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).

The Effect of a cyclic bending load on the bending resistance of ballooned, ruptured, and oxidized Zircaloy-4 cladding

Li, F.; 成川 隆文; 宇田川 豊

Journal of Nuclear Science and Technology, 12 Pages, 2023/00

https://doi.org/10.1080/00223131.2023.2293100

The seismic resistance of fuel cladding during the long-term core cooling after loss-of-coolant accidents (LOCAs) was investigated by performing cyclic four-point bending tests (4PBTs) of up to 1000 cycles with fresh fuel cladding samples that experienced integral thermal shock test, simulating LOCA conditions, including ballooning, rupture, oxidation, and quench. 4PBTs were performed on the samples that survived the quenching process. The results showed that up to 1000 cycles and 5.8 Nm of cyclic loading moment, there was no apparent effect on the bending fracture limit of the fuel cladding under the 4PBT. The scatter of the bending fracture limit for a given equivalent cladding reacted (ECR) evaluated by the Baker-Just oxidation rate equation (BJ-ECR) is attributed to two primary factors: first, the difference between the prescribed and the actual oxidation behavior, confirmed by comparing the BJ-ECR and the ECR evaluated based on metallographic observation (M-ECR), and second, the variated shape of the rupture-opening area after the integral thermal shock test. The strength of the alpha phase-dominant zone near the rupture opening seems to contribute to the bending fracture limit.

Leaching behavior of radionuclides from samples prepared from spent fuel rod comparable to core debris in the 1F NPS

大西 貴士; 前田 宏治; 勝山 幸三

Journal of Nuclear Science and Technology, 58(4), p.383 - 398, 2021/04

https://doi.org/10.1080/00223131.2020.1822943

To investigate the leaching behavior of radioactive nuclides in leaching samples comparable to core debris (partially molten ZrO/UO between fuel rods) in 1F NPS, the concentration of radionuclides in the leaching solution was measured. Leaching behaviors of actinides (U, Pu, Np) and Cs from the samples were similar to those from spent fuel. Leaching of U and Pu depends on pH in the cooling water of the core debris as predicted from the present thermodynamic database. While, if Mo and Tc are surrounded by zircaloy in the core debris, their leaching amount may become higher by one order of magnitude than those from spent fuel.

Effects of ballooning and rupture on the fracture resistance of Zircaloy-4 fuel cladding tube after LOCA-simulated experiments

湯村 尚典; 天谷 政樹

Annals of Nuclear Energy, 120, p.798 - 804, 2018/10

https://doi.org/10.1016/j.anucene.2018.06.046

To investigate the relationship between the fracture resistance of a cladding tube and the amount of deformation of the cladding tube due to ballooning and rupture during a loss-of-coolant accident (LOCA), four-point-bending tests were performed using non-irradiated Zircaloy-4 cladding tubes which experienced a LOCA-simulated sequence (ballooning, rupture, high temperature oxidation and quench). According to the obtained results, it was found that the maximum bending stress of the cladding tube after the LOCA-simulated sequence, which was defined as the fracture resistance, correlated to the average thickness of prior- layer in the cladding tube. Based on the average thickness of prior- layer, the fracture resistance of the cladding tube with ballooning and rupture was expressed as functions of isothermal oxidation time and temperature and the maximum circumferential strain on the cladding tube.

Uncertainty quantification of fracture boundary of pre-hydrided Zircaloy-4 cladding tube under LOCA conditions

成川 隆文; 山口 彰*; Jang, S.*; 天谷 政樹

Nuclear Engineering and Design, 331, p.147 - 152, 2018/05

https://doi.org/10.1016/j.nucengdes.2018.02.037

To quantify the fracture boundary uncertainty for non-irradiated, pre-hydrided Zircaloy-4 cladding tube specimens under loss-of-coolant accident conditions at a light-water reactor, data from integral thermal shock tests obtained by an earlier study are analyzed statistically and the fracture boundary is estimated in terms of probability, as follows. First, a method is proposed to obtain the specimens' fracture probability curve as a function of equivalent cladding reacted (ECR) and initial hydrogen concentration using Bayesian inference with a generalized linear model. A log-probit model is used, modified to reflect the effect of the initial hydrogen concentration on the fracture boundary and the ECR evaluation uncertainty, and scaled to improve convergence. Second, using the modified log-probit model, it is shown that the boundary representing a 5% fracture probability with 95% confidence for the pre-hydrided cladding tube sample is higher than 15% ECR, for initial hydrogen concentrations of up to 800 wppm.

