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under high temperatures and various water vapor concentrationsMohamad, A. B.; 中島 邦久; 井元 純平*; 高野 公秀
Journal of Nuclear Materials, 631, p.156826_1 - 156826_12, 2026/09
被引用回数：0It is estimated that considerable amounts of Cs remain in the reactors at the Fukushima Daiichi nuclear power plant and may react with the reactor materials such as UO fuel as reported by our previous paper. In order to understand the chemisorption behavior of CsOH vapor on UO fuel, chemisorption tests between CsOH vapor on UO under different water vapor concentrations and temperatures were performed. As predicted by the thermodynamic analysis, the experimental result indicated that, under the poor water vapor condition, chemisorption to form CsUO
occurred even at 1273 K. On the other hand, as predicted by the thermodynamic analysis, the experimental result indicated that, under the rich water vapor condition, chemisorption to form CsUO
occurred at 1273 K and 1473 K. Therefore, this study demonstrates the crucial role of thermodynamics in predicting the conditions under which chemisorption occurs. In addition, it was suggested that the chemisorption rate of CsOH vapor on UO pellet was considerably higher than that onto type 304 stainless steel.
中島 邦久; 井元 純平*; 西岡 俊一郎*; 逢坂 正彦; 三輪 周平
Journal of Nuclear Science and Technology, 63(6), p.727 - 736, 2026/06
被引用回数：0 パーセンタイル：0.00(Nuclear Science & Technology)ステンレス鋼に化学吸着されたセシウム(Cs)の長期的な溶解挙動を調べるため、303Kでの水浸出試験を実施した。その結果、Csは1200時間経過後も水に溶解し続け、Csはリング状粒子としてケイ素と共存していることがわかった。このことから、既存のシビアアクシデント解析コードに組み込まれているCsの化学吸着モデルで定義されている水不溶性Csでさえ、リング状のCsケイ酸塩粒子から長期間にわたってCsが水に溶出することが明らかとなった。さらに、これらの水浸出挙動については、Noyes-Whitneyの式でうまく記述できたことから化学吸着モデルにおける水不溶性Csの水溶解モデルの開発につながる可能性を示唆した。これらの知見から、福島第一原子力発電所の原子炉圧力容器内で化学吸着したCsについては、長期的な再分布が起こる可能性があることを意味しており、水相を介したCsの再分布を予測するための水溶解モデルが必要になることが分かった。
Mohamad, A. B.; 山下 真一郎; 根本 義之; 阿部 陽介; Pham, V. H.; 井岡 郁夫; 相馬 康孝; 石島 暖大; 佐藤 智徳; Rizaal, M.; et al.
Proceedings of TopFuel 2025; Nuclear Reactor Fuel Performance Conference (Internet), 8 Pages, 2025/10
In parallel with the Advanced Technology Fuel (ATF) development program in Japan, Japan Atomic Energy Agency has established an R&D program on the ATF to provide more scientific support to the ATF fuel vendors in Japan. Based on the identified phenomenological issues, the R&D program covers the issues mainly on the light water reactors conditions such as normal operation, loss of coolant accident, beyond design basis accident, and severe accident. The R&D program such as irradiation test, corrosion test, LOCA test, and etc. are proposed. By acquiring the data from the experiment, the final goal is to implement the experimental data and model into the simulation code in order to predict the fuel performance behaviour at high burn-up. In 2024 TOPFUEL, the introduction of the R&D has been presented. In 2025, the update on the Cr-coated research to simulate normal operation and accident conditions will be given. For example, tests are currently underway to understand the in-reactor environment, such as ion irradiation, gamma irradiation and proton irradiation tests. In addition, a loss-of-coolant accident is being simulated for accident conditions, and the chemical effects of fission products on the cladding are being studied.
