The Precipitation and redistribution of alloying element in Zircaloy-4 cladding tube oxidized in high-temperature steam

天谷 政樹

High Temperature Corrosion of Materials, 15 Pages, 2024/00

https://doi.org/10.1007/s11085-023-10216-9

Zirconium (Zr)-based alloys are widely used as fuel cladding material for light water reactors. Under a loss-of-coolant accident (LOCA) condition, the oxidation of fuel cladding by high-temperature steam induces the degradation of mechanical properties of the cladding and would affect the integrity of fuel rods and/or assemblies, etc., during LOCA. In this study, the distribution of the elements (zirconium, oxygen, tin, iron and chromium) in Zircaloy-4 cladding specimens oxidized in the temperature range of 1350- 1700 K in steam was analyzed along the radial direction of the specimens by using SEM/EPMA, and the cause of element distribution in the specimens was discussed in consideration of the morphology of precipitates in the specimens and hypothesized phase diagrams related to the elements contained in the specimens. The form of the particles precipitated and the comparison between SEM/EPMA results and hypothesized phase diagrams of Zr-Sn-O system suggested that the liquefaction of tin-rich material and/or Zr-(Fe,Cr) compounds occurred during the oxidation test. The results obtained indicate that Zircaloy-4 cladding tubes would start melting at the melting point of tin-oxide and the eutectic point of Zr-(Fe,Cr)compounds, which is much lower than the melting point of Zr, -Zr(O), or zirconium oxide (ZrO).

Microstructural evolution of intermetallic phase precipitates in Cr-coated zirconium alloy cladding in high-temperature steam oxidation up to 1400C

Mohamad, A. B.; 根本 義之; 古本 健一郎*; 岡田 裕史*; 佐藤 大樹*

Corrosion Science, 224, p.111540_1 - 111540_15, 2023/11

https://doi.org/10.1016/j.corsci.2023.111540

The steam oxidation test on the Cr-coated Zry cladding was studied up to 1400C to understand the oxidation behavior under the accidental conditions. The double-sided oxidation test study showed that Cr coating can protect Zry cladding at 1200C within 5 min. Cr coating has a protective effect on the Zry cladding up to 1200C in a steam environment. However, in the oxidation test up to 1200C/30 min and 1300C/5 min, Cr coating can no longer protect Zry cladding. Furthermore, at 1300C, the intermetallic phase of the Zr(Cr, Fe) phase that precipitated within the Zry substrate formed as globule microstructures with Fe enrichment. In addition, the transition of the intermetallic phase within the Zry substrate from the solid to the pre-liquid and liquid phases was observed, where it was determined at 1350C/60 min and 1400C/30 min within the ZrO phase (outer side region). The oxidation of the Zr(Cr, Fe) interlayer was also determined in this study, where it resulted in the formation of the oxide phase of Cr, Zr, and Fe. It is worth mentioning that further experiments, such as mechanical testing and modeling, should be considered to support the degradation of the Cr-coated Zry cladding mainly when the liquid phase of the intermetallic phase is obtained for beyond design-basis accident environment.

Steam oxidation of silicon carbide at high temperatures for the application as accident tolerant fuel cladding, an overview

Pham, V. H.; 倉田 正輝; Steinbrueck, M.*

Thermo (Internet), 1(2), p.151 - 167, 2021/09

https://doi.org/10.3390/thermo1020011

Since the nuclear accident at Fukushima Daiichi Nuclear Power Station in 2011, a considerable number of studies have been conducted to develop accident tolerant fuel (ATF) claddings for safety enhancement of light water reactors. Among many potential ATF claddings, silicon carbide is one of the most promising candidates with many superior features suitable for nuclear applications. In spite of many potential benefits of SiC cladding, there are some concerns over the oxidation/corrosion resistance of the cladding, especially at extreme temperatures (up to 2000C) in severe accidents. However, the study of SiC steam oxidation in conventional test facilities in water vapor atmospheres at temperatures above 1600C is very challenging. In recent years, several efforts have been made to modify existing or to develop new advanced test facilities to perform material oxidation tests in steam environments typical of severe accident conditions. In this article, the authors outline the features of SiC oxidation/corrosion at high temperatures, as well as the developments of advanced test facilities in their laboratories, and, finally, give some of the current advances in understanding based on recent data obtained from those advanced test facilities.

