High-Precision Measurement of the 238Pu/239Pu Isotope Ratio by TIMS,Journal of the American Society for Mass Spectrometry

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High-Precision Measurement of the 238Pu/239Pu Isotope Ratio by TIMS
Journal of the American Society for Mass Spectrometry ( IF 3.1 ) Pub Date : 2024-04-03 , DOI: 10.1021/jasms.4c00004
Preeti Goswami ₁ , K Sasi Bhushan ₁ , P G Jaison ₁

Affiliation

With an aim to improve the precision of isotopic standards of special nuclear materials like uranium and plutonium, National Bureau of Standards (NBS) undertook the recertification of isotopic standards prepared between 1960 and 1970. In a recent initiative, Lawrence Livermore National Laboratory (LLNL) in collaboration with New Brunswick Laboratory Program Office (NBL PO) undertaken efforts to recertify SRM 946, SRM 947, and SRM 948. The primary goal of this drive is to lower the uncertainties associated with the isotopic compositions of plutonium standards. The drive is also aims to minimize the uncertainty associated with measurement of the ²³⁸Pu content from 2% to ∼0.3%. In this connection, our laboratory at the Fuel Chemistry Division, Bhabha Atomic Research Centre, proposes a novel indicator “minima in the (R_MO^{254/(i + 16)})/(R_M^238/i) curve” (where i = m/z 233 or 235 amu), which is the ratio of the isotope ratio of metal oxides (²³⁸M¹⁶O/ⁱM¹⁶O) to that of metal ions (²³⁸M/ⁱM) of uranium in determining the accurate ²³⁸Pu content by thermal ionization mass spectrometry. Various enriched uranium spikes have been employed to study the efficacy of the minima in the (R_MO^{(254)/(i + 16)})/(R_M^238/i) curve. With the combination of monitoring the minima in the (R_MO^{(254)/(i + 16)})/(R_M^238/i) curve and the application of the ²³³U spike (with an isotope abundance of ²³⁸U ∼ 0.05%), an external precision of 0.2% has been achieved in the determination of the ²³⁸Pu/²³⁹Pu isotope ratio for isotopic standard SRM 947.

中文翻译：

利用 TIMS 高精度测量 238Pu/239Pu 同位素比

为了提高铀和钚等特殊核材料同位素标准的精度，国家标准局 (NBS) 对 1960 年至 1970 年间制定的同位素标准进行了重新认证。在最近的一项举措中，劳伦斯利弗莫尔国家实验室 (LLNL)与新不伦瑞克省实验室计划办公室 (NBL PO) 合作，努力重新认证 SRM 946、SRM 947 和 SRM 948。这一举措的主要目标是降低与钚标准品同位素成分相关的不确定性。该驱动力还旨在将²³⁸ Pu 含量测量相关的不确定性从 2% 降至约 0.3%。在这方面，我们巴巴原子研究中心燃料化学部的实验室提出了一个新指标“(R _MO ^{254/( i + 16)} )/(R _M ^{238/ i} ) 曲线中的最小值”（其中i = m / z 233 或 235 amu），是确定准确的²³⁸铀时金属氧化物（ ²³⁸ M ¹⁶ O/ ⁱ M ¹⁶ O）与金属离子（ ²³⁸ M/ ⁱ M）同位素比值的比值通过热电离质谱法测定Pu含量。已采用各种浓缩铀尖峰来研究 (R _MO ^{(254)/( i + 16)} )/(R _M ^{238/ i} ) 曲线中最小值的功效。结合监测 (R _MO ^{(254)/( i + 16)} )/(R _M ^{238/ i} ) 曲线中的最小值和应用²³³ U 尖峰（同位素丰度为²³⁸ U ∼ 0.05% ），同位素标准品SRM 947的²³⁸ Pu/ ²³⁹ Pu同位素比的测定达到了0.2%的外部精度。

更新日期：2024-04-03

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