Rizaal, M.; 中島 邦久; 鈴木 恵理子; 三輪 周平
Annals of Nuclear Energy, 218, p.111433_1 - 111433_10, 2025/08
被引用回数：1 パーセンタイル：50.28(Nuclear Science & Technology)The release of iodine in a case of severe nuclear accident is directly linked to short-term radiological consequences. This concern raises issues in understanding the chemical forms of the transported iodine to devise proper accident management measures/strategies. In contributing to such efforts, this work presents experimental and theoretical approaches to defining the impact of molybdenum as a semi-volatile fission product toward iodine speciation in the gas phase. Given humid atmospheric conditions with different oxygen potentials, the interactions were revealed through the reaction products consisting of both gas and aerosols upon their transport and condensation in the temperature range of 1150-450 K. Through thermodynamic equilibrium calculations where new thermodynamic data of cesium molybdates have been incorporated, the experimental observation was reproduced, hence general interaction mechanism was proposed in this work.
and Fe-Zr melt中島 邦久; 高野 公秀
Journal of Nuclear Science and Technology, 62(1), p.78 - 85, 2025/01
被引用回数：4 パーセンタイル：55.60(Nuclear Science & Technology)1Fでは、シビアアクシデント解析コードを用いた解析や汚染水からの逆解析により相当量のCsが炉内にまだ残っていると推定されている。そのため、炉心領域で想定されるCs蒸気とUOあるいはFe-Zr融体との化学的な相互作用の有無を調べた。その結果、CsUOやCsZrO
の生成が確認され、燃料から放出されたCsがUO燃料やFe-Zr融体と化学的な相互作用により付着する可能性があることが分かった。
-CsOHRizaal, M.; Luu, V. N.; 中島 邦久; 三輪 周平
Proceedings of International Topical Workshop on Fukushima Decommissioning Research 2024 (FDR2024) (Internet), 4 Pages, 2024/10
Thermochemistry prevailing between gaseous CsOH and concrete main chemical phase CaCO at temperatures up to 570
C was investigated with various scenarios using the thermogravimetric method. The aim was to elucidate the decreasing behavior of cesium (Cs) trapping on CaCO observed in the transpiration method. A quasi-two-compartment platinum crucible was developed to realize co-measurements of both CsOH and CaCO during thermal treatment. Post-test X-ray diffraction was conducted to identify the chemical compound formed on the CaCO precursor. The early presence (timely sensitivity) of CsOH near the heated surface of CaCO was found to play a key role in the trapping (in the form of CsCO). Such a factor is crucial because, otherwise, the Ca(OH) would predominate the surface upon CaCO decomposition where leading to no reaction with CsOH.
Luu, V. N.; 中島 邦久; Rizaal, M.; 三輪 周平
Proceedings of International Topical Workshop on Fukushima Decommissioning Research 2024 (FDR2024) (Internet), 4 Pages, 2024/10
The trapping behavior of cesium (Cs) on concrete, such as pedestal and shield plugs, was assessed through multiple deposition tests of CsOH aerosols on concrete phase-CaCO within a temperature range of 170C to 570C under humid conditions. The deposition rate of CsOH aerosols on CaCO as a function of temperature was examined. X-ray diffraction analysis revealed the presence of water-soluble CsCO on CaCO samples up to 420C, but negligible detection above this temperature. This finding is supported by quantitative analyses of Cs weight gain and chemical analysis, demonstrating an increase in deposition rate up to 420C, followed by a decline thereafter. The increased deposition rate is attributed to the chemical interaction between CsOH and CaCO, while the diminished rate beyond 420C may result from the decomposition of CaCO under steam, thereby reducing the available reactant for the chemical reaction with CsOH.
Mohamad, A. B.; 相馬 康孝; 根本 義之; 阿部 陽介; 井岡 郁夫; 佐藤 智徳; 石島 暖大; 三輪 周平; 中島 邦久; 山下 真一郎; et al.
Proceedings of TopFuel 2024 (Internet), 8 Pages, 2024/10
In parallel with the Accident Tolerant Fuel development program in Japan, Japan Atomic Energy Agency has established an R&D program on the ATF to provide more scientific support to the ATF fuel vendors in Japan. Based on the phenomenological issues identified, the R&D program covers the issues mainly on the light water reactors conditions such as normal operation, loss of coolant accident, beyond design basis accident, and severe accident. The R&D program such as irradiation test, corrosion test, LOCA test, and etc. are proposed. By acquiring the data from the experiment, the final goal is to implement the experimental data and model into the simulation code in order to predict the fuel performance behaviour at high burn-up.
