Chemical forms of uranium evaluated by thermodynamic calculation associated with distribution of core materials in the damaged reactor pressure vessel

池内 宏知; 矢野 公彦; 鷲谷 忠博

Journal of Nuclear Science and Technology, 57(6), p.704 - 718, 2020/06

https://doi.org/10.1080/00223131.2020.1720844

福島第一原子力発電所から取り出された燃料デブリへの効果的な処置方策を提案する上では、燃料デブリ中でUがとりうる化学形についての詳細な調査が不可欠である。特に、アクセス性に乏しい圧力容器内に残留する燃料デブリに関する情報が重要である。本研究では、圧力容器内燃料デブリ中、特にマイナー相におけるUの化学形を評価することを目的とし、1F-2号機の事故進展での材料のリロケーション及び環境変化を考慮した熱力学計算を実施した。組成,温度,酸素量といった計算条件は、既存の事故進展解析の結果から設定した。計算の結果、Uの化学形はFeとOの量によって変化し、Feの少ない領域で-(Zr,U)(O)、Feの多い領域でFe(Zr,U) (Laves相)の生成が顕著であった。還元性条件で生成するこれらの金属相中には数パーセントのUが移行しており、燃料デブリの処置において核物質の化学分離を考慮する場合はこれらの相の生成に留意すべきと考えられる。

Material characterization of the VULCANO corium concrete interaction test with concrete representative of Fukushima Daiichi Nuclear Plants

Brissonneau, L.*; 池内 宏知; Piluso, P.*; Gousseau, J.*; David, C.*; Testud, V.*; Roger, J.*; Bouyer, V.*; 北垣 徹; 仲吉 彬; et al.

Journal of Nuclear Materials, 528, p.151860_1 - 151860_18, 2020/01

https://doi.org/10.1016/j.jnucmat.2019.151860

In the framework of JAEA-CEA collaboration, experimental studies have been conducted for estimating the material characteristics of corium debris representative of the Fukushima Daiichi nuclear damaged plants. A test has been performed in the VULCANO facility in CEA Cadarache to simulate the concrete corium interaction (CCI) with prototypic corium (using depleted uranium) and concrete of Fukushima Daiichi 1F1 Nuclear Plant. This paper presents the Post Test Analyses on 9 samples representative of the CCI during this test: in the corium pool, in the crusts and at the vertical and horizontal interfaces with the concrete. Analyses have been performed by SEM/EDS, X-Ray Diffraction, complete dissolution and ICP, micro-hardness measurements of the main phases. The major phases encountered are uranium rich and zirconium rich oxides forming nodules from micrometers to millimeters size, chromium-iron rich precipitates of several micrometers, metallic Fe-Ni droplets and chromium-silicon rich filaments in a matrix, likely vitreous, rich in concrete elements: Si, Al, Ca, but containing up to 12 cations. The matrix is the softer oxide phase, when the Cr rich precipitates are the harder. The analyses are consistent with the estimated macroscopic ablation ratio, but do not still explain the important axial ablation observed for this specific basaltic concrete. The different phases formation, distribution and solidification path are discussed. First comparisons are proposed with the former CCI tests with European concretes. These results give helpful insights for the future dismantling of the plant and for a deeper understanding of the CCI process for basaltic concrete.

Effect of quenching on molten core-concrete interaction product

北垣 徹; 池内 宏知; 矢野 公彦; Brissonneau, L.*; Tormos, B.*; Domenger, R.*; Roger, J.*; 鷲谷 忠博

Journal of Nuclear Science and Technology, 56(9-10), p.902 - 914, 2019/09

AA2018-0409.pdf:2.12MB

https://doi.org/10.1080/00223131.2019.1604272

Characterization of fuel debris is required to develop fuel debris removal tools. Especially, knowledge pertaining to the characteristics of molten core-concrete interaction (MCCI) product is needed because of the limited information available at present. The samples of a large-scale MCCI test performed under quenching conditions, VULCANO VW-U1, by CEA were analyzed to evaluate the characteristics of the surface of MCCI product generated just below the cooling water. As a result, the microstructure of the samples were found to be similar despite the different locations of the test sections. The Vickers hardness of each of the phases in these samples was higher than that of previously analyzed samples in another VULCANO test campaign, VBS-U4. From the comparison between analytical results of VULCANO MCCI test product, MCCI product generated under quenching condition is homogeneous and its hardness could be higher than that of the bulk MCCI product.

