Thermal analysis of the hydrogen release behavior of sodium hydride and kinetic analysis using master plot methods

土井 大輔

International Journal of Hydrogen Energy, 91, p.1245 - 1252, 2024/11

https://doi.org/10.1016/j.ijhydene.2024.10.227

Hydrogen is a major nonmetallic impurity in the coolant of sodium-cooled fast reactors (SFRs) during normal operation. A higher hydrogen concentration than the gas-liquid equilibrium has been transiently detected in the gas space of actual SFR plants. The presence of several sodium compounds can increase hydrogen generation; however, a thorough understanding of the thermal behavior of candidate reactions is lacking. Herein, thermal analysis reveals the hydrogen release behavior of sodium hydride. Mass spectrometry indicates hydrogen generation with decreasing sample mass, indicating thermal decomposition. Detailed kinetic analysis based on master plot methods indicates that the hydrogen release reaction occurred through a mechanism involving random nucleation and growth of nuclei. Furthermore, the reaction rate was newly formulated based on a kinetic model function representing the above mechanism and the Arrhenius-type reaction rate constant comprising an activation energy of 119.0 0.8 kJ mol and a frequency factor of 1.8 10 s. These findings will enable the numerical simulation of the hydrogen release behavior in SFRs.

Measurements of capture cross-section of Nb by activation method and half-life of Nb by mass analysis

中村 詔司; 芝原 雄司*; 遠藤 駿典; 木村 敦

Journal of Nuclear Science and Technology, 60(11), p.1361 - 1371, 2023/11

https://doi.org/10.1080/00223131.2023.2198526

廃止措置の対象核種の中からNbについて、熱中性子捕獲断面積()および共鳴積分(I)を放射化法により測定した。また、Nbの半減期を質量分析により測定した。ニオブ93試料は、京都大学複合原子力科学研究所の研究炉に整備されている水圧輸送艦を用いて照射した。金-アルミ合金線、およびコバルト-アルミ合金線を用いて、照射位置における中性子束成分を測定した。厚さ25mのガドリニウム箔を用いた照射も行って、熱および熱外中性子による反応率の寄与をより分けた。ガドリニウムの厚さから、カットオフ・エネルギーは0.133eVに設定した。ニオブ試料中に含まれている不純物により生成されるTaの放射能を減衰させるために、約2年間ニオブ試料を冷却した。線スペクトロスコピーにより照射されたニオブ試料およびモニタの生成放射能を測定した。Westcottコンベンションに基づいて解析を行い、およびIを、それぞれ1.110.04barnおよび10.50.6barnと導出することができた。線測定の後に、ニオブ試料の質量分析を行い、反応率を導出した。線スペクトロスコピーと質量分析で得られたデータを組み合わせることにより、Nbの半減期を、(2.000.15)10年と導出することができた。

Hydrogen release reaction from sodium hydride with different sample quantities

土井 大輔

Proceedings of 29th International Conference on Nuclear Engineering (ICONE 29) (Internet), 7 Pages, 2022/08

https://doi.org/10.1115/ICONE29-91847

In sodium-cooled fast reactors (SFRs), hydrogen is a major nonmetallic impurity in the coolant during normal operation. A higher hydrogen concentration than the gas-liquid equilibrium had been transiently detected in the gas space of the actual SFR plant. However, the chemical reactions that caused hydrogen generation, which involve several sodium compounds, have not been identified. Furthermore, the thermal behavior of these hydrogen release reactions has not been thoroughly investigated. In this study, the hydrogen release behavior of sodium hydride, which could be involved in all of these reactions, was clarified by two experimental methods dealing with different sample quantities. In the thermal analysis with a semi-micro sample of about 1mmol, the hydrogen generation was demonstrated by mass spectrometry as the sample mass decreased, suggesting thermal decomposition. A monomodal hydrogen release curve similar to the thermal analysis result was obtained in the heating experiment with a macro amount sample of about 1mol. These experimental results showed consistent activation energies within the standard error. Therefore, it was elucidated that the ideal reaction behavior obtained by thermal analysis could be sufficiently extrapolated to the reaction behavior occurring in a larger amount of sample. These findings provide fundamental insights into the thermal decomposition of sodium hydride and are indispensable for analyzing hydrogen release behavior in other hydrogen release reactions involving sodium hydride.

