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

古高 和禎; 大図 章; 藤 暢輔

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

https://doi.org/10.1016/j.net.2023.07.015

An integrated neutron interrogation system has been developed for non-destructive assay of highly radioactive special nuclear materials, to accumulate knowledge of the method through developing and using it. The system combines a differential die-away (DDA) measurement system for the quantification of nuclear materials and a prompt gamma-ray analysis (PGA) system for the detection of neutron poisons which disturb the DDA measurements; a common D-T neutron generator is used. A special care has been taken for the selection of materials to reduce the background gamma rays produced by the interrogation neutrons. A series of measurements were performed to test the basic performance of the system. The results show that the DDA system can quantify plutonium of as small as 20~mg and it is not affected by intense neutron background up to 4.2~TBq and gamma ray of 2.2~TBq. As a result of the designing of the combined system as a whole, the gamma-ray background counting rate at the PGA detector was reduced down to s even with the use of the D-T neutron generator. The test measurements show that the PGA system is capable of detecting less than 1~g of boron compound and about 100~g of gadolinium compound in~30 min. This research was implemented under the subsidy for nuclear security promotion of MEXT.

Oxygen potential of neodymium-doped UPuAmO uranium-plutonium-americium mixed oxides at 1573, 1773, and 1873 K

Vauchy, R.; 砂押 剛雄*; 廣岡 瞬; 中道 晋哉; 村上 龍敏; 加藤 正人

Journal of Nuclear Materials, 580, p.154416_1 - 154416_11, 2023/07

https://doi.org/10.1016/j.jnucmat.2023.154416

Oxygen potentials of UPuAmO incorporating 10 and 20 mol% of neodymium (Nd/Metal) were investigated by thermogravimetry at 1573, 1773, and 1873 K. The presence of neodymium induced an increase in the oxygen potential of the U-Pu mixed oxide. The correlation between oxygen partial pressure pO and deviation from stoichiometry x was analyzed, and a model of defect chemistry was proposed. Finally, the crystal structure of these mixed oxides was discussed at the light of the mechanisms of possible Nd(III)/U(V) charge compensation, and deviation from stoichiometry.

HTTR1次ヘリウム循環機フィルタの差圧上昇事象,1; 差圧上昇事象の原因調査

根本 隆弘; 荒川 了紀; 川上 悟; 長住 達; 横山 佳祐; 渡部 雅; 大西 貴士; 川本 大樹; 古澤 孝之; 猪井 宏幸; et al.

JAEA-Technology 2023-005, 33 Pages, 2023/05

JAEA-Technology-2023-005.pdf:5.25MB

HTTR (High Temperature engineering Test Reactor) RS-14サイクルの原子炉出力降下において、ヘリウムガス循環機のフィルタ差圧が上昇傾向となった。この原因を調査するため、1次ヘリウム純化設備のガス循環機の分解点検等を実施した結果、ガス循環機内のシリコンオイルミストがチャコールフィルタの性能低下で捕集できなくなり、1次系統に混入したためと推定された。今後は、フィルタ交換を実施するとともに、さらなる調査を進め、再発防止対策を策定する予定である。

Applicability of differential die-away self-interrogation technique for quantification of spontaneous fission nuclides for fuel debris at Fukushima Daiichi Nuclear Power Plants

長谷 竹晃; 相樂 洋*; 小菅 義広*; 能見 貴佳; 奥村 啓介

Journal of Nuclear Science and Technology, 60(4), p.460 - 472, 2023/04

https://doi.org/10.1080/00223131.2022.2114958

This paper provides an overview of the applicability of the Differential Die-Away Self-Interrogation (DDSI) technique for quantification of spontaneous fissile nuclides in fuel debris at the Fukushima Daiichi Nuclear Power Plants. In this research, massive fuel debris stored in a canister was evaluated, and the void space of the canister was assumed to be filled with water for wet storage and air for dry storage. The composition of fuel debris was estimated based on elements such as the inventory in the reactor core and operation history. The simulation results show that for wet storage, the DDSI technique can properly evaluate the neutron leakage multiplication and quantify spontaneous fissile nuclides with a total measurement uncertainty (TMU) of approximately 8%. For dry storage, the known-alpha technique, which was previously established, can be applied to quantify spontaneous fissile nuclides with a TMU of approximately 4%. In both cases, the largest uncertainty factor is the variation in water content in the canister. In the case of wet storage, the uncertainty could be significantly increased in cases where the fuel debris is extremely unevenly distributed in the canister.