Fracture limit of high-burnup advanced fuel cladding tubes under loss-of-coolant accident conditions

成川 隆文; 天谷 政樹

Journal of Nuclear Science and Technology, 57(1), p.68 - 78, 2020/01

https://doi.org/10.1080/00223131.2019.1659873

To evaluate the fracture limit of high-burnup advanced fuel cladding tubes under loss-of-coolant accident (LOCA) conditions, laboratory-scale integral thermal shock tests were performed using the following advanced fuel cladding tubes with burnups of 73 - 85 GWd/t: M-MDA, low-tin ZIRLO, M5, and Zircaloy-2 (LK3). In total eight integral thermal shock tests were performed for these specimens, simulating LOCA conditions including ballooning and rupture, oxidation, hydriding, and quenching. During the tests, the specimens were oxidized to 10% - 30% equivalent cladding reacted (ECR) at approximately 1473 K and were quenched under axial restraint load of approximately 520 - 530 N. The effects of burnup extension and use of the advanced fuel cladding tubes on the ballooning and rupture, oxidation, and hydriding under LOCA conditions were inconsiderable. Further, the high-burnup advanced fuel cladding tube specimens did not fracture in the ECR values equal to or lower than the fracture limits of the unirradiated Zircaloy-4 cladding tube reported in previous studies. Therefore, it can be concluded that the fracture limit of fuel cladding tubes is not significantly reduced by extending the burnup to approximately 85 GWd/t and using the advanced fuel cladding tubes, though it slightly decreases with increasing initial hydrogen concentration.

Oxidation behavior of high-burnup advanced fuel cladding tubes in high-temperature steam

成川 隆文; 天谷 政樹

Journal of Nuclear Science and Technology, 56(7), p.650 - 660, 2019/07

https://doi.org/10.1080/00223131.2019.1613268

To evaluate the oxidation behavior of high-burnup advanced fuel cladding tubes in high-temperature steam, laboratory-scale isothermal oxidation tests were conducted using the following advanced fuel cladding tubes with burnups of up to 85 GWd/t: M-MDA, low-tin ZIRLO, M5, and Zircaloy-2 (LK3). These oxidation tests were performed in steam-flowing conditions at temperatures ranging from 1173 to 1473 K for durations between 120 and 4000 s, and the oxidation kinetics was evaluated. The oxidation kinetics of the high-burnup advanced fuel cladding tube specimens estimated by assuming the parabolic rate law was comparable to or slower than that of the unirradiated Zircaloy-4 cladding tube specimens reported in a previous study. It is considered that the protective effect of the corrosion layer hindered oxidation. Furthermore, no increase in the oxidation kinetics because of the pre-hydriding was observed. The onset times of the breakaway oxidations of these cladding tube specimens were comparable to those of the unirradiated Zircaloy-4 cladding tubes reported in previous studies. Therefore, it is considered that the burnup extension up to 85 GWd/t and the use of the advanced fuel cladding tubes do not significantly increase the oxidation kinetics and do not significantly reduce the onset time of the breakaway oxidation.

Oxidation kinetics of Zry-4 fuel cladding in mixed steam-air atmospheres at temperatures of 1273 - 1473 K

Negyesi, M.; 天谷 政樹

Journal of Nuclear Science and Technology, 54(10), p.1143 - 1155, 2017/10

https://doi.org/10.1080/00223131.2017.1344583

This paper deals with the oxidation behavior of Zry-4 nuclear fuel cladding tubes in mixed steam_air atmospheres at temperatures of 1273 and 1473 K. The main goal is to study the oxidation kinetics of Zry-4 fuel cladding in dependence on the air fraction in steam in the range from 0 up to 100%. The purpose of this study is to provide experimental data suitable for an oxidation correlation applicable for thermomechanical analysis codes of nuclear power reactor under severe accidents. The influence of the air addition in steam on parameters of Zry-4 kinetic equation has been quantified using the results of weight gain measurements. At 1273 K, both pre-transient and post-transient regimes were treated. The results of weight gain measurements showed a strong dependence of the Zry-4 oxidation kinetics on the air fraction in steam, especially at 1473 and at 1273 K in the post-transient regime.

