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論文

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

 被引用回数:0

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 $$pm$$ 0.8 kJ mol$$^{-1}$$ and a frequency factor of 1.8 $$times$$ 10$$^{7}$$ s$$^{-1}$$. These findings will enable the numerical simulation of the hydrogen release behavior in SFRs.

論文

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

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.

論文

放射性硫化水素ガス(H$$_{235}$$S)に対する活性炭素繊維フィルタの捕集効率の評価法

神永 博史; 梶本 与一; 大貫 孝哉; 遠藤 章; 池沢 芳夫

保健物理, 29, p.189 - 194, 1994/00

RI製造施設で製造されている放射性硫黄($$^{35}$$S)の製造廃液を貯留しているタンク内の空気中に$$^{35}$$Sによる比較的高いレベルの汚染が発生し、排気筒から放出された。$$^{35}$$Sの化学形はガスクロマトグラフ分析の結果、硫化水素(H$$_{2}$$S)であった。H$$_{235}$$Sガスの放射能濃度は活性炭素繊維フィルタで捕集し、評価しているが、フィルタの捕集効率が未知であった。このためH$$_{235}$$Sガスに対し捕集放射能のフィルタ内での分布に関する仮定と$$^{35}$$S-$$beta$$線の自己吸収を仮定し、1枚のフィルタだけで、その後面と前面の計数率の比を指標として捕集効率を評価する方法を開発した。さらに、H$$_{235}$$Sガスの捕集・実測実験によりフィルタの捕集効率を求め、捕集効率評価方法の妥当性について検討した。また、脱着率に関する測定実験結果について報告する。

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