Rizaal, M.; 中島 邦久
Chemosphere, 363, p.142870_1 - 142870_9, 2024/09
Retention or trapping of cesium, one of the radiologically important fission products, in the nuclear reactor becomes a great concern as the occurrence may affect radioactivity in the long term or its environmental fate. Herein the chemical compound of cesium that had been largely trapped on the nuclear reactor structural material of (calcium silicate) thermal insulator in a simulated nuclear accident condition was investigated. A combined pre- and post-water dissolution analysis through infrared (IR) spectroscopy and optical emission spectroscopy (OES) was explored to resolve the characterization difficulty encountered in conventional X-ray diffraction analysis reported in the previous works. This method allowed us to identify for the first time the related large amount of water-soluble cesium in the calcium silicate material after a high-temperature chemical reaction as cesium metasilicate (CsSiO). It was evidenced by similar vibrational characteristics of the material to that in the synthesized CsSiO as well as the dissolved Cs and Si in the leaching water having a molar ratio of 2.16
0.33. The corresponding 79-98% of the retained cesium in calcium silicate materials in the case study of 700 and 800C reactions was of this compound, emphasizing its significance once formed. Thermodynamic considerations further corroborated the higher stability of CsSiO in the cesium-calcium silicate reaction than other cesium silicates such as CsSiO
, CsSiO
, or Cs
SiO
. This clearly poses a high environmental risk due to the volatility of cesium metasilicate as it may spread out further through the water leak path from a damaged nuclear reactor.
at temperature range 170 - 290CLuu, V. N.; 中島 邦久
Nuclear Engineering and Design, 426, p.113402_1 - 113402_7, 2024/09
被引用回数：3 パーセンタイル：40.43(Nuclear Science & Technology)A field assessment at the Fukushima-Daiichi Nuclear Power Station revealed high radioactivity on the concrete shield plugs, which is estimated above 20 PBq for Cs-137 at units 2 and 3. This leads to significant interest in the retention of Cs on concrete during severe accidents (SA). However, the interaction of CsOH, as one of the main Cs forms released in SA, with concrete surfaces at elevated temperatures remains poorly researched. In this study, we have experimentally investigated the deposition behavior of CsOH on CaCO, which is the primary phase existing on the surface of concrete, under humid atmosphere. As a result, the chemical reaction enhanced deposition rate (N), and increased linearly with CsOH concentration (C
), as following expression: N(
g/cm
s) = v
C, where v is temperature-dependent deposition velocity as given by ln v (cm/s) = -3785.8/T + 3.766, for T in the range of 170 and 290 C. This empirical model can be integrated into severe accident codes to quantify the chemical trapping of cesium on concrete surfaces during ex-vessel release. Moreover, it can contribute to understanding the reasons behind the high dose rate on concrete shield plugs at the Fukushima Daiichi Nuclear power stations and aid in developing effective decommissioning practices for concrete structures.
reaction systemRizaal, M.; 中島 邦久; 鈴木 恵理子; 三輪 周平
Proceedings of 11th European Review Meeting on Severe Accident Research Conference (ERMSAR 2024) (Internet), 11 Pages, 2024/05
The pseudo-binary CsI-MoO reaction system during transportation in the reactor under severe accident conditions has been investigated by using the JAEA-TeRRa semi-integral test facility. An oxygen gas with approximately 10 mbar of partial pressure was given to argon-steam upstream gas flow during the reaction to study its effect on downstream chemistry between CsI and MoO (Mo/Cs molar ratio of 2.13). The product of CsI-MoO reactions both gas and aerosols were analyzed upon their condensation on type-304L stainless steel sampling coupons at respective temperatures (T= 1150-450 K). Post-test analyses revealed that at a low oxygen potential of -192 kJ/mol (i.e. reference case with argon-steam only), most of the CsI reached downstream (T 
400 K) without any reaction with MoO. On the other hand, when oxygen potential was slightly increased to about -144 kJ/mol, the CsI vapor could react with MoO to form cesium polymolybdates (CsMoO
and CsMoO
) and gaseous iodine which predominated the aerosol and gas that reached the downstream region. Particle size at this location was found to be less than 2.7 m in contrast to the former case having an irregularly large size. The gaseous iodine in the latter case, based on the thermodynamic analyses, was estimated to be hypoiodous acid (HIO) or molecular iodine (I). The results in this study indicated that speciation of both Cs and I with the Mo chemistry during a severe accident could be variedly formed depending on the prevailing oxygen potential.