冷却材喪失事故時の被覆管延性低下に及ぼす冷却時温度履歴の影響

宇田川 豊; 永瀬 文久; 更田 豊志

JAERI-Research 2005-020, 40 Pages, 2005/09

JAERI-Research-2005-020.pdf:4.63MB

急冷開始温度及び急冷前の冷却速度がLOCA時の被覆管延性低下に及ぼす影響を調べることを目的とし、未照射PWR用1717型ジルカロイ-4被覆管から切り出した試料を水蒸気中、1373及び1473Kで酸化し、ゆっくりと冷却(徐冷)してから急冷した。試験条件のうち、徐冷の速度を27K/s、急冷開始温度を10731373Kの範囲で変化させて複数の試験を行い、冷却条件の異なる試料を得た。酸化,急冷した試料に対しリング圧縮試験,ミクロ組織観察,ビッカース硬さ試験を実施した。急冷開始温度低下に伴い、金属層中に析出する相の面積割合が大幅に増加し、被覆管の延性が明確に低下した。徐冷速度の減少に伴い、析出した相の単位大きさ及び硬さの増大が生じたが、面積割合及び被覆管の延性はほとんど変化しなかった。析出相は周りの金属層より硬く、また酸素濃度が高いことから、その延性は非常に低いと考えられる。したがって、析出相の面積割合増大が、急冷開始温度低下に伴う延性低下促進の近因である。

Results from simulated LOCA experiments with high burnup PWR fuel claddings

永瀬 文久; 更田 豊志

Proceedings of 2004 International Meeting on LWR Fuel Performance, p.500 - 506, 2004/09

原研は、さらなる燃焼度延伸がLOCA時の燃料挙動に及ぼす影響を評価するために必要なデータを取得することを目的に、系統的な研究計画を進めている。その計画の一環として、LOCA時に起こる全過程を模擬した総合的な試験を、PWRにおいて3944GWd/tまで照射したジルカロイ-4被覆管に対して実施した。30%ECRまで酸化した被覆管は、急冷時に破断した。この破断は、同等の水素濃度を有する未照射被覆管の破断クライテリア(約25%ECR)に合致する。約16及び18%ECRまで酸化した2本の被覆管は急冷時に破断しなかったことから、調べた燃焼度範囲では、照射によって著しく破断限界が低下することはないと考えられる。本報告では、酸化速度や破裂挙動も含め、試験の結果を報告する。

Recent results from LOCA study at JAERI

永瀬 文久; 更田 豊志

NUREG/CP-0185, p.321 - 331, 2004/00

原研は、高燃焼度燃料の冷却材喪失事故時挙動に関する知見を得ることを目的に、試験計画を進めている。本試験計画では、総合的な急冷試験及び、被覆管の酸化速度や機械特性に関する基礎試験を行う。照射した被覆管に対する試験に先立ち、原子炉運転中に生じる腐食や水素吸収が及ぼす影響を分離的に調べるため、未照射被覆管を用いた試験を実施した。水素吸収は被覆管の脆化に関し重要であることから、その影響を特に詳しく調べた。また、照射した被覆管に対する試験にも着手し、初期のデータを取得した。本報告は、これらの成果をとりまとめたものである。

Study of high burnup fuel behavior under LOCA conditions at JAERI; Hydrogen effects on the failure-bearing capability of cladding tubes

永瀬 文久; 上塚 寛

NUREG/CP-0176, p.335 - 342, 2002/05

高燃焼度燃料のLOCA時挙動を評価するための基礎データを得ることを目的とした試験計画の一環として、被覆管中の水素濃度の増大が急冷時の耐破損特性に及ぼす影響を分離効果的に調べた。試験の結果、水素濃度と急冷時の軸方向拘束力に依存した被覆管の破断しきい値(酸化量)の変化を明らかにすることができた。拘束力が比較的大きな場合は、破断しきい値は水素添加により明確に低下した。拘束力の減少とともに破断しきい値は低下し、調べた水素濃度範囲(1200ppm以下)において、拘束力が540N以下であれば破断しきい値は20% ECR(等価酸化量)を超えた。