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Rizaal, M.; Luu, V. N.; 中島 邦久; 三輪 周平
Proceedings of International Topical Workshop on Fukushima-Daiichi 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 Cs
CO
). 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
Nuclear Engineering and Design, 426, p.113402_1 - 113402_7, 2024/09
被引用回数:0 パーセンタイル:0.00(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.
Luu, 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 200
C 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 Cs
CO
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.
Luu, 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 200
C 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 Cs
CO
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.
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:6 パーセンタイル:74.74(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 Cs
CO
(H
O)
. The interaction with aggregates occurred above 100
C and resulted in the formation of CsAlSiO
. Additionally, amorphous and crystalline SiO
interacted with CsOH, forming a glass-like product above 200
C. These results suggest that formation of Cs
CO
(H
O)
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.
Luu, V. N.; 中島 邦久
no journal, ,
To investigate the source of high dose rates at the concrete shield plugs of Unit 2 and 3 at 1F, high temperature tests on the mixture of CsOH and pulverized concrete/main components were conducted. Results showed that both water-soluble and -insoluble phases were formed below 300C. Namely, Cs
CO
(H
O)
was formed due to chemical reaction with CaCO
at room temperature. The authors will discuss the possibility that this might be one of the main trapping mechanisms on shield plugs.
三輪 周平; 中島 邦久; 唐澤 英年; Rizaal, M.; Luu, V. N.; Mohamad, A. B.
no journal, ,
東京電力福島第一原子力発電所内のセシウム等のFPの分布や性状を把握することが廃炉に向けた重要な課題であり、日本原子力研究開発機構ではそれらに大きな影響を与えるFP化学に着目した基礎研究を実施し、事故時の原子力発電所内のFP化学を評価するためのデータベースECUMEを開発している。ECUMEは福島第一原子力発電所の事故により明らかになった重要な現象、例えば、セシウムの制御材ホウ素との反応や、構造材との反応に関するデータやモデルを収納している。近年の内部調査により明らかとなったシールドプラグでの高線量等の原因を明らかにするため、コンクリートや他の炉内物質との化学反応を調べ、モデル化を行い、ECUMEの更新を進めている。
Luu, V. N.; 中島 邦久
no journal, ,
This study investigated the possibility of chemical interaction between concrete/aggregate and cesium hydroxide at high temperatures. CsOH interaction with CaCO in concrete forms water-soluble Cs
CO
(H
O)
even at room temperature, whereas CsOH interaction with aluminosilicate minerals in aggregate forms water-insoluble CsAlSiO
just above 100
C, according to TG/DTA and XRD analyses on the mixture of CsOH and pulverized concrete/aggregate. The results suggest that the formation of Cs
CO
(H
O)
would be one of the main trapping mechanisms at shield plugs because CaCO
is commonly formed on concrete surfaces and reacts with CsOH at room temperature.
Luu, V. N.; 中島 邦久
no journal, ,
Chemisorption tests of CsOH onto concrete and aggregate were carried out at 200C in both dry and humid conditions to investigate the source of high dose rates at the concrete shield plugs of Units 2 and 3 at 1F. Post-test analyses using XRD, Raman, and SEM revealed that water-insoluble Cs-bearing deposits formed different morphologies under dry and humid conditions. Namely, uniform and large Cs deposits were formed under humid conditions, while heterogenous growth and smaller size Cs deposits were observed under dry conditions.
Rizaal, M.; 中島 邦久; 唐澤 英年; Luu, V. N.; 三輪 周平
no journal, ,
Our research focused on, but is not limited to, cesium (Cs) and iodine (I) chemistry due to their high impact on the overall source term. The retention or release of both elements is largely affected by chemical interaction with materials that are present in the reactor. To understand their chemistry during transport in the event of a nuclear severe accident (SA), we studied the interaction phenomena taking place from high- to low-temperature conditions. We have succeeded in elucidating these phenomena (particularly Cs) and summarized them in a fission product (FP) chemistry database ECUME. This database not only could deepen our understanding of the mechanism of Cs and I chemistry in an SA, but could also improve source term analysis. Improvement in the reaction between Cs vapor and stainless steel was shown by the use of the ECUME database in SA analysis code SAMPSON. Better reproducibility of Cs retention at high temperatures of the large-scale experiment was obtained, in contrast to using the MELCOR Cs interaction model (i.e. widely used model in SA code) that was worse in reproducing such phenomenon. Taking into consideration of near-term implementation of Accident Tolerant Fuel (ATF) materials such as chromium (Cr)-coated Zircaloy, further study on the interaction with FP would be important to ensure the material impact on source term because the reaction between Cs and Cr can be thermodynamically expected.
Luu, V. N.; 中島 邦久
no journal, ,
A recent field survey revealed extremely high radioactivity on the concrete shield plugs, exceeding 20 PBq for Cs-137 at units 2, 3 of 1F. This leads to significant interest in the retention of Cs on concrete during severe accident. Despite this, the interaction of Cs vapors and/or aerosols in the gas phase with concrete surfaces at high temperatures remains inadequately explored. In this work, we investigated the deposition behavior of CsOH on CaCO, as a primary phase on the concrete surface, under humid atmosphere. As a result, the chemical reaction enhanced deposition rate, and increased linearly with CsOH concentration.