ウラン同位体とフッ素の同時検出が核不拡散監視を前進させる(Simultaneous detection of uranium isotopes, fluorine advances nuclear nonproliferation monitoring)

2004-09-26 オークリッジ国立研究所(ORNL)

＜関連情報＞

• https://www.ornl.gov/news/simultaneous-detection-uranium-isotopes-fluorine-advances-nuclear-nonproliferation-monitoring
• https://pubs.acs.org/doi/full/10.1021/jacs.4c03965

レーザー誘起ブレークダウン分光法/レーザーアブレーション-マルチコレクター-誘導結合プラズマ質量分析法によるフッ素とウランの同位体同時決定のためのウラン単一粒子分析 Uranium Single Particle Analysis for Simultaneous Fluorine and Uranium Isotopic Determinations via Laser-Induced Breakdown Spectroscopy/Laser Ablation–Multicollector–Inductively Coupled Plasma–Mass Spectrometry

Benjamin T. Manard,C. Derrick Quarles Jr,Veronica C. Bradley,Tyler L. Spano,N. Alex Zirakparvar,Brian W. Ticknor,Daniel R. Dunlap,Paula Cable-Dunlap,Cole R. Hexel,Hunter B. Andrews
Journal of the American Chemical Society  Published: May 8, 2024
DOI:https://doi.org/10.1021/jacs.4c03965

Abstract

Uranyl fluoride (UO₂F₂) 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 UO₂F₂ 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., ²³⁴U, ²³⁵U, and ²³⁸U) analysis. This method, LIBS/LA–MC–ICP–MS was optimized and employed to rapidly measure 80+ UO₂F₂ 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 ²³⁵U/²³⁸U 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 ²³⁴U/²³⁸U 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.