包壳破损对燃料包壳化学相互作用层和裂变产物行为的影响研究

Effect of Cladding Failure on FCCI Layer and Fission Product Behavior

  • 摘要: 了解完整和破损燃料棒不同的燃料包层化学相互作用(FCCI)层和裂变产物分布特征,对于预测压水堆(PWR)燃料棒在服役期间和服役后的性能以及设计乏燃料后处理工艺等至关重要。本文通过屏蔽型电子探针显微分析(EPMA)技术,对来自商用压水堆核电站的燃耗为45 GW·d/tU的完整燃料棒和燃耗为41 GW·d/tU的破损燃料棒的FCCI层进行了系统的分析。实验结果显示,完整燃料棒的FCCI层成分均匀,主要由ZrO2−x组成。而破损燃料棒FCCI层存在明显的分层现象,高温蒸汽的进入促使ZrO2−x层和UO2芯块之间形成了(U, Zr)O2−x层以及U、Zr元素过渡层。两种燃料棒在裂变产物元素分布上也有所不同,完整棒中Mo、Ru和Pd等元素主要存在于芯块和FCCI层反冲范围内,而破损棒中Mo元素在整个FCCI层中均有所分布,表明包壳失效造成的更高氧含量和更大温度梯度能够显著促进裂变产物Mo元素从芯块向外的迁移。

     

    Abstract: Nuclear fuel rods are the first barrier preventing the release of fission products to the environment in the operation of nuclear power plants. Zirconium alloys are favored for their advantages, such as a low neutron absorption cross-section, excellent mechanical properties, and corrosion resistance, making them commonly used as cladding materials for UO2 fuel in pressurized water reactors (PWRs). During reactor operation, a robust fuel-cladding chemical interaction (FCCI) layer forms upon contact between UO2 fuel and zirconium alloy cladding. Furthermore, UO2 fuel will produce a large number of fission products during operation. The accumulation of fission products can change the chemical environment inside the fuel rods, and may also affect the chemical composition and structural stability of FCCI layer and cladding. Understanding the different FCCI layers and fission product distribution characteristics of intact and damaged fuel rods is crucial for predicting the performance of PWR fuel rods during and after service, and designing spent fuel reprocessing technology. The FCCI layer of an intact fuel rod with a burnup of 45 GW·d/tU and a leak fuel rod with a burnup of 41 GW·d/tU from a commercial PWR was systematically analyzed by shielded electron probe microanalysis (EPMA) technique. The experimental results show that the FCCI layer of the intact fuel rod is composed of ZrO2−x. The FCCI layer of the leak fuel rod presents an obvious stratification phenomenon. The entry of high-temperature steam promotes the formation of a (U, Zr)O2−x layer and a transition layer of U and Zr elements between the ZrO2−x layer and UO2 pellet. The two fuel rods also differ in the distribution of fission product elements. In the intact rod, elements such as Mo, Ru and Pd mainly exist in the pellet and the recoil range of the FCCI layer, while in the leak rod, Mo element is distributed in the whole FCCI layer. The results show that the higher oxygen content and larger temperature gradient caused by cladding failure can significantly promote the outward migration of Mo element from the pellet.

     

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