Flow electrolytic separation of radionuclides for interference suppression in γ-spectrometry

IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Analytica Chimica Acta Pub Date : 2024-12-12 DOI:10.1016/j.aca.2024.343527
Paul Dutheil, Martin Heule, Fabian Köhler, Sandra Baur, Alexander Vögele, Patrick Steinegger
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In this case a complex chemical separation is required to remove interfering radionuclides prior to <span><span style=\"\"></span><span data-mathml='&lt;math xmlns=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;mi is=\"true\"&gt;&amp;#x3B3;&lt;/mi&gt;&lt;/math&gt;' role=\"presentation\" style=\"font-size: 90%; display: inline-block; position: relative;\" tabindex=\"0\"><svg aria-hidden=\"true\" focusable=\"false\" height=\"1.855ex\" role=\"img\" style=\"vertical-align: -0.697ex;\" viewbox=\"0 -498.8 543.5 798.9\" width=\"1.262ex\" xmlns:xlink=\"http://www.w3.org/1999/xlink\"><g fill=\"currentColor\" stroke=\"currentColor\" stroke-width=\"0\" transform=\"matrix(1 0 0 -1 0 0)\"><g is=\"true\"><use xlink:href=\"#MJMATHI-3B3\"></use></g></g></svg><span role=\"presentation\"><math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mi is=\"true\">γ</mi></math></span></span><script type=\"math/mml\"><math><mi is=\"true\">γ</mi></math></script></span>-spectrometric analysis. Several radionuclides such as, <sup>110m</sup>Ag, <sup>124,125</sup>Sb, <sup>113</sup>Sn and <sup>123m</sup>Te are of relevance for radioanalytical analysis in nuclear facilities. These may be readily electrodeposited at controlled-potential using flow electrolysis in aqueous solution. Here, the development and use of flow electrolysis for the pre-analytical separation of different radionuclides to suppress interferences in <span><span style=\"\"></span><span data-mathml='&lt;math xmlns=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;mi is=\"true\"&gt;&amp;#x3B3;&lt;/mi&gt;&lt;/math&gt;' role=\"presentation\" style=\"font-size: 90%; display: inline-block; position: relative;\" tabindex=\"0\"><svg aria-hidden=\"true\" focusable=\"false\" height=\"1.855ex\" role=\"img\" style=\"vertical-align: -0.697ex;\" viewbox=\"0 -498.8 543.5 798.9\" width=\"1.262ex\" xmlns:xlink=\"http://www.w3.org/1999/xlink\"><g fill=\"currentColor\" stroke=\"currentColor\" stroke-width=\"0\" transform=\"matrix(1 0 0 -1 0 0)\"><g is=\"true\"><use xlink:href=\"#MJMATHI-3B3\"></use></g></g></svg><span role=\"presentation\"><math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mi is=\"true\">γ</mi></math></span></span><script type=\"math/mml\"><math><mi is=\"true\">γ</mi></math></script></span>-spectrometric measurements is presented.<h3>Results:</h3>Model electrochemical systems containing inactive Ag, Sb, Sn, and Te were first characterized by voltammetry. 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The separation of, e.g., <sup>110m</sup>Ag or <sup>123m</sup>Te by flow electrolysis afforded a substantial decrease of the uncertainty and the detection limits by one order of magnitude during <span><span style=\"\"></span><span data-mathml='&lt;math xmlns=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;mi is=\"true\"&gt;&amp;#x3B3;&lt;/mi&gt;&lt;/math&gt;' role=\"presentation\" style=\"font-size: 90%; display: inline-block; position: relative;\" tabindex=\"0\"><svg aria-hidden=\"true\" focusable=\"false\" height=\"1.855ex\" role=\"img\" style=\"vertical-align: -0.697ex;\" viewbox=\"0 -498.8 543.5 798.9\" width=\"1.262ex\" xmlns:xlink=\"http://www.w3.org/1999/xlink\"><g fill=\"currentColor\" stroke=\"currentColor\" stroke-width=\"0\" transform=\"matrix(1 0 0 -1 0 0)\"><g is=\"true\"><use xlink:href=\"#MJMATHI-3B3\"></use></g></g></svg><span role=\"presentation\"><math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mi is=\"true\">γ</mi></math></span></span><script type=\"math/mml\"><math><mi is=\"true\">γ</mi></math></script></span>-spectrometry. This allowed for a more accurate determination of low-level activity radionuclides in a sample from a nuclear facility (<sup>123m</sup>Te) as well as for the identification of others which were previously below the detection limit (<sup>103</sup>Ru, <sup>110m</sup>Ag).<h3>Significance:</h3>These results demonstrate the benefits of combining flow electrolysis with <span><span style=\"\"></span><span data-mathml='&lt;math xmlns=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;mi is=\"true\"&gt;&amp;#x3B3;&lt;/mi&gt;&lt;/math&gt;' role=\"presentation\" style=\"font-size: 90%; display: inline-block; position: relative;\" tabindex=\"0\"><svg aria-hidden=\"true\" focusable=\"false\" height=\"1.855ex\" role=\"img\" style=\"vertical-align: -0.697ex;\" viewbox=\"0 -498.8 543.5 798.9\" width=\"1.262ex\" xmlns:xlink=\"http://www.w3.org/1999/xlink\"><g fill=\"currentColor\" stroke=\"currentColor\" stroke-width=\"0\" transform=\"matrix(1 0 0 -1 0 0)\"><g is=\"true\"><use xlink:href=\"#MJMATHI-3B3\"></use></g></g></svg><span role=\"presentation\"><math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mi is=\"true\">γ</mi></math></span></span><script type=\"math/mml\"><math><mi is=\"true\">γ</mi></math></script></span>-spectrometry for analysis of low-level radionuclides in the presence of dominating radionuclides, and can be readily combined with other measurement techniques such as liquid scintillation counting or <span><span style=\"\"></span><span data-mathml='&lt;math xmlns=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;mi is=\"true\"&gt;&amp;#x3B1;&lt;/mi&gt;&lt;/math&gt;' role=\"presentation\" style=\"font-size: 90%; display: inline-block; position: relative;\" tabindex=\"0\"><svg aria-hidden=\"true\" focusable=\"false\" height=\"1.394ex\" role=\"img\" style=\"vertical-align: -0.235ex;\" viewbox=\"0 -498.8 640.5 600.2\" width=\"1.488ex\" xmlns:xlink=\"http://www.w3.org/1999/xlink\"><g fill=\"currentColor\" stroke=\"currentColor\" stroke-width=\"0\" transform=\"matrix(1 0 0 -1 0 0)\"><g is=\"true\"><use xlink:href=\"#MJMATHI-3B1\"></use></g></g></svg><span role=\"presentation\"><math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mi is=\"true\">α</mi></math></span></span><script type=\"math/mml\"><math><mi is=\"true\">α</mi></math></script></span>-spectrometry. The presented approach not only provides a different chemical selectivity when compared to traditional separation methods, but can also be used in combination with other flow separation methods such as ion-exchange or extraction chromatography.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"233 1","pages":""},"PeriodicalIF":5.7000,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Analytica Chimica Acta","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1016/j.aca.2024.343527","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, ANALYTICAL","Score":null,"Total":0}
引用次数: 0

