Determination of ethylenediaminetetraacetic acid in nuclear waste by high-performance liquid chromatography coupled with electrospray mass spectrometry
Determination of ethylenediaminetetraacetic acid in nuclear waste by high-performance liquid chromatography coupled with electrospray mass spectrometry
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DOI：
10.1016/j.chroma.2012.10.055
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发表时间：
2013-02-08
影响因子：
4.1
通讯作者：
Thiebaut, Didier
中科院分区：
文献类型：
--
作者：
de Maquille, Laurence du Bois;Renaudin, Laetitia;Thiebaut, Didier
EDTA 是一种用于净化过程的螯合剂。核废物管理需要对其进行量化，因为它会影响放射性核素和金属在环境中的流动性，从而损害储存的安全。离子对色谱法与电喷雾质谱检测相结合是定量分析 EDTA 的便捷方法，但 EDTA 应以单一阴离子螯合物形式存在。然而，放射性液体废物含有高浓度的重金属和盐，因此，EDTA 以多种螯合物形式存在。进行形态研究以选择过量添加到溶液中的金属阳离子以获得主要螯合物形式。 Fe 是主要阳离子，Fe(III)-EDTA 在热力学上是有利的，但这些形态研究表明，氢氧化铁在 pH 值高于 2 时沉淀。因此，不可能将 EDTA 定量为 Fe(III)-EDTA 络合物。因此，选择了 Ni2+，但其使用意味着用溶液碱进行预处理以消除 Fe。使用氘代 EDTA 作为示踪剂，以验证从碱处理到 HPLC-ESI-MS 最终分析的整个过程。该分析方法已成功应用于核废液处理过程中产生的两种实际流出物中的 EDTA 定量。回收率在 60% 至 80% 之间。该方法的检测限确定为34 x 10(-9) mol L-1。 (C) 2012 Elsevier B.V. 保留所有权利。
EDTA is a chelating agent that has been used in decontamination processes. Its quantification is required for nuclear waste management because it affects the mobility of radionuclides and metals in environment and, thus, can harm the safety of the storage. Ion-pair chromatography coupled with electrospray mass spectrometry detection is a convenient method for quantitative analysis of EDTA but EDTA should be present as a single anionic chelate form. However, radioactive liquid wastes contain high concentrations of heavy metals and salts and consequently, EDTA is present as several chelates. Speciation studies were carried out to choose a metal cation to be added in excess to the solution to obtain a major chelate form. Fe is the predominant cation and Fe(III)-EDTA is thermodynamically favored but these speciation studies showed that ferric hydroxide precipitated above pH2. Consequently, it was not possible to quantify EDTA as Fe(III)-EDTA complex. Therefore, Ni2+ was chosen but its use implied pretreatment with a base of the solution to eliminate Fe. Deuterated EDTA was used as tracer in order to validate the whole procedure, from the treatment with a base to the final analysis by HPLC-ESI-MS. This analytical method was successfully applied for EDTA quantification in two real effluents resulting from a nuclear liquid waste process. A recovery rate between 60 and 80% was obtained. The limit of detection of this method was determined at 34 x 10(-9) mol L-1. (C) 2012 Elsevier B.V. All rights reserved.