Development of a theoretical scaling factor method for the inventory estimation of difficult-to-measure nuclide Cs-135 in fuel debris and radioactive wastes

坂本 雅洋; 奥村 啓介; 神野 郁夫; 松村 太伊知; 寺島 顕一; Riyana, E. S.; 金子 純一*; 溝上 暢人*; 溝上 伸也*

Journal of Nuclear Science and Technology, 62(8), p.756 - 765, 2025/08

https://doi.org/10.1080/00223131.2025.2478926

In this paper, we propose a new nuclide inventory estimation method based on computational methods, called a "theoretical scaling factor method" for difficult-to-measure (DTM) nuclides in fuel debris and radioactive wastes. The theoretical scaling factor method provides a method similar to a conventional scaling factor method. The theoretical scaling factor method, however, does not require performing many measurements to obtain correlations between a key nuclide which is easy-to-measure and a DTM nuclide. Instead of actual analytical measurements, the results of theoretical calculations are used. A correlation equation between the key nuclide and the DTM nuclide is created based on the results of theoretical calculations, and the DTM nuclide is deterministically estimated using the measurement value of the key nuclide only. In this paper, we selected Cs-135 as the DTM nuclide and Cs-137 as the key nuclide. Cs-135 has a long half-life of 2.310 years and is one of the important fission products in the safety evaluation for the geological disposal of high-level radioactive waste, because it dissolves and migrates in groundwater easily. We confirmed the validity of the proposed method using measured data of Cs-137 and Cs-135 on radioactive wastes from the Fukushima Daiichi Nuclear Power Station (1F) accident obtained by many researchers. It can be used as a rational and efficient technology to reduce the analysis costs of various types of fuel debris and radioactive waste present at 1F.

Characterization of neutrons emitted by an expected small amount of fuel debris in a trial retrieval from Fukushima Daiichi Nuclear Power Station

松村 太伊知; 奥村 啓介; 坂本 雅洋; 寺島 顕一; Riyana, E. S.; 近藤 千博*

Nuclear Engineering and Design, 432, p.113791_1 - 113791_9, 2025/02

https://doi.org/10.1016/j.nucengdes.2024.113791

Retrieving objects with a small amount of fuel debris, such as a few grams, will begin soon at the Fukushima Daiichi Nuclear Power Station (1F) at the start of decommissioning. Objects retrieved from the primary containment vessel are not necessarily fuel debris; fuel debris is an object from which neutrons are emitted because it contains nuclear-fuel material. However, the characteristics of the neutrons emitted by fuel debris are unknown. Fuel debris was categorized into five types according to the elapsed time from the accident, burnup, and fuel type (UO or mixed oxide). The number and energy spectra of (, ) and spontaneous fission neutrons emitted from 1 g of each fuel debris type were estimated using the SOURCES 4C code to obtain the neutron characteristics. The results showed that the average neutron energy is approximately 2.1 MeV, regardless of the type of fuel debris. However, the intensities of neutrons emitted from the fuel debris in 1F Units 2 and 3 varied by four orders of magnitude according to the fuel debris type.

Characterization of bremsstrahlung and -rays of fuel debris

松村 太伊知; 奥村 啓介; 藤田 学*; 坂本 雅洋; 寺島 顕一; Riyana, E. S.

Radiation Physics and Chemistry, 199, p.110298_1 - 110298_8, 2022/10

https://doi.org/10.1016/j.radphyschem.2022.110298

The characterization of bremsstrahlung and -rays from fuel debris differs from that of spent fuels evaluated to date, due to factors such as material composition and release of volatile fission products. In this work, in order to clarify the conditions under which the effect of bremsstrahlung compared to the total photons (bremsstrahlung and -rays) in fuel debris is maximized, the average energies and dose rates from the energy spectra of bremsstrahlung and -rays on the fuel debris surface were obtained using a Monte Carlo simulation. In the simulation, the average energies and dose rates were evaluated with consideration of the composition, size, fission product release, and retrieval time of the fuel debris. The simulation showed that the composition with the largest amount of change to the average total photons energy caused by bremsstrahlung was the molten fuel debris, and the composition with the maximum fraction of bremsstrahlung in the dose rate was the UO. The maximum value of the fraction of bremsstrahlung in the dose rate was evaluated to be about 17%. This work is expected to contribute to the prediction of the radiation characteristics of the fuel debris that will be retrieved from the Fukushima Daiichi Nuclear Power Station in the near future.

Depletion calculation of subcritical system with consideration of spontaneous fission reaction

Riyana, E. S.; 奥村 啓介; 坂本 雅洋; 松村 太伊知; 寺島 顕一

Journal of Nuclear Science and Technology, 59(4), p.424 - 430, 2022/04

https://doi.org/10.1080/00223131.2021.1974970

Modification of the Monte Carlo depletion calculation code OpenMC was performed to enable the depletion calculation of the subcritical neutron multiplying system. With the modified code, it became possible to evaluate the quantity of short half-life fission products from spontaneous and induced fissions in the subcritical system. As a preliminary study, it was applied to the fuel debris storage canister filled with nuclear materials and spontaneous fission nuclides. It was confirmed that the code could successfully provide a quantity of short half-life FPs over time and provide the relationship between the activity ratio of Kr-88 to Xe-135 and effective neutron multiplication factor of the canister.

Towards optimizing the performance of self-regenerating Pt-based perovskite catalysts

Jarrige, I.*; 石井 賢司; 松村 大樹; 西畑 保雄; 吉田 雅洋*; 岸 浩史*; 谷口 昌司*; 上西 真里*; 田中 裕久*; 笠井 秀明*; et al.

