Characterization of un-irradiated MIMAS MOX fuel by Raman spectroscopy and EPMA

Characterization of un-irradiated MIMAS MOX fuel by Raman spectroscopy and EPMA
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通过拉曼光谱和 EPMA 表征未辐照的 MIMAS MOX 燃料

DOI:
10.1016/j.jnucmat.2017.11.014
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发表时间:
2018
影响因子:
3.1
通讯作者:
C. Jegou
C. Jegou
中科院分区:
工程技术2区
文献类型:
--
作者:
Z. Talip;S. Peuget;M. Magnin;M. Tribet;C. Valot;Romain Vauchy;C. Jegou

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在这项研究中,拉曼光谱技术的实施,以表征未辐照的MIMAS(微粉化-MASter共混物)混合氧化物燃料样品平均7重量%,钚含量和不同的损伤水平,13年后的制造,热恢复后一年和退火后不久,分别。评估了局部钚含量、化学计量偏差和自辐射损伤对所研究的MIMAS MOX样品的拉曼光谱的影响。MIMAS MOX燃料具有三个不同的相:富钚团块、包覆相和铀基体。为了区分这些阶段,拉曼结果与电子探针分析进行钚含量测量。拉曼结果表明,当Pu含量从0.2wt. %增加到25wt. %时,T2g频率从445 cm-1显著移动到453 cm-1。这些数据与用Gruneisen参数得到的计算结果令人满意地一致。T2g带的位置主要受钚含量和自辐射损伤的控制。偏离化学计量对T2g带位置没有显著影响。自辐射损伤导致T2g带向较低频率移动(对于损伤样品的UO2基体为1.1 - 2 cm − 1)。然而,这种转变是难以量化的涂层相和钚团聚体的高钚浓度的分散体。此外,525 cm-1带,这归因于亚化学计量结构缺陷,是第一次为自辐射损伤的MOX样品。由于各相的抗氧化性不同,因此激光诱导氧化可以交替地用于识别相。它表明,显微拉曼光谱是一种有效的技术,用于表征非均相MOX样品,由于其低的空间分辨率。
In this study, Raman spectroscopy technique was implemented to characterize un-irradiated MIMAS (MIcronized - MASter blend) MOX fuel samples with average 7 wt.% Pu content and different damage levels, 13 years after fabrication, one year after thermal recovery and soon after annealing, respectively. The impacts of local Pu content, deviation from stoichiometry and self-radiation damage on Raman spectrum of the studied MIMAS MOX samples were assessed. MIMAS MOX fuel has three different phases Pu-rich agglomerate, coating phase and uranium matrix. In order to distinguish these phases, Raman results were associated with Pu content measurements performed by Electron Microprobe Analysis. Raman results show that T2gfrequency significantly shifts from 445 to 453 cm−1for Pu contents increasing from 0.2 to 25 wt.%. These data are satisfactorily consistent with the calculations obtained with Gruneisen parameters. It was concluded that the position of the T2gband is mainly controlled by Pu content and self-radiation damage. Deviation from stoichiometry does not have a significant influence on T2gband position. Self-radiation damage leads to a shift of T2gband towards lower frequency (∼1–2 cm−1for the UO2matrix of damaged sample). However, this shift is difficult to quantify for the coating phase and Pu agglomerates given the dispersion of high Pu concentrations. In addition, 525 cm−1band, which was attributed to sub-stoichiometric structural defects, is presented for the first time for the self-radiation damaged MOX sample. Thanks to the different oxidation resistance of each phase, it was shown that laser induced oxidation could be alternatively used to identify the phases. It is demonstrated that micro-Raman spectroscopy is an efficient technique for the characterization of heterogeneous MOX samples, due to its low spatial resolution.
DOI: 10.1016/c2017-1-02873-8
发表时间: 2012
期刊: --
影响因子: --
作者:
R. Konings
通讯作者: R. Konings