Abstract

Background:

The direct and accurate measurement of low-level γ-emitters in samples from nuclear facilities is a challenging task due to the presence of high activities of dominant radionuclides. In this case a complex chemical separation is required to remove interfering radionuclides prior to γ-spectrometric analysis. Several radionuclides such as, 110mAg, 124,125Sb, 113Sn and 123mTe are of relevance for radioanalytical analysis in nuclear facilities. These may be readily electrodeposited at controlled-potential using flow electrolysis in aqueous solution. Here, the development and use of flow electrolysis for the pre-analytical separation of different radionuclides to suppress interferences in γ-spectrometric measurements is presented.

Results:

Model electrochemical systems containing inactive Ag, Sb, Sn, and Te were first characterized by voltammetry. Their separation by selective electrodeposition and stripping was evaluated with a custom-made, low-cost electrochemical flow-through cell. After optimization, the use of the flow-through cell yielded good separation procedures for stable elements at carefully chosen applied potentials. The developed electrochemical procedures were finally employed for the separation of model mixtures of radioactive tracers as well as for samples from nuclear facilities. The separation of, e.g., 110mAg or 123mTe by flow electrolysis afforded a substantial decrease of the uncertainty and the detection limits by one order of magnitude during γ-spectrometry. This allowed for a more accurate determination of low-level activity radionuclides in a sample from a nuclear facility (123mTe) as well as for the identification of others which were previously below the detection limit (103Ru, 110mAg).

Significance:

These results demonstrate the benefits of combining flow electrolysis with γ-spectrometry for analysis of low-level radionuclides in the presence of dominating radionuclides, and can be readily combined with other measurement techniques such as liquid scintillation counting or α-spectrometry. The presented approach not only provides a different chemical selectivity when compared to traditional separation methods, but can also be used in combination with other flow separation methods such as ion-exchange or extraction chromatography.

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背景:由于存在高活性的主要放射性核素,直接准确测量核设施样品中的低浓度γγ-发射体是一项具有挑战性的任务。在这种情况下,在进行 γγ 光谱分析之前,需要进行复杂的化学分离,以去除干扰放射性核素。有几种放射性核素,如 110mAg、124,125Sb、113Sn 和 123mTe 与核设施中的放射性分析有关。利用水溶液中的流动电解法,可以很容易地在受控电位下对这些放射性核素进行电沉积。结果:首先通过伏安法对含有非活性银、锑、锡和碲的模型电化学系统进行了表征。使用定制的低成本电化学流通池对通过选择性电沉积和剥离分离这些物质进行了评估。经过优化后,在精心选择的应用电位下,使用流动池对稳定元素进行了良好的分离。开发的电化学程序最终被用于分离放射性示踪剂的模型混合物以及核设施样品。通过流动电解分离 110mAg 或 123mTe 等放射性示踪剂,γ-γ 光谱法的不确定性和检测限大幅降低了一个数量级。意义:这些结果表明,将流动电解法与γγ光谱法结合起来,可以在存在主要放射性核素的情况下对低放射性核素进行分析,并可随时与液体闪烁计数法或αα光谱法等其他测量技术相结合。与传统分离方法相比,该方法不仅具有不同的化学选择性,而且还可与离子交换或萃取色谱等其他流动分离方法结合使用。
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来源期刊
Analytica Chimica Acta
Analytica Chimica Acta 化学-分析化学
CiteScore
10.40
自引率
6.50%
发文量
1081
审稿时长
38 days
期刊介绍: Analytica Chimica Acta has an open access mirror journal Analytica Chimica Acta: X, sharing the same aims and scope, editorial team, submission system and rigorous peer review. Analytica Chimica Acta provides a forum for the rapid publication of original research, and critical, comprehensive reviews dealing with all aspects of fundamental and applied modern analytical chemistry. The journal welcomes the submission of research papers which report studies concerning the development of new and significant analytical methodologies. In determining the suitability of submitted articles for publication, particular scrutiny will be placed on the degree of novelty and impact of the research and the extent to which it adds to the existing body of knowledge in analytical chemistry.
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