| Autor: |
Manard BT; Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States., Quarles CD Jr; Elemental Scientific Inc, Omaha, Nebraska 68122, United States., Bradley VC; Laser Technologies Group, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States., Spano TL; Nuclear Nonproliferation Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States., Zirakparvar NA; Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States., Ticknor BW; Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States., Dunlap DR; Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States., Cable-Dunlap P; Nuclear Nonproliferation Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States., Hexel CR; Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States., Andrews HB; Radioisotope Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States. |
| Abstrakt: |
Uranyl fluoride (UO 2 F 2 ) particles (<20 μm) were subjected to first-of-its-kind analysis via simultaneous laser-induced breakdown spectroscopy (LIBS) and laser ablation multi-collector inductively coupled plasma-mass spectrometry (LA-MC-ICP-MS). Briefly, a nanosecond pulsed high-energy laser was focused onto the sample (particle) surface. In a single laser pulse, the UO 2 F 2 particle was excited/ionized within the microplasma volume, and the emission of light was collected via fiber optics such that emission spectroscopy could be employed for the detection of uranium (U) and fluorine (F). The ablated particle was simultaneously transported into the MC-ICP-MS for high precision isotopic (i.e., 234 U, 235 U, and 238 U) analysis. This method, LIBS/LA-MC-ICP-MS was optimized and employed to rapidly measure 80+ UO 2 F 2 particles, which were subjected to different calcination processes, which results in varying degrees of F loss from the individual particles. In measuring the particles, the average F/U ratios for the populations treated at 100 and 500 °C were 2.78 ± 1.28 and 1.01 ± 0.50, respectively, confirming loss of F through the calcination process. The average 235 U/ 238 U on the particle populations for the 100 and 500 °C were 0.007262 (22) and 0.007231 (23), which was determined to be <0.2% from the expected value. The 234 U/ 238 U ratios on the same particles were 0.000053 (11) and 0.000050 (10) for the 100 and 500 °C, respectively, <10% from the expected value. Notably, each population was analyzed in under 5 min, demonstrating the truly rapid analysis technique presented here. |
