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Raman spectroscopy coupled to principal component analysis for studying UO2 nuclear fuels with different grain sizes due to the chromia addition

机译:拉曼光谱耦合到基于Chromia添加引起的不同粒度的UO2核燃料的主成分分析

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Current necessities of nuclear power plants have led to increase burn-up of the fuel during operation. In this context, some undesirable processes, such as a higher release of gaseous fission products, may occur. New UO2-based fuels are being developed by adding doping agents. Chromia (Cr2O3) has proved to considerably enhance grain growth during sintering, and thus promote the retention of these fission products. The study of these Cr-doped UO2 fuels at in situ conditions would allow testing the real performance of the fuel in operating conditions. The existence of Raman portable instruments makes this scenario feasible. But first, the measurement protocols need to be developed. Therefore, in this paper, we explore the use of Raman spectroscopy as an approach for the analysis of the effect of Cr2O3 addition in a set of UO2-Cr2O3 sintered pellets. The validity of Raman is demonstrated by using Principal Component Analysis (PCA). Three Principal Components describe 98.8% of the total variance of the data, and they are related to the main Raman modes of the samples. In addition, SEM images have shown the presence of bigger precipitates of Cr2O3 not only when the solubility limit of Cr3+ is exceeded, but also when it is not reached. By XRD, the well-known Vegard behavior is observed, and a solubility limit of Cr3+ dissolved into the UO2 matrix is found to be (748 +/- 16) ppm for the particular sintering conditions used. (C) 2020 The Authors. Published by Elsevier B.V.
机译:目前核电站的需求导致运行期间燃料的燃耗增加。在这种情况下,可能会发生一些不希望发生的过程,例如气体裂变产物的更高释放。通过添加掺杂剂,正在开发新的UO2基燃料。事实证明,氧化铬(Cr2O3)能显著促进烧结过程中的晶粒生长,从而促进这些裂变产物的保留。在原位条件下对这些掺铬UO2燃料的研究将有助于测试燃料在运行条件下的实际性能。拉曼便携式仪器的存在使这一设想成为可能。但首先,需要制定测量协议。因此,在本文中,我们探索了使用拉曼光谱作为一种方法来分析在UO2-Cr2O3烧结球团中添加Cr2O3的效果。利用主成分分析(PCA)验证了拉曼光谱的有效性。三个主成分描述了数据总方差的98.8%,它们与样品的主要拉曼模式有关。此外,SEM图像显示,不仅当Cr3+的溶解度超过极限时,而且当未达到极限时,Cr2O3的沉淀更大。通过XRD,观察到了众所周知的Vegard行为,发现在所用的特定烧结条件下,溶解在UO2基体中的Cr3+的溶解度极限为(748+/-16)ppm。(C) 2020年,作者。由Elsevier B.V.出版。

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