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利用共振电离质谱法对乏核燃料颗粒中的裂变产物 Sr、Mo 和 Ru 进行同位素同时分析。

Simultaneous isotopic analysis of fission product Sr, Mo, and Ru in spent nuclear fuel particles by resonance ionization mass spectrometry.

机构信息

Lawrence Livermore National Laboratory, Nuclear and Chemical Sciences Division, Livermore, CA, USA.

Oak Ridge National Laboratory, Material Security and Counterproliferation, Nuclear Nonproliferation Division, Oak Ridge, TN, USA.

出版信息

Sci Rep. 2023 Mar 30;13(1):5193. doi: 10.1038/s41598-023-32203-5.

Abstract

Fission product Sr, Mo, and Ru isotopes in six 10-μm particles of spent fuel from a pressurized water reactor were analyzed by resonance ionization mass spectrometry (RIMS) and evaluated for utility in nuclear material characterization. Previous measurements on these same samples showed widely varying U, Pu, and Am isotopic compositions owing to the samples' differing irradiation environments within the reactor. This is also seen in Mo and Ru isotopes, which have the added complication of exsolution from the UO fuel matrix. This variability is a hindrance to interpreting data from a collection of particles with incomplete provenance since it is not always possible to assign particles to the same batch of fuel based on isotopic analyses alone. In contrast, the measured Sr/Sr ratios were indistinguishable across all samples. Strontium isotopic analysis can therefore be used to connect samples with otherwise disparate isotopic compositions, allowing them to be grouped appropriately for interpretation. Strontium isotopic analysis also provides a robust chronometer for determining the time since fuel irradiation. Because of the very high sensitivity of RIMS, only a small fraction of material in each of the 10 μm samples was consumed, leaving the vast majority still available for other analyses.

摘要

利用共振电离质谱法(RIMS)分析了压水堆中 6 个 10μm 废弃燃料颗粒中的裂变产物 Sr、Mo 和 Ru 同位素,并评估了它们在核材料特性表征中的应用。之前对这些相同样品的测量结果表明,由于反应堆内不同的辐照环境,U、Pu 和 Am 同位素组成存在广泛差异。Mo 和 Ru 同位素也存在这种情况,它们还存在从 UO 燃料基质中分离的额外复杂性。这种可变性对于解释来自具有不完整来源的颗粒集合的数据造成了阻碍,因为仅基于同位素分析,并非总是可以将颗粒分配到相同的燃料批次。相比之下,所有样品中的 Sr/Sr 比值都无法区分。因此,锶同位素分析可用于连接具有不同同位素组成的样品,以便对它们进行适当的分组进行解释。锶同位素分析还为确定燃料辐照后的时间提供了可靠的计时器。由于 RIMS 的灵敏度非常高,每个 10μm 样品中只有一小部分材料被消耗,而绝大多数材料仍可用于其他分析。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e294/10063544/8ecff18c5abb/41598_2023_32203_Fig1_HTML.jpg

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