University of Natural Resources and Life Sciences Vienna, Department of Chemistry, Division of Analytical Chemistry, VIRIS-Laboratory, Konrad-Lorenz-Strasse 24, 3430 Tulln, Austria.
J Environ Radioact. 2012 Nov;113(8):8-15. doi: 10.1016/j.jenvrad.2012.03.017. Epub 2012 May 16.
We present the application of nanosecond laser ablation (LA) coupled to a 'Nu Plasma HR' multi collector inductively coupled plasma mass spectrometer (MC-ICP-MS) for the direct analysis of U isotope ratios in single, 10-20 μm-sized, U-doped glass particles. Method development included studies with respect to (1) external correction of the measured U isotope ratios in glass particles, (2) the applied laser ablation carrier gas (i.e. Ar versus He) and (3) the accurate determination of lower abundant (236)U/(238)U isotope ratios (i.e. 10(-5)). In addition, a data processing procedure was developed for evaluation of transient signals, which is of potential use for routine application of the developed method. We demonstrate that the developed method is reliable and well suited for determining U isotope ratios of individual particles. Analyses of twenty-eight S1 glass particles, measured under optimized conditions, yielded average biases of less than 0.6% from the certified values for (234)U/(238)U and (235)U/(238)U ratios. Experimental results obtained for (236)U/(238)U isotope ratios deviated by less than -2.5% from the certified values. Expanded relative total combined standard uncertainties U(c) (k = 2) of 2.6%, 1.4% and 5.8% were calculated for (234)U/(238)U, (235)U/(238)U and (236)U/(238)U, respectively.
我们展示了纳秒激光烧蚀(LA)与“Nu Plasma HR”多接收电感耦合等离子体质谱仪(MC-ICP-MS)相结合,直接分析单个 10-20μm 大小、掺杂 U 的玻璃颗粒中的 U 同位素比值的应用。方法开发包括以下几个方面的研究:(1)对玻璃颗粒中测量的 U 同位素比值进行外部校正;(2)应用的激光烧蚀载气(即 Ar 与 He);(3)准确测定低丰度(236)U/(238)U 同位素比值(即 10-5)。此外,还开发了一种数据处理程序,用于评估瞬态信号,这对于开发方法的常规应用具有潜在的用途。我们证明了所开发的方法是可靠的,非常适合于确定单个颗粒的 U 同位素比值。在优化条件下测量的 28 个 S1 玻璃颗粒,其(234)U/(238)U 和(235)U/(238)U 比值的平均偏差小于认证值的 0.6%。(236)U/(238)U 同位素比值的实验结果偏差小于认证值的-2.5%。(234)U/(238)U、(235)U/(238)U 和(236)U/(238)U 的相对总扩展标准不确定度 U(c)(k = 2)分别计算为 2.6%、1.4%和 5.8%。