Large scale VULCANO molten core concrete interaction test considering Fukushima Daiichi condition

Bouyer, V.*; Journeau, C.*; Haquet, J. F.*; Piluso, P.*; 仲吉 彬; 池内 宏知; 鷲谷 忠博; 北垣 徹

Proceedings of 9th Conference on Severe Accident Research (ERMSAR 2019) (Internet), 13 Pages, 2019/03

Fuel debris removal is one of the most important processes for decommissioning a severely damaged nuclear power plant (NPP) such as Fukushima Daiichi NPP (1F). In order to develop relevant removal tools, characteristics of fuel debris are required. In the frame of a JAEA-CEA cooperation, a large-scale MCCI test was performed at the CEA/VULCANO facility using a prototypic metal and oxide corium representative from Fukushima Daiichi unit 1 conditions. Conclusions arising from the material analysis of the selected samples will be relevant for future dismantling operations. This paper deals with the experimental device and process, objective and initial conditions of this MCCI test, and ablation of the concrete quantified in term of volume, depths and velocities. The test section concrete, made with Japanese components, is siliceous with basaltic origin. The main objective of the test was to get a significant ablation leading to an ablation volume ratio of 1.6 in order to produce fuel debris with a composition corresponding to expected conditions in the damaged plant. On a phenomenological point of view, it must be noted that the concrete ablation was clearly anisotropic with a predominantly downwards ablation contrary to previous experiments with silica and limestone concrete.

R&D strategy on mid- and long-term behavior of fuel debris

矢野 公彦; 北垣 徹; 鷲谷 忠博; 宮本 泰明; 小川 徹

Progress in Nuclear Science and Technology (Internet), 5, p.225 - 228, 2018/11

https://doi.org/10.15669/pnst.5.225

福島第一原子力発電所の廃炉に向けたロードマップによると、燃料デブリ取り出しは2021年、すなわち燃料デブリ生成の10年後に開始される予定である。また燃料デブリは燃料取り出しの終了まで炉内に存在することになる。加えて、炉から取り出された燃料デブリに対して保管が必要になることは想像に難くない。このような事故後の燃料デブリに対する作業を検討するうえで、数十年間の燃料デブリの状態や特性を議論することは不可欠である、そこで原子力機構は燃料デブリの中長期的挙動に関する研究開発戦略を暫定するとともに、この課題に対して国内の大学や他の研究機関と協力し基礎研究を立ち上げている。

Thermodynamic evaluation of the solidification phase of molten core-concrete under estimated Fukushima Daiichi Nuclear Power Plant accident conditions

北垣 徹; 矢野 公彦; 荻野 英樹; 鷲谷 忠博

Journal of Nuclear Materials, 486, p.206 - 215, 2017/04

AA2016-0278.pdf:0.74MB

https://doi.org/10.1016/j.jnucmat.2017.01.032

The solidification phases of molten core-concrete under the estimated molten core-concrete interaction (MCCI) conditions in the Fukushima Daiichi Nuclear Power Plant Unit 1 were predicted using the thermodynamic equilibrium calculation tool in order to contribute toward the 1F decommissioning work and to understand the accident progression via the analytical results for the 1F MCCI products. We showed that most of the U and Zr in the molten core-concrete forms (U,Zr)O and (Zr,U)SiO, and the formation of other phases with these elements is limited. However, the formation of (Zr,U)SiO requires a relatively long time. Therefore, the formation of (Zr,U)SiO is limited under quenching conditions. The solidification phenomenon of the crust under quenching conditions and that of the molten pool under thermodynamic equilibrium conditions in the 1F MCCI progression are discussed.