Zircaloy-4の高温酸化挙動に及ぼす固体ホウ酸の影響

小宮山 大輔; 天谷 政樹

JAEA-Research 2016-013, 20 Pages, 2016/08

JAEA-Research-2016-013.pdf:6.05MB

PWRの冷却材喪失事故(LOCA)において、流路の閉塞等により燃料棒の冷却が十分に行われない場合、燃料被覆管表面に冷却材中のホウ酸が析出する可能性が考えられる。通常運転温度域では、実機での実績からホウ酸水はZircaloy-4の酸化挙動に影響を及ぼさないと考えられるが、LOCAを想定した高温域におけるホウ酸とZircaloy-4との反応に係る知見は十分に得られていない。本研究では、固体ホウ酸を載せたZircaloy-4の板材を900Cまでの温度及び複数の雰囲気で酸化させることにより、固体ホウ酸の高温時挙動、ホウ酸とZircaloy-4との反応の有無、及びホウ酸がZircaloy-4の酸化挙動に及ぼす影響を調べた。実験結果から、高温酸化雰囲気においてZircaloy-4表面に固体ホウ酸の脱水により生成する無水ホウ酸が存在すると、この無水ホウ酸がZircaloy-4と雰囲気との接触を断つことでZircaloy-4の酸化を抑制することが示唆された。また、酸化膜付きZircaloy-4の表面に固体ホウ酸が付着し高温まで加熱された場合は、形成している酸化膜の空隙に無水ホウ酸が浸透することでその後の酸化を抑制することがうかがえた。

The Effect of oxidation and crystal phase condition on the ballooning and rupture behavior of Zircaloy-4 cladding tube-under transient-heating conditions

成川 隆文; 天谷 政樹

Journal of Nuclear Science and Technology, 53(1), p.112 - 122, 2016/01

https://doi.org/10.1080/00223131.2015.1025884

In order to investigate the effect of oxidation and crystal phase condition on the ballooning and rupture behaviors of cladding tube under simulated loss-of-coolant-accident (LOCA) conditions, laboratory-scale experiments were performed in which internally pressurized non-irradiated Zircaloy-4 (Zry-4) cladding specimens were heated to burst in steam and argon gas conditions. Values of the maximum circumferential strain were normalized by dividing them by engineering hoop stress at the time of rupture. The dependence of the normalized value on burst temperature and the relationship between the normalized value and the length, width and area of rupture opening were evaluated. The correlation between the normalized value and the burst temperature suggested that the fraction of the phase in Zry-4 cladding specimens affected the strain in the specimens and the oxidation of specimens suppressed the amount of ballooning of the specimens. The relationship between the normalized value and the length, width and area of rupture opening indicated that the length, width and area of rupture opening depended on the crystal phase condition in Zry-4 cladding specimens irrespective of atmosphere in the case of the heating rate of 3 K/s.

Effect of oxide film formed during -ray irradiation on pitting corrosion of fuel cladding in water containing sea salt

本岡 隆文; 塚田 隆

Proceedings of 2014 Nuclear Plant Chemistry Conference (NPC 2014) (USB Flash Drive), 9 Pages, 2014/10

福島第一原子力発電所(1F)では、2011年3月に海水が使用済燃料プールに注入された。ジルカロイ-2は1Fで燃料被覆管材として採用されているが、ジルカロイ-2を含むジルコニウム合金は、酸化性の塩化物水溶液で孔食の影響を受けやすい。本研究では、海水成分を含む水の放射線分解生成物が、ジルカロイ-2の孔食生起に及ぼす影響を調査した。線照射の前後に、海水成分を含有する水の組成変化を分析した。また、ジルカロイ-2の孔食電位測定を実施した。さらに、ジルカロイ-2表面に形成された酸化膜の特性をX線光電子分光法により評価した。海水成分を含む水の溶液分析では、線照射での過酸化水素の発生が示された。線照射下で皮膜形成したジルカロイ-2の孔食電位は非照射下のそれより高かった。ジルカロイ-2の酸化皮膜は酸化ジルコニウムであり、これは線照射中に厚くなることがわかった。線照射下で生成した皮膜を有するジルカロイ-2の孔食電位が高くなった原因は線照射下で酸化皮膜形成が進行することで説明された。

Results from studies on high burn-up fuel behavior under LOCA conditions

永瀬 文久; 更田 豊志

NUREG/CP-0192, p.197 - 230, 2005/10

LOCAに関する日本の安全基準は、事故条件を模擬した試験により決められた急冷時燃料棒破断限界に基づいている。このため、原研はLOCA条件を模擬した総合的な急冷実験を行い、高燃焼度燃料の破断限界を評価している。水素を添加した未照射被覆管やPWRにおいて39あるいは44GWd/tまで照射した高燃焼度燃料被覆管を用いた試験をこれまでに行った。破断限界は基本的に酸化量に依存し、初期水素濃度と急冷時の軸方向拘束力に伴い低下することが明らかになった。また、試験対象とした高燃焼度燃料被覆管の破断限界は、同等の水素濃度を有する未照射被覆管の破断限界とほぼ同等であることも明らかになった。

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。