Li, N.*; Sun, Y.*; 中島 邦久; 黒崎 健*
Journal of Nuclear Science and Technology, 61(3), p.343 - 353, 2024/03
被引用回数：1 パーセンタイル：12.78(Nuclear Science & Technology)福島原子力発電所(1F)事故では、表面積の大きなステンレス鋼(SS304)製の気水分離器や蒸気乾燥器にセシウムが大量に残っている可能性がある。そして、1F廃止措置においてこのようなCsは、放射性粉塵を生成する可能性があるため、安全上問題になることが予想される。しかし、水酸化セシウム(CsOH)の化学吸着により生成した酸化被膜の付着強度については、まだ、明らかになっていない。本研究では、CsOHによる化学吸着がどの程度酸化被膜の付着強度に影響するかスクラッチ試験機を用いて調査した。その結果、CsOHの化学吸着により酸化被膜の付着強度は低下したが、剥離させることはできなかった。
CLuu, V. N.; 中島 邦久
Mechanical Engineering Journal (Internet), 11(2), p.23-00446_1 - 23-00446_11, 2024/01
Cesium distribution is crucial for decommissioning Fukushima Daiichi Nuclear Power Station (1F). Several experimental studies confirmed Cs retention on stainless steels by performing chemical reactions at high temperatures (typically above 800C)), but the Cs retention on concrete, used in large quantities in light water reactors, is not fully understood. This study demonstrated that Cs might have been deposited and retained on the concrete structures where the temperature was not so high during the 1F accident. Results showed that the CsOH/concrete interaction at around 200C occurred in water-insoluble Cs-(Al,Fe)-Si-O deposits and water-soluble phases, i.e., cesium carbonate hydrate and possibly cesium silicate if Al and Fe are not present. CsOH might be trapped on concrete by chemical reaction with CaCO to form CsCO hydrate, and with aluminosilicate and SiO(quartz) to form Cs-Al-Si-O and Cs-Si-O deposits, respectively. This output could help elucidate the trapping mechanism that caused extremely high radioactivity on concrete shield plugs at 1F and develop an effective decommissioning practice for concrete structures.
CLuu, V. N.; 中島 邦久
Proceedings of 30th International Conference on Nuclear Engineering (ICONE30) (Internet), 9 Pages, 2023/05
Information of Cs distribution is important for decommissioning of the Fukushima Daiichi Nuclear Power Station (1F). Several experimental studies confirmed the Cs retention on stainless steels by chemical reaction at very high temperatures (commonly above 800C), but the Cs retention on non-metallic materials, such as concrete and thermal insulators, was not fully understood though they are used with large quantity in light water reactors. This study demonstrated that Cs might be deposited and retained on the concrete structure where the temperature was not so high during the 1F accident. It was revealed that the CsOH/concrete interaction at around 200C resulted in the formation of water-insoluble Cs-(Al,Fe)-Si-O deposits and water-soluble phases, i.e., cesium carbonate hydrate and possibly cesium silicate, if Al and Fe are not present. CsOH might be trapped on concrete by chemical reaction with CaCO to form CsCO hydrate, and with aluminosilicate and SiO(quartz) to form Cs-Al-Si-O and Cs-Si-O deposits, respectively. This output will be useful for elucidating the trapping mechanism that caused an extremely high radioactivity on concrete shield plugs at 1F, and for developing an effective decommissioning practice for concrete structure.
