Quantitative prediction of rare earth concentrations in salt matrices using laser-induced breakdown spectroscopy for application to molten salt reactors and pyroprocessing
Quantitative prediction of rare earth concentrations in salt matrices using laser-induced breakdown spectroscopy for application to molten salt reactors and pyroprocessing
复制标题
使用激光诱导击穿光谱定量预测盐基体中的稀土浓度，应用于熔盐反应堆和高温处理
DOI：
10.1039/d0ja00352b
复制
发表时间：
2021
影响因子：
3.4
通讯作者：
Hull G
中科院分区：
文献类型：
--
作者：
Hull G
乏核燃料的热处理是一种电化学分离方法，将乏金属燃料溶解在熔盐浴中，使铀(U)和钚（Pu）与裂变产物（FPs）和其他杂质分离。这使得有用的材料可以在混合氧化物燃料（MOx）中重复使用，或者进一步提炼成新的反应堆燃料。监测熔盐容器内U、Pu、FPs和其他物质浓度的变化是一个独特的挑战，激光诱导击穿光谱（LIBS）可能能够克服这一挑战，因为它能够使用一次测量同时分析多种元素，并具有原位隔离能力。本文用LIBS对LiCl + KCl共晶（LKE）盐中的镨（Pr）、钬（Ho）和铒（Er）氯（LnCl3）样品进行了分析。为了最大限度地提高信号与背景比，对多个激光脉冲能量进行了测试，在最低脉冲能量为85 mJ /脉冲时获得了最佳效果。使用前向区间偏最小二乘（iPLS）回归建立每种元素的预测浓度与测量浓度模型。该方法获得的交叉验证均方根误差（RMSECV）值在3.20 × 10−3和16.3 × 10−3 mmmolln gLKE−1之间，在所有三种镧系元素混合样品的交叉验证均方根误差为2.84 × 10−3和7.62 × 10−3 mmmolln gLKE−1之间。在1000和9000 ppm之间的定量限表明，LIBS应该是一个候选的在线分析在热处理过程中的元素浓度。
Pyroprocessing of spent nuclear fuels is an electrochemical separation method where spent metallic fuel is dissolved in a molten salt bath to allow uranium (U) and plutonium (Pu) to be isolated from fission products (FPs) and other impurities. This allows the useful materials to be reused in mixed oxide fuel (MOx) or further refined to new reactor fuel. Monitoring the changing concentrations of U, Pu, FPs and other species inside a molten salt vessel presents a unique challenge which laser-induced breakdown spectroscopy (LIBS) may be able to overcome, due to its ability to simultaneously analyse multiple elements using a single measurement with stand-off capability in situ. In this study, samples of praseodymium (Pr), holmium (Ho) and erbium (Er) chloride (LnCl3) in LiCl + KCl eutectic (LKE) salt were analysed with LIBS. Multiple laser pulse energies were tested to maximise the signal to background ratio, the best results were obtained at the lowest pulse energy of 85 mJ per pulse. Forward interval Partial Least Squares (iPLS) regression was used to create predicted versus measured concentration models for each element. This method achieved Root Mean Squared Error of Cross Validation (RMSECV) values of between 3.20 × 10−3 and 16.3 × 10−3 mmolLn gLKE−1 for single lanthanide samples and 2.84 × 10−3 and 7.62 × 10−3 mmolLn gLKE−1 for mixed samples of all three lanthanide elements. Limits of quantification of between 1000 and 9000 ppm suggest LIBS should be a candidate for on-line analysis of elemental concentrations during pyroprocessing.
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DOI：
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发表时间：
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期刊：
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