SiC辐照损伤对耐高温氧化性能的影响

Effect of SiC Radiation Damage on High Temperature Oxidation Resistance

  • 摘要: 碳化硅(SiC)材料在高温氧化时会生成SiO2保护膜,但经辐照后高温氧化,材料结构和氧化速率会发生变化,影响材料性能。为研究其晶格损伤与氧化规律之间的关系,利用6H-SiC单晶片和烧结SiC多晶片,开展了在室温下经过能量为5 MeV、注量为5×1014 cm-2的Xe20+离子辐照后再进行1 300 ℃氧化1 h的实验。利用X射线衍射、拉曼光谱、傅里叶变换红外光谱、扫描电镜、透射电镜进行表征,对比了不同晶型的SiC氧化前后辐照与未辐照区域。结果显示:辐照破坏了晶格有序度,造成了晶格损伤,这些损伤在氧化过程中促进了多种SiO2基团的形成;生成的SiO2形成氧化层,由于与SiC基体热膨胀系数的差异,以及重结晶作用,导致碳化硅产生内应力,使氧化膜破裂;截面TEM图像显示,辐照引起的层错致使氧化程度加深,这是导致氧化速度加快的重要原因。

     

    Abstract: Silicon carbide (SiC) materials have many excellent properties, especially high temperature oxidation resistance, radiation resistance and low reaction activity in the presence of water vapor. In the future, it can be used as a new type of fuel cladding to replace zirconium alloy in light water reactor (LWR) and improve the structural integrity and safety of the reactor. However, when SiC materials are oxidized at high temperature after irradiation, the structure and oxidation rate of SiC materials will change, which will affect the properties. At present, it has been confirmed that the oxidation rate of SiC materials will increase after irradiation, but the specific reason is not clear. Therefore, the relationship between the lattice damage and the accelerated oxidation rate of SiC materials with different crystal forms after irradiation was studied. The experimental materials are 6H-SiC single wafer and SiC poly crystalline wafer, and they were irradiated by 5 MeV and fluence of 5×1014 cm-2 Xe20+ ions at room temperature. After that, the irradiated samples were oxidized by dry air at 1 300 ℃ for 1 h. The irradiated and unirradiated areas of SiC with different crystal forms before and after oxidation were compared by means of X-ray diffraction, Raman spectroscopy, Fourier transform infrared spectroscopy, scanning electron microscopy and transmission electron microscopy. The results show that irradiation destroys the lattice order and causes lattice damage. These damages promote the formation of a variety of SiO2 groups in the process of oxidation. Due to the difference of thermal expansion coefficient between SiO2 oxide layer and SiC matrix and recrystallization, SiC material produces internal stress. It leads to the rupture of SiO2 oxide film on the surface and accelerates the oxidation. In the process of oxidation, partial C atoms in SiC are replaced by O atoms, which will form gases such as CO, CH2 and so on. The gases spills out of SiC, and the pores formed on the surface also accelerate the oxidation. The cross-sectional TEM images show that the thickness of the oxide layer formed is about 140 nm. However, the thickness of the oxide layer is not uniform and the interface between the oxide layer and SiC is wavy in the local area. This shows that the defects formed after irradiation and oxidation provide an oxygen diffusion channel and promote the oxidation in the area near the stacking fault, which is an important reason for accelerating the oxidation rate.

     

/

返回文章
返回