Mohamad, A. B.; 中島 邦久; 三輪 周平; 逢坂 正彦
Journal of Nuclear Science and Technology, 60(3), p.215 - 222, 2023/03
被引用回数：1 パーセンタイル：9.64(Nuclear Science & Technology)The distribution of Sr in the reactor would be influenced by a chemical reaction of Sr vapor species with a structural material of internal reactor and fuel cladding materials; stainless steel (SS) or Zircaloy (Zry) cladding during 1F-NPS accident. The chemical interaction between Sr-Zry and Sr-SS has been described. The reaction tests have been performed to investigate the chemical interaction behavior under possible severe accident conditions. The tests have been conducted up to 1523 K under steam atmosphere. It was confirmed that Sr-Zr-O and Sr-Si-O compounds were formed through 2 kinds chemical interactions; gas-solid reaction and liquid-solid reaction. The gas and liquid species of Sr in a good contact with the solid Zry and SS to form Sr-Zr-O and Sr-Si-O compounds, respectively. Sr was deposited onto the Zry and SS surfaces and lead to the formation of reaction product. Thus, this study highlights the possibility that Sr was deposited and retained in the core structure where the temperature was elevated during the accident in the 1F-NPS.
Luu, V. N.; 中島 邦久
Journal of Nuclear Science and Technology, 60(2), p.153 - 164, 2023/02
被引用回数：8 パーセンタイル：61.11(Nuclear Science & Technology)Recently, extremely high dose rates were detected in the three-layer concrete plugs of Units 2 and 3 at the Fukushima Daiichi Nuclear Power Plant. The high dose rates suggest that there are some trapping effects of radioactive materials on shield plugs when gas species and aerosols (e.g., CsOH, CsI) are released from reactor through the plug layers. To determine the trapping mechanism, concrete and commonly used aggregate and minerals are pulverized and mixed with CsOH, followed by heating at different temperatures to clarify the chemical interaction. The results showed that interactions of CsOH and CaCO in concrete occurred even at room temperature to form CsCO(HO). The interaction with aggregates occurred above 100C and resulted in the formation of CsAlSiO. Additionally, amorphous and crystalline SiO interacted with CsOH, forming a glass-like product above 200C. These results suggest that formation of CsCO(HO) would be one of the main trapping mechanism at shield plugs because CaCO is commonly formed on concrete surface and reacts with CsOH at room temperature.
三輪 周平; 唐澤 英年; 中島 邦久; 木野 千晶*; 鈴木 恵理子; 井元 純平
JAEA-Data/Code 2021-022, 32 Pages, 2023/01
JAEA-Data-Code-2021-022.pdf:1.41MBJAEA-Data-Code-2021-022(errata).pdf:0.17MB
東京電力福島第一原子力発電所の原子炉内におけるセシウム分布のより正確な予測に向けて、核分裂生成物の化学挙動データベースECUMEに格納されているステンレス鋼へのセシウム化学吸着モデルをシビアアクシデント解析コードSAMPSONに組み込んだ。改良モデルを組み込んだSAMPSONにより、当該モデルを構築した実験の結果を再現し、コードに誤りが無いことを確認した。また、SAMPSONに組み込まれた改良モデルのセシウム化学着挙動解析への有効性を確認するため、温度勾配管を有する装置を用いた実験の解析を実施した。改良モデルを組み込んだSAMPSONにより、実験の結果を再現し、SAMPSONにおけるノードジャンクションの設定方法、エアロゾル生成モデル、CsOH蒸気の飽和蒸気圧等の計算方法等の解析方法、そして改良モデルがセシウム化学吸着挙動解析に適用可能であることを確認した。また、セシウムがシビアアクシデント後に水相を介して移行したことから、原子炉内におけるセシウム分布を予測するためには、セシウム沈着物の水への溶解性の評価が前提となる。このため、ステンレス鋼へのセシウム化学吸着生成物の水への溶解性を調べた。ステンレス鋼304へのセシウム化学吸着生成物は、873Kから973Kで水溶性の高いCsFeO、973Kから1273Kで水溶性の低いCsFeSiO、1073Kから1273Kで水溶性の低いCsSiOであることが分かった。これらの結果から、セシウム化学吸着量に影響を与える原子炉内温度やCsOH蒸気種濃度のようなシビアアクシデント解析条件に応じて、セシウム化学吸着生成物の水への溶解性を予測できる可能性を得た。