ACS Catalysis, 5(2), p.1112 - 1118, 2015/02

https://doi.org/10.1021/cs501608k

Self-regenerating automotive catalysts owe their remarkable performance to the repeated motion of the precious metal atoms in and out of the perovskite lattice under fluctuating oxidizing and reducing conditions, preventing coalescence of the metal nanoparticles. Here we use resonant inelastic X-ray scattering to characterize the occupied and unoccupied Pt 5d states in two self-regenerating Pt-perovskite catalysts, CaTiPtO and CaZrPtO. Upon reduction, the element and symmetry-specific charge excitation spectra reveal a sizeable hybridization between the Pt 5d and the Ti 3d or Zr 4d states at the interface between the nanoparticles and the perovskite, which involves the occupied states and is thus invisible in X-ray absorption spectra. A correlation is found between the strength of this d-band hybridization and the proportion of Pt nanoparticles that remain buried below the surface during reduction, indicating that the motion of the Pt atoms towards the surface is hindered by this hybridization specifically, rather than by the Pt-O bonding. These results provide direct evidence that the strength of the metal-metal d-band hybridization plays a pivotal role in determining the efficiency of self-regeneration in perovskite catalysts.

Magnetic structure determination of CeAl ( = Ru and Os); Single crystal neutron diffraction studies

加藤 治一*; 小林 理気; 竹坂 智明*; 西岡 孝*; 松村 政博*; 金子 耕士; 目時 直人

Journal of the Physical Society of Japan, 80(7), p.073701_1 - 073701_4, 2011/07

https://doi.org/10.1143/JPSJ.80.073701

Neutron diffraction studies of CeAl ( = Ru and Os), which shows an anomalous transition at K for CeRuAl and at 29 K for CeOsAl, have been carried out using single crystal samples. In the ordered state below , obvious superlattice reflections have been found, indicating the appearance of ordered magnetic moments. The magnetic structures of both compounds could be commonly explained with a propagation vector , where collinear antiferromagnetic moments with magnitudes of 0.42(1) for CeRuAl and of 0.29(1) for CeOsAl are aligned along the -axis.

A Cu NQR study in a -electron heavy-fermion system, CaCuRuO

加藤 治一*; 鶴田 拓也*; 西岡 孝*; 松村 政博*; 酒井 宏典; 神戸 振作

Journal of Physics and Chemistry of Solids, 68(11), p.2187 - 2190, 2007/11

https://doi.org/10.1016/j.jpcs.2007.08.038

f電子を含まない重い電子系化合物と考えられているCaCuRuOについてCu核の核四重極共鳴(NQR)を用いた研究を行った。Cu核NQRスペクトルは、ローレンツ型の曲線になっており、少なくとも5Kの低温まで、なんらの磁気秩序も示さないことを示唆する。Cu核のスピン格子核磁気緩和率は、Cuの3電子状態の変化を捉え、低温でフェルミ液体的挙動をすることがわかった。このことは、この系の重い電子描像を強く支持する。

地下水中の核種移行解析に用いるデータのまとめ

古賀 修; 長柄 収一; 松村 敏博; 竹内 章*; 武田 伸二; 山本 正博*; 佐藤 和彦

JNC TN6440 2004-003, 66 Pages, 2004/03

JNC-TN6440-2004-003.pdf:1.95MB

夜次露天採掘場跡地周辺及び夜次鉱さいたい積場周辺の精度の高い地下水流動解析及び核種移行解析を行うことを目的に、既往解析における課題を抽出するとともに、以下に示す対応方法の検討及び解析用物性値の整理を行った。

積算線量計を用いた燃料デブリの核燃料物質評価のための技術開発; バブル線量計の基礎データ取得

寺島 顕一; 冠城 雅晃; 坂本 雅洋; 松村 太伊知; 藤田 学*; 奥村 啓介

no journal, , 

中性子用積算線量計であるバブル線量計(BD)は、ガンマ線に不感、外部電源不要、目視確認が可能、中性子フルエンス率に応じた照射時間調整、などの特長を持っており、福島第一原子力発電所(1F)におけるデブリ検知や容器の非破壊測定への適用が期待できる。そこでBDの適用性評価を目的とし、中性子照射試験を行って基礎データを取得した。

燃料デブリから放出される中性子の特性評価

松村 太伊知; 坂本 雅洋; 寺島 顕一; Riyana, E. S.; 奥村 啓介

no journal, , 

これまでの原子炉格納容器(PCV)内部調査から、福島第一原子力発電所(1F)の1-3号機には、燃料と被覆管等が溶融した後に固化した燃料デブリが存在すると考えられている。2023年には、2号機(1F2)から数g程度の燃料デブリ試料の試験的取り出しが予定されている。燃料デブリの検知において中性子が検出されれば燃料デブリであると推定できるため、燃料デブリから放出される中性子の特性評価を行うことは重要である。そこで、UO燃料のみで構成されていた1F2と本格取出し時期での対象とされMOX燃料を部分的に含んでいた3号機(1F3)からの取出し燃料デブリに対する検出器開発や中性子応答の物理的解釈に資するため、1F2(広範囲燃焼度UO)、1F3(低燃焼度MOX)、TMI-2(低燃焼度UO)の3種類の代表的な燃料デブリモデルに対し、それぞれの燃焼履歴に基づく核種インベントリデータとSOURCES 4Cコードを用いて、燃料デブリから放出される自発核分裂(遅発中性子を含む)と(, n)反応によって放出される中性子の特性評価を行った。