Evolution of the reaction and alteration of granite with Ordinary Portland cement leachates; Sequential flow experiments and reactive transport modelling

Bateman, K.*; 村山 翔太*; 花町 優次*; Wilson, J.*; 瀬田 孝将*; 天野 由記; 久保田 満*; 大内 祐司*; 舘 幸男

Minerals (Internet), 12(7), p.883_1 - 883_20, 2022/07

https://doi.org/10.3390/min12070883

The construction of a repository for geological disposal of radioactive waste will include the use of cement-based materials. Following closure, groundwater will saturate the repository and the extensive use of cement will result in the development of a highly alkaline porewater, pH 12.5; this fluid will migrate into and react with the host rock. The chemistry of the fluid will evolve over time, initially high [Na] and [K], evolving to a Ca-rich fluid, and finally returning to the groundwater composition. This evolving chemistry will affect the long-term performance of the repository, altering the physical and chemical properties, including radionuclide behaviour. Understanding these changes forms the basis for predicting the long-term evolution of the repository. This study focused on the determination of the nature and extent of the chemical reaction, as well as the formation and persistence of secondary mineral phases within a granite, comparing data from sequential flow experiments with the results of reactive transport modelling. The reaction of the granite with the cement leachates resulted in small changes in pH and the precipitation of calcium aluminum silicate hydrate (C-(A-)S-H) phases of varying compositions, of greatest abundance with the Ca-rich fluid. As the system evolved, secondary C-(A-)S-H phases re-dissolved, partly replaced by zeolites. This general sequence was successfully simulated using reactive transport modelling.

Correction method of measurement volume effects on time-averaged statistics for laser Doppler velocimetry

和田 裕貴; 古市 紀之*; 辻 義之*

European Journal of Mechanics B, Fluids, 91, p.233 - 243, 2022/01

https://doi.org/10.1016/j.euromechflu.2021.10.007

A new correction method of LDV (Laser Doppler Velocimetry) measurement volume effects on the time-averaged velocity statistics is proposed by considering the PDF (Probability Density Function) of streamwise fluctuating velocity and the streamwise cross-sectional area of the measurement volume. It is fundamentally different from the previous method using a laser intensity profile of LDV. We propose a simple equation to correct the measurement volume effects. Using this equation and calculating precisely both the measurement locations and the measurement volume, the correction of measurement volume effects on the time averaged statistics can be performed based on the LDV measurement data. From a comparison with correction method proposed by Durst et al. (1995), the present correction method provides almost same result with Durst method, and then the validity and applicability to higher Reynolds number or lower spatial conditions of two correction methods are confirmed.

A Theoretical investigation on the intermolecular potential curve between ruthenium tetroxide and NO (X = 1, 2)

城戸 健太朗

International Journal of Quantum Chemistry, 121(21), p.e26781_1 - e26781_15, 2021/11

https://doi.org/10.1002/qua.26781

Ruthenium tetroxide (RuO) is one of chemical species of fission products assumed to be released to the environment during a severe accident of nuclear facilities and a target compound to assess the amount produced, reactivity, mobility and release timing. In this article, the NO (X = 1, 2) adduct formation of RuO has been investigated, based on the potential energy curve (PEC) evaluated by UM06, UTPSSh, CASSCF, and CASPT2 methods. At several stationary points, CCSD and LR-CCSD(T) energies are also computed for a comparison. The PEC shows that there is an activation barrier to form the NO adduct and that the process is endothermic in terms of free energy. In the system, the electron transfer occurs from NO to RuO when the bond between the nitrogen and oxo ligand is formed. It has been discussed in detail using active orbitals, weight of electron configurations and spin population obtained by CASSCF.

