Detection of 238Pu at picogram quantities by laser resonance ionization mass spectrometry

IF 1.6 3区化学 Q3 PHYSICS, ATOMIC, MOLECULAR & CHEMICAL

International Journal of Mass Spectrometry Pub Date : 2024-03-07 DOI:10.1016/j.ijms.2024.117236

Peng-fei Zhang, Zhi-ming Li, Wen-liang Wang, lei Feng, Jiang Xu, Man-chao Zhang, Xiao-pan Shen, Xiang-long Yuan, Fei-teng Li, Hu Deng, Li-hua Zhai

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Abstract

Based on the laser resonance ionization mass spectrometry (LRIMS) developed in the laboratory, a preliminary method was established to determine Pu isotope ratios. A three-color-three-photon resonance ionization scheme was confirmed, and the laser wavelengths of each excitation/ionization step were λ₁ = 586.654 nm, λ₂ = 606.181 nm and λ₃ = 642.722 nm. The selective ionization of ²³⁸Pu/²³⁸U was realized by testing the Pu and U mixed sample, a selectivity ratio of over 10⁷ was obtained. More effective electrothermal atomization of Pu was implemented by loading graphene oxide solution on the Pu sample surface, and the total detection efficiency of ∼40 ng Pu sample was above 3 × 10⁻⁴, which was three orders of magnitude higher than the efficiency of the unloaded graphene oxide solution Pu sample. Results showed that the relative standard deviation of ²³⁸Pu/²³⁹Pu ratio was ∼0.20%, indicating that LRIMS could effectively avoid the isobaric interference of ²³⁸U faced by other commercial mass spectrometers such as TIMS and ICP-MS, and could achieve precise measurement of ²³⁸Pu/²³⁹Pu ratio.

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利用激光共振电离质谱法检测微微克级的 238Pu

基于实验室开发的激光共振电离质谱仪，初步建立了测定钚同位素比值的方法。确定了三色三光子共振电离方案，各激发/电离步骤的激光波长分别为 λ = 586.654 nm、λ = 606.181 nm 和 λ = 642.722 nm。通过测试钚和铀混合样品，实现了钚/铀的选择性电离，获得了超过 10 的选择性比。通过在 Pu 样品表面负载氧化石墨烯溶液，实现了更有效的 Pu 电热雾化，∼40 ng Pu 样品的总检测效率超过 3 × 10，比未负载氧化石墨烯溶液的 Pu 样品的效率高三个数量级。结果表明，钚/钚比值的相对标准偏差为∼0.20%，表明 LRIMS 能有效避免 TIMS 和 ICP-MS 等其他商用质谱仪所面临的 U 的等压干扰，实现了钚/钚比值的精确测量。

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来源期刊

International Journal of Mass Spectrometry 物理-光谱学

CiteScore

3.60

自引率

5.60%

发文量

145

审稿时长

71 days

期刊介绍： The journal invites papers that advance the field of mass spectrometry by exploring fundamental aspects of ion processes using both the experimental and theoretical approaches, developing new instrumentation and experimental strategies for chemical analysis using mass spectrometry, developing new computational strategies for data interpretation and integration, reporting new applications of mass spectrometry and hyphenated techniques in biology, chemistry, geology, and physics. Papers, in which standard mass spectrometry techniques are used for analysis will not be considered. IJMS publishes full-length articles, short communications, reviews, and feature articles including young scientist features.