Non-destructive assay of plutonium in absence of gamma-ray spectrometry

IF 16.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Accounts of Chemical Research Pub Date : 2024-02-14 DOI:10.1515/ract-2023-0193

Sanhita Chaudhury, Ashwani Kumar, Sabyasachi Patra, Rahul Tripathi

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Abstract

Gamma-ray spectrometry-based isotopic composition analysis is a prerequisite for absolute non-destructive assay of Pu by neutron counting or calorimetry. However, gamma-ray spectrometry can be complicated in samples that are heavily shielded or have a high 241Am fraction. Herein, for the absolute non-destructive assay of Pu, a simple yet potent empirical methodology combining neutron multiplicity counting and calorimetry is proposed, which obviates the need for gamma-ray spectrometry-based isotopic composition analysis. The approach includes stepwise correlation between the parameters obtained from neutron multiplicity counting, i.e., α ((α, n) neutron to spontaneous fission neutron ratio), effective mass of 240Pu, and D (doubles neutron rate) with the thermal power output (W Pu) due to radioactive decay (measured by calorimetry). Because D and W Pu both are governed by the Pu isotopic composition, their correlation should be sensitive to the isotopic information in a given sample. Mandatory correction for the 241Am contribution in W Pu was done using the linear plot between its weight fraction and the corresponding α. The proposed methodology was validated by analyzing several PuO2 standards containing high 241Am fraction (0.02–0.09). The measured Pu amounts were within 8 % of the actual values with measurement uncertainties between 8 and 10 %, which shows the potential of the proposed methodology for the assay of samples having high 241Am content or for the quantification of Pu in heavily shielded samples.

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在没有伽马射线光谱仪的情况下对钚进行无损检测

基于伽马射线光谱法的同位素组成分析是通过中子计数法或量热法对钚进行绝对无损化验的先决条件。然而，对于屏蔽较强或 241Am 含量较高的样品，伽马射线光谱分析可能比较复杂。本文提出了一种结合中子倍率计数法和量热法的简单而有效的经验方法，用于钚的绝对无损检测，从而避免了基于伽马射线光谱法的同位素组成分析。该方法包括逐步将中子倍率计数获得的参数，即α（（α，n）中子与自发裂变中子比）、240Pu 的有效质量和 D（倍率中子）与放射性衰变产生的热功率输出（W Pu）（通过量热计测量）进行关联。由于 D 和 W Pu 都受 Pu 同位素组成的影响，因此它们之间的相关性对特定样品中的同位素信息非常敏感。通过分析几种含有高 241Am 分数（0.02-0.09）的二氧化钚标准样品，对所提出的方法进行了验证。测得的钚含量在实际值的 8% 以内，测量不确定性在 8% 到 10% 之间，这表明所提出的方法有潜力用于检测 241Am 含量较高的样品或用于定量重屏蔽样品中的钚。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Accounts of Chemical Research 化学-化学综合

CiteScore

31.40

自引率

1.10%

发文量

312

审稿时长

2 months

期刊介绍： Accounts of Chemical Research presents short, concise and critical articles offering easy-to-read overviews of basic research and applications in all areas of chemistry and biochemistry. These short reviews focus on research from the author’s own laboratory and are designed to teach the reader about a research project. In addition, Accounts of Chemical Research publishes commentaries that give an informed opinion on a current research problem. Special Issues online are devoted to a single topic of unusual activity and significance. Accounts of Chemical Research replaces the traditional article abstract with an article "Conspectus." These entries synopsize the research affording the reader a closer look at the content and significance of an article. Through this provision of a more detailed description of the article contents, the Conspectus enhances the article's discoverability by search engines and the exposure for the research.