Oak Ridge National Laboratory, Chemical Sciences Division, 1 Bethel Valley Rd, Oak Ridge, Tennessee 37830, United States.
Anal Chem. 2021 Aug 17;93(32):11133-11139. doi: 10.1021/acs.analchem.1c01569. Epub 2021 Jul 8.
The ability to directly measure uranium isotope ratios on environmental swipes has been achieved through a solution-based microextraction process and represents a significant advancement toward the development of a rapid method to analyze international nuclear safeguard samples. Here, a microextraction probe is lowered and sealed onto the swipe surface, and analytes within the sampling site (∼8 mm) are dissolved and extracted into a flowing solvent of 2% nitric acid (HNO). The mobilized species are subsequently directed into an inductively coupled plasma-mass spectrometer (ICP-MS) for accurate and precise isotope ratio determination. This work highlights the novelty of the sampling mechanism, particularly with the direct coupling of the microextraction probe to the ICP-MS and measurement of uranium isotope ratios. The preliminary method detection limit for the microextraction-ICP-MS method, utilizing a quadrupole-based MS, was determined to be ∼50 pg of U. Additionally, precise and accurate isotope ratio measurements were achieved on uranium reference materials for both the major (U/U) and minor (U/U and U/U) ratios. While the present work is focused on directly measuring uranium isotopic systems on swipe surfaces for nuclear safeguards and verification applications, the benefits would extend across many applications in which direct solid sampling is sought for elemental and isotopic analysis.
已经通过基于溶液的微萃取过程实现了直接测量环境拭子中铀同位素比的能力,这是朝着开发快速分析国际核保障样品的方法迈出的重要一步。在这里,将微萃取探头降低并密封到拭子表面上,然后将采样点(约 8 毫米)内的分析物溶解并萃取到 2%硝酸(HNO3)的流动溶剂中。随后,将被移动的物质引导到电感耦合等离子体质谱仪(ICP-MS)中,以进行准确和精确的同位素比测定。这项工作突出了采样机制的新颖性,特别是微萃取探头与 ICP-MS 的直接耦合以及铀同位素比的测量。利用基于四极杆的 MS,微萃取-ICP-MS 方法的初步方法检测限被确定为约 50 pg U。此外,还对铀参考物质进行了精确和准确的同位素比测量,包括主要(U/U)和次要(U/U 和 U/U)比值。虽然目前的工作重点是直接测量拭子表面上的铀同位素系统,用于核保障和核查应用,但这一成果将扩展到许多寻求直接进行固体采样进行元素和同位素分析的应用领域。