Energy-dependent angular distribution of individual rays in the La()La reaction

奥平 琢也*; 遠藤 駿典; 藤岡 宏之*; 広田 克也*; 石崎 貢平*; 木村 敦; 北口 雅暁*; 古賀 淳*; 新實 裕大*; 酒井 健二; et al.

Physical Review C, 104(1), p.014601_1 - 014601_6, 2021/07

https://doi.org/10.1103/PhysRevC.104.014601

Neutron energy-dependent angular distributions were observed for individual rays from the 0.74 eV -wave resonance of La+ to several lower excited states of La. The -ray signals were analyzed in a two dimensional histogram of the -ray energy, measured with distributed germanium detectors, and neutron energy, determined with the time-of-flight of pulsed neutrons, to identify the neutron energy dependence of the angular distribution for each individual rays. The angular distribution was also found for a photopeak accompanied with a faint -wave resonance component in the neutron energy spectrum. Our results can be interpreted as interference between - and -wave amplitudes which may be used to study discrete symmetries of fundamental interactions.

Oxygen potential measurement of (U,Pu,Am)O and (U,Pu,Am,Np)O

廣岡 瞬; 松本 卓; 加藤 正人; 砂押 剛雄*; 宇野 弘樹*; 山田 忠久*

Journal of Nuclear Materials, 542, p.152424_1 - 152424_9, 2020/12

https://doi.org/10.1016/j.jnucmat.2020.152424

(UPuAm)Oに対しては1,673, 1,773, 1,873K、(UPuAmNp)Oに対しては1,873, 1,973Kにおいて、酸素ポテンシャルの測定を実施した。測定は、熱天秤と酸素センサーを用いる気相平衡法により実施した。Uの代わりにAmを添加した場合、酸素ポテンシャルは大きく上昇した。同様に、Uの代わりにNpを添加した場合も酸素ポテンシャルは上昇したが、上昇の効果はPuやAmを添加した場合と比べても小さいものであった。酸素ポテンシャルの測定結果について、酸素分圧と定比組成からのずれをプロットし、欠陥化学により解析することで、欠陥反応の種類を推定した。推定した欠陥反応における平衡定数を評価し、AmとNpを平衡定数の中のエントロピーに組み込むことで、酸素ポテンシャルの測定結果を再現する評価式を導出した。

Investigation of high-temperature chemical interaction of calcium silicate insulation and cesium hydroxide

Rizaal, M.; 中島 邦久; 斉藤 拓巳*; 逢坂 正彦; 岡本 孝司*

Journal of Nuclear Science and Technology, 57(9), p.1062 - 1073, 2020/09

https://doi.org/10.1080/00223131.2020.1755733

福島第一原子力発電所2号機においてペデスタル内よりもペデスタル外で線量が高くなっている現象が見つかっている。この線量の上昇については、原子炉格納容器内の配管に使用されている保温材(ケイ酸カルシウム)がガス状あるいは粒子状となって沈着したセシウム(Cs)と化学反応を起こして固着するとともに破損してペデスタル外に堆積することで線量が上昇した可能性があると考えている。そこで、本研究では、化学反応の有無を調べるため、反応温度等を調べることのできる熱重量示差熱分析装置(TG-DTA)を用いて、水素-水蒸気含有雰囲気下、最高1100Cまで温度を上昇させて、主なセシウム化合物の一つである水酸化セシウムと保温材との混合物に対して分析を行った。その結果、575-730Cの範囲で反応が起こり、試験後試料のX線回折パターンや元素分析機能付き走査型電子顕微鏡(SEM/EDS)による試料表面の元素分布の結果から、保温材の構成物質であるケイ素(Si)に加え、不純物として含まれるアルミニウム(Al)と安定な化合物(CsAlSiO)を形成することが分かった。したがって、ペデスタル外で見つかった高線量の原因として、保温材が関係する可能性があることが分かった。