Study of treatment scenarios for fuel debris removed from Fukushima Daiichi NPS

鷲谷 忠博; 矢野 公彦; 鍛治 直也; 山田 誠也*; 紙谷 正仁

Proceedings of 23rd International Conference on Nuclear Engineering (ICONE-23) (DVD-ROM), 7 Pages, 2015/05

福島第一原子力発電所の燃料デブリ取出し後の処置については、燃料デブリ取出し開始時までにデブリの処置の選択決定に係る一定の議論が必要になるものと想定し、それまでに各シナリオの比較評価に用いる情報や比較評価の進め方を決める必要がある。そのため、本検討では燃料デブリの取出し後の処置シナリオの検討に向けた技術的要件の整理として、各処置シナリオ案の得失評価を行った。評価の結果、総合すると技術課題は有するものの経済性、廃棄物発生量の面で有利なシナリオは長期保管及び直接処分と推定された。一方、安定化処理、湿式処理、乾式処理は経済性、廃棄物発生量の面で不利と推定された。

Dissolution behavior of (U,Zr)O-based simulated fuel debris in nitric acid

池内 宏知; 石原 美穂; 矢野 公彦; 鍛治 直也; 中島 靖雄; 鷲谷 忠博

Journal of Nuclear Science and Technology, 51(7-8), p.996 - 1005, 2014/07

https://doi.org/10.1080/00223131.2014.924445

To explore the possibility of dissolving fuel debris as a potential pre-treatment for waste treatment, dissolution tests of UZrO and (U,Pu)ZrO were carried out in 6 M HNO at 353 K. While the U and Zr indicated congruent leaching from the simulated debris with U-rich compositions, a preferential leaching of U was observed with Zr-rich compositions. Taking into account these different dissolution phenomena, the dissolution rate analysis was carried out using surface-area model to calculate the instantaneous dissolution rate (IDR). From these findings, dissolution with HNO is expected to be only applicable in U-rich compositions ( 0.3) if the dissolution in 6 M HNO at 353 K is assumed. Application of complexing acids such as mixture of HNO and HF should be considered to increase the dissolution rate of the phases with Zr-rich compositions.

Direction on characterization of fuel debris for defueling process in Fukushima Daiichi Nuclear Power Station

矢野 公彦; 北垣 徹; 池内 宏知; 涌井 遼平; 樋口 英俊; 鍛治 直也; 小泉 健治; 鷲谷 忠博

Proceedings of International Nuclear Fuel Cycle Conference; Nuclear Energy at a Crossroads (GLOBAL 2013) (CD-ROM), p.1554 - 1559, 2013/09

For the decommissioning of Fukushima Daiichi Nuclear Power Station (1F), defueling work for the fuel debris in the reactor core of Unit 1-3 is planned to be started within 10 years. Preferential items in the characterization of the fuel debris were identified for the defueling work at 1F, in which the procedure and handling tools were assumed from information of 1F and experience of Three Mile Island Unit 2 (TMI-2) accident. The candidates of defueling tools for 1F were selected from TMI-2 defueling tools. It was found out that they were categorized as 6 groups by their working principles. Important properties on the fuel debris for the defueling were picked up from considering influence of objective materials on their performance. The selected properties are shape, size, density, thermal conductivity, heat capacity, melting point, hardness, elastic modulus, and fracture toughness. In these properties, mechanical properties, i.e. hardness, elastic modulus, fracture toughness were identified as preferential items, because there are few data on that of fuel debris in the past severe accident studies.

Applicability of single mode fiber laser for wrapper tube cutting

涌井 遼平; 北垣 徹; 樋口 英俊; 竹内 正行; 小泉 健治; 鷲谷 忠博

Proceedings of 20th International Conference on Nuclear Engineering and the ASME 2012 Power Conference (ICONE-20 & POWER 2012) (DVD-ROM), 7 Pages, 2012/07

Japan Atomic Energy Agency (JAEA) has been developing a fuel disassembly system with reliability for FBR fuel reprocessing. Laser technology has a high cutting performance and stable operation. However, it was hard to apply to the fuel disassembly system in our previous study, because of pin damage and dross adhesion between a wrapper tube and fuel pins. The advance of the laser cutting technology has recently attracted. Development of single mode fiber laser (SMFL) with small diameter of a beam spot has been especially reported. Then, we believed that it has become possible to prevent the dross adhesion in the disassembly. The main purpose of this study is to reevaluate an applicability of laser for the wrapper tube cutting by the basic cutting tests. Concretely, we researched whether cutting conditions such as SMFL etc, have the effects on dross adhesion and pin damage or not and tried to prevent these original matters. As the result, it was demonstrated that the kerf width of SMFL is still thinner than that of multi mode fiber laser (MMFL). The phenomenon is very important to decrease the amount of dross. Therefore, we confirmed that SMFL is suitable for prevention of the original matters and this experimental results shown the new feasibility method of wrapper tube cutting.