Direct detection and isotope analysis of individual particles in suspension by single particle mode MC-ICP-MS for nuclear safety
Direct detection and isotope analysis of individual particles in suspension by single particle mode MC-ICP-MS for nuclear safety
复制标题
通过单颗粒模式 MC-ICP-MS 对悬浮液中的单个颗粒进行直接检测和同位素分析，以实现核安全
DOI：
10.1039/c4ja00339j
复制
发表时间：
2015-01-01
影响因子：
3.4
通讯作者：
Ren Xiangjun
中科院分区：
文献类型：
--
作者：
Su Yongyang;Wang Wei;Ren Xiangjun
单个粒子携带的同位素指纹信息在核安全、核保障和核环境方面具有重要价值。已经开发了多种技术，例如单颗粒模式 ICP-MS、激光烧蚀 ICP-MS 和 LA-MC-ICP-MS，用于直接检测或对固体样品中的单个颗粒进行同位素分析。在本研究中，提出了单颗粒模式 MC-ICP-MS 用于悬浮液中单个颗粒的精确同位素测量。将具有天然同位素丰度的氧化铒粉末用作铀粒子替代物，将其分散在超纯水中以制备悬浮液样品。铒同位素范围可以涵盖不同浓缩水平的铀同位素。在粒子分析之前和之后雾化铒溶液以确定质谱仪中的质量偏差因子。将亚微米级铒粒子雾化，然后引入ICP炬以单粒子模式进行检测和同位素测量。根据脉冲强度直方图，估计球形等效物理直径约为 226 nm，164Er 量为 7 × 10−16 g。使用逐点（PBP）和线性回归斜率（LRS）两种数据处理策略来确定铒同位素比率。结果表明，PBP法测定170Er/166Er、168Er/166Er和167Er/166Er比值的精度分别为5.5%、4.6%和3.9%。这些测量的同位素比值经过质量偏差校正后的相对误差在 0.2-4% 之间。由于164Er信号较弱，164Er/166Er比值的精度和准确度较差。通过LRS方法，测定170Er/166Er、168Er/166Er、167Er/166Er和164Er/166Er比值的精度至少提高了一个数量级。 170Er/166Er、168Er/166Er、167Er/166Er比值精度优于0.3%。 164Er/166Er比值的精度和准确度显着提高。此外，还可以确定10−3水平的162Er/166Er比值。该技术适用于尺寸范围为 130 nm–3 μm 的颗粒的检测和同位素分析。样品制备过程简单，消除了可能的污染。该技术结合了快速筛选、灵敏检测和单个粒子的同位素识别。
Isotopic fingerprint information carried by an individual particle is of great value in nuclear safety, nuclear safeguards, and nuclear environment. Several techniques, such as single particle mode ICP-MS, laser ablation ICP-MS and LA-MC-ICP-MS, have been developed for direct detection or isotope analysis of individual particles in the solid sample. In this study, single particle mode MC-ICP-MS was proposed for the precise isotopic measurement of individual particles in suspension. Erbium oxide powder with natural isotopic abundance used as uranium particle surrogate was dispersed in ultrapure water to prepare a suspension sample. Uranium isotope at different enrichment levels could be covered by the erbium isotope range. Erbium solution was nebulized before and after particle analysis to determine the mass bias factors in the mass spectrometer. The submicron-sized erbium particle was nebulized and then introduced into the ICP torch for detection and isotopic measurement in single particle mode. From the histogram of pulse intensities, the spherical equivalent physical diameter was estimated to be around 226 nm with 164Er amount of 7 × 10−16 g. Two data processing strategies, point by point (PBP) and linear regression slope (LRS), were used to determine the erbium isotope ratios. Results show that the precisions of 170Er/166Er, 168Er/166Er, and 167Er/166Er ratios determined by PBP method are 5.5%, 4.6% and 3.9%, respectively. The relative errors of these measured isotope ratios after mass bias correction lies between 0.2–4%. The precision and accuracy of 164Er/166Er ratio are worse due to the weak signal of 164Er. By LRS method, the precisions of determined 170Er/166Er, 168Er/166Er, 167Er/166Er and 164Er/166Er ratios improved by one order of magnitude at least. The precisions of 170Er/166Er, 168Er/166Er and 167Er/166Er ratios are better than 0.3%. The precision and accuracy of the 164Er/166Er ratio are significantly improved. Moreover, the 162Er/166Er ratio at 10−3 level could also be determined. The proposed technique is suitable for the detection and isotope analysis of particles with size range of 130 nm–3 μm. The sample preparation process is simple, which eliminates possible contamination. The technique combines fast screening, sensitive detection, and isotopic identification of an individual particle.