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Fate of Plutonium at a Former Nuclear Testing Site in Australia

机译：a在澳大利亚前核试验场的命运

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摘要

A series of the British nuclear tests conducted on mainland Australia between 1953 and 1963 dispersed long-lived radioactivity and nuclear weapons debris including plutonium (Pu), the legacy of which is a long-lasting source of radioactive contamination to the surrounding biosphere. A reliable assessment of the environmental impact of Pu contaminants and their implications for human health requires an understanding of their physical/chemical characteristics at the molecular scale. In this study, we identify the chemical form of the Pu remaining in the local soils at the Taranaki site, one of the former nuclear testing sites at Maralinga, South Australia. We herein reveal direct spectroscopic evidence that the Pu legacy remaining at the site exists as particulates of Pu(Ⅳ) oxyhydroxide compounds, a very concentrated and low-soluble form of Pu, which will serve as ongoing radioactive sources far into the future. Gamma-ray spectrometry and X-ray fluorescence analysis on a collected Pu particle indicate that the Pu in the particle originated in the so-called "Minor trials" that involved the dispersal of weapon components by highly explosive chemicals, not in the nuclear explosion tests called "Major trials". A comprehensive analysis of the data acquired from X-ray fluorescence mapping (XFM), X-ray absorption near-edge structure (XANES), and extended X-ray absorption fine structure (EXAFS) suggests that the collected Pu particle forms a "core-shell" structure with the Pu(Ⅳ) oxyhydroxide core surrounded by an external layer containing Ca, Fe, and U, which further helps us to deduce a possible scenario of the physical/chemical transformation of the original Pu materials dispersed in the semiarid environment at Maralinga more than 50 years ago. These findings also highlight the importance of the comprehensive physical/chemical characterization of Pu contaminants for reliable environmental- and radiotoxicological assessment.
机译：1953年至1963年间，英国在澳大利亚大陆进行的一系列核试验散布了长期存在的放射性物质和包括weapons（Pu）在内的核武器碎片，其残留物是对周围生物圈的持久放射性污染源。要对Pu污染物的环境影响及其对人类健康的影响进行可靠的评估，需要了解其在分子尺度上的物理/化学特性。在这项研究中，我们确定了塔拉纳基（Taranaki）站点（南澳大利亚马拉林加的前核试验站点之一）的当地土壤中残留的Pu的化学形式。我们在这里揭示了直接的光谱学证据，即残留在现场的Pu残留物是以Pu（Ⅳ）羟基氧化物化合物的形式存在，Pu（Ⅳ）是一种非常浓缩和低溶解度的Pu，将作为未来的放射性源。对收集到的Pu粒子进行的伽马能谱分析和X射线荧光分析表明，粒子中的Pu起源于所谓的“次要试验”，该次要试验涉及通过高爆炸性化学物质扩散武器部件，而不是在核爆炸试验中进行。称为“重大审判”。对通过X射线荧光映射（XFM），X射线吸收近边缘结构（XANES）和扩展X射线吸收精细结构（EXAFS）采集的数据的综合分析表明，收集到的Pu颗粒形成了“核”。壳”结构，其Pu（Ⅳ）羟基氢氧化物核被包含Ca，Fe和U的外层包围，这进一步帮助我们推论了分散在半干旱环境中的原始Pu材料的物理/化学转变的可能情况50多年前在马拉林加（Maralinga）。这些发现还强调了对Pu污染物进行全面物理/化学表征对于可靠的环境和放射毒理学评估的重要性。

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  • 来源
    《Environmental Science & Technology》 |2016年第17期|9098-9104|共7页
  • 作者

    Atsushi Ikeda-Ohno; Lida Mokhber Shahin; Daryl L. Howard; Richard N. Collins; Timothy E. Payne; Mathew P. Johansen;

  • 作者单位

    Helmholtz-Zentrum Dresden-Rossendorf, Institute of Resource Ecology, Bautzner Landstrasse 400, 01328 Dresden, Germany,Institute for Environmental Research, Australian Nuclear Science and Technology Organisation, Locked Bag 2001, Kirrawee DC, New South Wales 2232, Australia,School of Civil and Environmental Engineering, The University of New South Wales, Sydney, New South Wales 2052, Australia;

    Institute for Environmental Research, Australian Nuclear Science and Technology Organisation, Locked Bag 2001, Kirrawee DC, New South Wales 2232, Australia;

    Australian Synchrotron, 800 Blackburn Road, Clayton, Victoria 3168, Australia;

    School of Civil and Environmental Engineering, The University of New South Wales, Sydney, New South Wales 2052, Australia;

    Institute for Environmental Research, Australian Nuclear Science and Technology Organisation, Locked Bag 2001, Kirrawee DC, New South Wales 2232, Australia;

    Institute for Environmental Research, Australian Nuclear Science and Technology Organisation, Locked Bag 2001, Kirrawee DC, New South Wales 2232, Australia;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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