Plasticity correction on stress intensity factor evaluation for underclad cracks in reactor pressure vessels

Lu, K.; 勝山 仁哉; Li, Y.

Journal of Pressure Vessel Technology, 142(5), p.051501_1 - 051501_10, 2020/10

https://doi.org/10.1115/1.4046977

Structural integrity assessment of reactor pressure vessels (RPVs) is essential for the safe operation of nuclear power plants. For RPVs in pressurized water reactors (PWRs), the assessment should be performed by considering neutron irradiation embrittlement and pressurized thermal shock (PTS) events. To assess the structural integrity of an RPV, a traditional method is usually employed by comparing fracture toughness of the RPV material with the stress intensity factor () of a crack postulated near the RPV inner surface. When an underclad crack (i.e., a crack beneath the cladding of an RPV) is postulated, of this crack can be increased owing to the plasticity effect of cladding. This is because the yield stress of cladding is lower than that of base metal and the cladding may yield earlier than base metal. In this paper, detailed three-dimensional (3D) finite element analyses (FEAs) were performed in consideration of the plasticity effect of cladding for underclad cracks postulated in Japanese RPVs. Based on the 3D FEA results, a plasticity correction method was proposed on calculations of underclad cracks. In addition, the effects of RPV geometries and loading conditions were investigated using the proposed plasticity correction method. Moreover, the applicability of the proposed method to the case which considers the hardening effect of materials after neutron irradiation was also investigated. All of these results indicate that the proposed plasticity correction method can be used for calculations of underclad cracks and is applicable to structural integrity assessment of Japanese RPVs containing underclad cracks.

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。

Thermal-hydraulic analysis of the LBE spallation target head in JAEA

Wan, T.; 大林 寛生; 佐々 敏信

Nuclear Technology, 205(1-2), p.188 - 199, 2019/01

https://doi.org/10.1080/00295450.2018.1478591

To perform basic research and development to realize future accelerator-driven systems, a lead-bismuth eutectic (LBE) alloy spallation target will be installed within the framework of the Japan Proton Accelerator Research Complex (J-PARC) project, Japan Atomic Energy Agency. The target will be bombarded by high-power pulsed proton beams (250 kW, 400 MeV, 25 Hz, and 0.5 ms in pulse duration). The Beam Window (BW) of the spallation target is critical because it should survive under severe conditions that occur, i.e., high temperature, high irradiation, intense stress, and various kinds of damage. Therefore, the target vessel should be carefully designed to obtain an adequate safety margin. Our previous research indicates that there is a stagnant flow region in the LBE at the BW tip due to the symmetric configuration of the target, which causes high temperature and concentration of stress on the BW. On the basis of our previous work, three types of upgraded target head designs are studied in the current research to reduce/move the stagnant flow region from the BW tip and to increase the target safety margin. Thermal-hydraulic analyses and structural analyses for the target head designs are carried out numerically under a steady-state condition. Results illustrate that the designs can almost eliminate the stagnant flow region in the LBE. As a consequence, the concentration of thermal stress on the BW is released and greatly decreased. The safety margin of the target is improved through this study.

Study on the thermal-hydraulic of TEF-T LBE spallation target in JAEA

Wan, T.; 大林 寛生; 佐々 敏信

Proceedings of 17th International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH-17) (USB Flash Drive), 13 Pages, 2017/09

To realize the future Accelerator-driven systems (ADSs), an ADS Target Test Facility (TEF-T) will be constructed within the framework of Japan Proton Accelerator Research Complex (J-PARC) project to carry out basic R&Ds. A LBE spallation target will be installed in the TEF-T facility and be bombarded by high power pulsed proton beams (250 kW, 400 MeV, 25 Hz, 0.5 ms in pulse duration). The beam window (BW) of the spallation target is critical because it should survive under severe conditions, i.e., high temperature, high irradiation, intense stress and various occurred damage. Therefore, the target vessel should be carefully designed to obtain enough safety margin. Our previous research indicated that there are stagnant flow region in LBE at the BW tip due to the symmetric configuration of target, which causes high temperature and stress concentration on the BW. To reduce/move the stagnant flow region from BW tip and to increase the target safety margin, on the basis of our previous work, three types of upgraded target head designs were performed steadily in the present study. The thermal-hydraulic analyses and structural analyses for the target head designs have been carried out numerically under a steady-state condition. Results illustrated that the designs can almost eliminate the stagnant flow region in LBE. As a consequence, the thermal stress concentration on BW has been released and greatly decreased. The safety margin of target has been improved through this study.