Rizaal, M.; 中島 邦久; 斉藤 拓巳*; 逢坂 正彦; 岡本 孝司*
ACS Omega (Internet), 7(33), p.29326 - 29336, 2022/08
被引用回数：7 パーセンタイル：30.10(Chemistry, Multidisciplinary)Here we report an investigation of the gas-solid reaction between cesium hydroxide (CsOH) and siliceous (calcium silicate) thermal insulation at high temperature, which was postulated as the origin for the formation mechanism of cesium-bearing material emitted from the Fukushima Daiichi Nuclear Power Plant. A developed reaction furnace consisting of two heating compartments was used to study the reaction at temperatures of 873, 973, and 1073 K. Under the influence of hydrogen-steam atmospheric conditions (H/HO = 0.2), the reaction between cesium hydroxide vapor and solid thermal insulation was confirmed to occur at temperatures of 973 and 1073 K with the formation of dicalcium silicate (CaSiO) and cesium aluminum silicate (CsAlSiO). Water-dissolution analyses of the reaction products have demonstrated their stability, in particular, the CsAlSiO. Constituents similarity of the field-observed cesium-bearing materials near the Fukushima Daiichi Nuclear Power Plants with CsAlSiO suggests for the first time that gaseous reaction between CsOH with calcium silicate thermal insulation could be one of the original formation mechanisms of the cesium-bearing materials.
Liu, J.; 中島 邦久; 三輪 周平; 白数 訓子; 逢坂 正彦
Journal of Nuclear Science and Technology, 59(4), p.484 - 490, 2022/04
被引用回数：0 パーセンタイル：0.00(Nuclear Science & Technology)A new method named TG calibration curve method has been proposed to evaluate the Ru activity in the Ru-containing alloys by using the kinetic relationship between oxidative evaporation rate of Ru atom and overall vapor pressures of various RuOx gases in the experimental system constructed by the authors. The experimental results show that the oxidative evaporation rate of Ru atom from experimental powders is approximately proportional to the overall vapor pressures over powders. By using their specific quantitative relationship, we determined the Ru activity in Ru
Pd alloy in the temperature range from 1523 to 1673 K. The obtained values of Ru activity agree well with those theoretically calculation, and indicated the reliability of this new method.
鈴木 知史; 中島 邦久; 逢坂 正彦
Journal of Nuclear Science and Technology, 59(3), p.345 - 356, 2022/03
被引用回数：4 パーセンタイル：32.33(Nuclear Science & Technology)福島第一原子力発電所事故などの過酷事故(SA)では、原子炉の構造材料の表面に核分裂生成物(FP)が沈着する可能性がある。FPの中でも特にセシウム(Cs)は重要であり、SA発生時には原子炉内の構造材のステンレス鋼(SS)の表面にCsケイ酸塩等の種々のCs化合物が形成される。これらのCs化合物の相安定性を評価するために、Cs-Si-O化合物のエネルギーの計算を実施した。その結果、CsSiO
がCs-Si-O化合物の中で最も安定していることが分かった。さらに、Cs-Si-Fe-O化合物のエネルギーの計算を実施した。計算結果より、Cs-Si-Fe-O化合物はCs-Si-O化合物よりも安定しており、CsSiFeOがCs-Si-O化合物およびCs-Si-Fe-O化合物の中で最も安定していることが分かった。今回の計算と過去の実験の結果によって、Cs-Si-Fe-O化合物はCs化学吸着によってSS表面に安定して形成できることが示された。
