ inside of the concrete cell where the HALW tank is located was measured to design new detectors and check MCNP model applicability. Using the newly designed detectors, gamma rays and neutron were continuously measured at the outside/ inside of the concrete cell to assess the radiation characteristics and to optimize detector position. Finally, the applicability for Pu monitoring technology was evaluated based on the simulation results and gamma-ray/neutron measurement results. We have found that there is possibility to monitor the change of Pu amount in solution by combination both of gamma-ray and neutron measurement. The results of this study suggested the applicability and capability of the Pu motoring to enhance safeguards for entire reprocessing facility which handles Pu with FP as a feasibility study. This is final report of this project.

Systematic measurements and analyses for lead void reactivity worth in a plutonium core and two uranium cores with different enrichments

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

https://doi.org/10.1080/00295639.2019.1663089

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.

Pu nuclear magnetic resonance in the candidate topological insulator PuB

Dioguardi, A. P.*; Yasuoka, Hiroshi*; Thomas, S. M.*; Sakai, Hironori; Cary, S. K.*; Kozimor, S. A.*; Albrecht-Schmitt, T. E.*; Choi, H. C.*; Zhu, J.-X.*; Thompson, J. D.*; et al.

Physical Review B, 99(3), p.035104_1 - 035104_6, 2019/01

https://doi.org/10.1103/PhysRevB.99.035104

We present a detailed nuclear magnetic resonance (NMR) study of Pu in bulk and powdered single-crystal plutonium tetraboride (PuB), which has recently been investigated as a potential correlated topological insulator. The Pu NMR spectra are consistent with axial symmetry of the shift tensor showing for the first time that Pu NMR can be observed in an anisotropic environment and up to room temperature. The temperature dependence of the Pu shift, combined with a relatively long spin-lattice relaxation time (), indicate that PuB adopts a nonmagnetic state with gaplike behavior consistent with our density functional theory calculations. The temperature dependencies of the NMR Knight shift and imply bulk gaplike behavior confirming that PuB is a good candidate topological insulator.

CIELO collaboration summary results; International evaluations of neutron reactions on uranium, plutonium, iron, oxygen and hydrogen

Chadwick, M. B.*; Capote, R.*; Trkov, A.*; Herman, M. W.*; Brown, D. A.*; Hale, G. M.*; Kahler, A. C.*; Talou, P.*; Plompen, A. J.*; Schillebeeckx, P.*; et al.

Nuclear Data Sheets, 148, p.189 - 213, 2018/02

https://doi.org/10.1016/j.nds.2018.02.003

The CIELO collaboration has studied neutron cross sections on nuclides that significantly impact criticality in nuclear facilities - U, U, Pu, Fe, O and H - with the aim of improving the accuracy of the data and resolving previous discrepancies in our understanding. This multi-laboratory pilot project, coordinated via the OECD/NEA Working Party on Evaluation Cooperation (WPEC) Subgroup 40 with support also from the IAEA, has motivated experimental and theoretical work and led to suites of new evaluated libraries that accurately reflect measured data and also perform well in integral simulations of criticality. This report summarizes our results and outlines plans for the next phase of this collaboration.

Improvement of INVS measurement uncertainty for Pu and U-Pu nitrate solution

Swinhoe, M. T.*; Menlove, H. O.*; Marlow, J. B.*; Makino, Risa; Nakamura, Hironobu

LA-UR-17-23474, 28 Pages, 2017/04

https://doi.org/10.2172/1356101

The Inventory Verification Sample system (INVS) has been used for IAEA verification measurement at the Plutonium Conversion Development Facility for MOX powder and Pu solution samples (measurement uncertainty: about 3-5%). If the measurement uncertainty can be improved (to 1%), it is expected that the range of usage can be extended and it could reduce the number of destructive analyses. In order to improve the measurement uncertainty for solution samples, we conducted three different types of calibration method that are passive calibration curve method, known- method and multiplicity method after optimization of detector parameter and sample position. In the range of concentration of typical solution samples, a good correlation was found between measured doubles and Pu effective mass in the three methods. Especially, the result of the conventional calibration curve method and known- method met our target uncertainty within 1% (22 hours measurement). Since it is thought that background singles change may affect measurement uncertainty, an additional shielding was installed around the INVS to reduce those effects. This shielding improved measurement uncertainty in known- method. The results with this shielding suggests passive calibration method and known- method could achieve the target uncertainty within 1% less than 1 hour measurement time.

Field test and evaluation of He replacement technologies; Development of HLNB counter

Tanigawa, Masafumi; Mukai, Yasunobu; Nakamura, Hironobu; Kurita, Tsutomu; Henzlova, D.*; Menlove, H. O.*

Dai-37-Kai Kaku Busshitsu Kanri Gakkai Nihon Shibu Nenji Taikai Rombunshu (CD-ROM), 9 Pages, 2017/02

no abstracts in English

Feasibility study of advanced technology for Pu with FP solution monitoring; Overview of research plan and modelling for simulation

Sekine, Megumi; Matsuki, Takuya; Suzuki, Satoshi; Tanigawa, Masafumi; Yasuda, Takeshi; Yamanaka, Atsushi; Tsutagi, Koichi; Nakamura, Hironobu; Tomikawa, Hirofumi; LaFleur, A. M.*; et al.

EUR-28795-EN (Internet), p.788 - 796, 2017/00

https://esarda.jrc.ec.europa.eu/index.php?option=com_content&view=article&id=53&Itemid=204

The IAEA has proposed in its long-term R&D plan, the development of technology to enable real-time flow measurement of nuclear material as a part of an advanced approach to effective and efficient safeguards for reprocessing facilities. To address this, JAEA has designed and developed a neutron coincidence based nondestructive assay system to monitor Pu directly in solutions which is after purification process and contains very little fission products (FPs). A new detector to enable monitoring of Pu in solutions with numerous FPs is being developed as a joint research program with U.S. DOE at the High Active Liquid Waste (HALW) Storage Facility in Tokai Reprocessing Plant. As the first step, the design information of HALW tank was investigated and samples of HALW was taken and analyzed for Pu concentration and isotope composition, density, content of dominant nuclides emitting ray or neutron, etc. in order to develop a Monte Carlo N-Particle Transport Code (MCNP) of the HALW tank. In addition, ray source spectra simulated by Particle and Heavy Ion Transport code System (PHITS) was developed by extracting peaks from the analysis data with germanium detector. These outputs are used for the fundamental data in the MCNP model which is then used to evaluate the type of detector, shielding design and measurement positions. In order to evaluate available radiations to measure outside the cell wall, continuous ray and neutron measurement were carried out and the results were compared to the simulation results. The measurement results showed that there are no FP peaks above 3 MeV. This paper presents an overview of the research plan, characteristics of HALW, development of source term for MCNP, simulation of radiation dose from the HALW tank and radiation measurement results at outside of cell wall.