Thermal mixing characteristics of helium gas in high-temperature gas-cooled reactor, 1; Thermal mixing behavior of helium gas in HTTR

栃尾 大輔; 藤本 望

Journal of Nuclear Science and Technology, 53(3), p.425 - 431, 2016/03

https://doi.org/10.1080/00223131.2015.1054910

JAEAでは、将来型高温ガス炉の設計を行っている。この原子炉には異なる温度のヘリウムガスの合流点が多くある。構造物健全性又は温度制御の観点から高温ガス炉の配管内におけるヘリウムガスの混合特性を明らかにする必要がある。過去にHTTRで、ヘリウムガスの混合が十分でないことにより、原子炉入口温度が目標値より低くなるよう制御されていた。現在、この制御系は原子炉入口ヘリウムガスの混合平均温度を使った制御方法へと改良されている。本論文は、HTTRの1次系におけるヘリウムガスの混合挙動を明らかにするために、熱流動解析を行った。その結果、1次系におけるヘリウムガスの混合挙動は主に環状部流路のアスペクト比に影響を受け、高温ガス炉の配管設計では混合特性を考慮する必要があることが分かった。

鉛ビスマス冷却加速器駆動核変換システム用熱設計解析コードの整備

秋本 肇

JAEA-Data/Code 2014-031, 75 Pages, 2015/03

JAEA-Data-Code-2014-031.pdf:37.23MB

鉛ビスマス冷却加速器駆動核変換システム(ADS)の熱設計解析に資するため、軽水炉過渡解析コードJ-TRACをコードの骨組みとして、ADS用熱設計解析コードを整備した。軽水炉, ナトリウム冷却高速炉に対する安全解析及びこれまで行われたADSに対する熱流動解析を対象としてADS用熱設計解析コードに必要な解析機能を摘出した。J-TRACコードに不足する解析機能を追加するため、鉛ビスマス共晶合金(LBE), アルゴンガス, 窒化物燃料の物性値ルーチン並びに液体金属に対する強制対流領域における壁面熱伝達率相関式をJ-TRACコードに組み込んだ。LBE単相流の圧力損失解析、窒化物燃料集合体の熱伝達解析、及び蒸気発生器熱伝達解析を行い、追加した解析機能が所期の通りにJ-TRACコードに組み込めていることを確認した。

Large-scale direct simulation of two-phase flow structure around a spacer in a tight-lattice nuclear fuel bundle

高瀬 和之; 吉田 啓之; 小瀬 裕男*; 秋本 肇

Computational Fluid Dynamics 2004, p.649 - 654, 2006/00

日本原子力研究開発機構が研究を進めている革新的水冷却炉は減速材の割合を減らして中性子の減速を抑制することで高い転換比が期待できる原子炉であり、炉心には直径13mm程の燃料棒が1mm程度の燃料棒間ギャップ幅で三角ピッチ状に稠密に配置される。このような狭隘流路内の二相流挙動を高温高圧の原子炉条件下で詳細に計測することは困難であることから、著者らは実験データを必要としないシミュレーションだけによる評価法の開発を行っている。本論文では、革新的水冷却炉の炉心燃料集合体1カラム内二相流を対象にして、超高性能計算機による大規模シミュレーションの結果を示す。本研究によって、燃料集合体内の狭隘流路に設置されるスペーサまわりの気相と液相の挙動や燃料棒外表面を薄膜状に流れる液膜挙動などが定量的に明らかになるとともに、シミュレーションを主体とした炉心熱設計手法の実現に対して高い見通しが得られた。