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结合TK200-TK221串联柱萃取色谱法和SF ICP-MS测定海洋沉积物和海水中的超痕量镅

Determination of ultra-trace level Am in marine sediment and seawater by combining TK200-TK221 tandem-column extraction chromatography and SF ICP-MS.

作者信息

Zhang Ling, Vassileva Emilia

机构信息

International Atomic Energy Agency, Environment Laboratories, 4 Quai Antoine 1er, Principality of Monaco, 98000, Monaco; Institute of Materials, China Academy of Engineering Physics, Mianyang, 621900, China.

International Atomic Energy Agency, Environment Laboratories, 4 Quai Antoine 1er, Principality of Monaco, 98000, Monaco.

出版信息

Talanta. 2024 May 1;271:125724. doi: 10.1016/j.talanta.2024.125724. Epub 2024 Jan 26.

Abstract

Sound strategies for marine chemical monitoring call for measurement systems capable of producing comparable analytical results with demonstrated quality. This work presents the development and validation of a new analytical procedure for the determination of the Am mass fraction in marine sediment and seawater samples at low levels. The procedure includes a tandem-column extraction chromatography for separation of Am and sector field-inductively coupled plasma mass spectrometry (SF ICP-MS) for its determination. The separation is based on the application of two new extraction resins, TK200 and TK221. The acid leaching method was employed for the pre-treatment of marine sediments, while Fe(OH)3 co-precipitation was used for Am pre-concentration in seawater samples. The extraction behaviors of Am on TK221 resins in the different acidic mediums were investigated. The removal capabilities of the tandem TK200-TK221 columns for the 241Am in the presence of interfering elements including Pu, Pb, Hg, Bi, Tl, Pt, Hf, U, and Th were carefully investigated and the corresponding decontamination factors (DFs) estimated to be in the range from 10 to 10. The main interfering element Pu was efficiently removed with a DF of about 6 × 10. Matrix rare earth elements (REEs) in marine sediments were further removed by the application of TEVA resins. Am mass fraction was quantified by the application of external calibration and SF ICP-MS. Following the recommendations of the ISO/IEC 17025 guidelines, the validation of the analytical procedure was accomplished by executing it on the certified reference material (CRM) IAEA-385 (marine sediment) and the seawater IAEA-443 reference materials (RM). The obtained results showed that Am mass fractions were accurately determined in both reference samples, with excellent reproducibility (2.1 % and 7.6 %) and low LODs (0.4 fg g and 0.2 fg g). The relative expanded uncertainties (k = 2) obtained were 17.1 % and 29.0 %, respectively. The overall analytical times for the application of the proposed procedure on the marine sediment and seawater samples were evaluated to be only about 9 h and 6.5 h, respectively. It shows great advantages for its potential applications for emergency monitoring of Am contamination in the marine environment.

摘要

海洋化学监测的合理策略要求测量系统能够产生具有可证明质量的可比分析结果。这项工作展示了一种新分析程序的开发与验证,该程序用于测定海洋沉积物和海水样品中低含量的镅质量分数。该程序包括用于镅分离的串联柱萃取色谱法以及用于其测定的扇形场电感耦合等离子体质谱法(SF ICP-MS)。分离基于两种新型萃取树脂TK200和TK221的应用。采用酸浸法对海洋沉积物进行预处理,而在海水样品中采用氢氧化铁共沉淀法对镅进行预浓缩。研究了镅在不同酸性介质中在TK221树脂上的萃取行为。仔细研究了串联的TK200-TK221柱在存在包括钚、铅、汞、铋、铊、铂、铪、铀和钍等干扰元素的情况下对241Am的去除能力,相应的去污因子(DFs)估计在10至10的范围内。主要干扰元素钚以约6×10的去污因子被有效去除。通过应用TEVA树脂进一步去除海洋沉积物中的基体稀土元素(REEs)。通过外部校准和SF ICP-MS对镅质量分数进行定量。按照ISO/IEC 17025指南的建议,通过在认证参考物质(CRM)IAEA-385(海洋沉积物)和海水IAEA-443参考物质(RM)上执行该分析程序来完成其验证。所得结果表明,在两个参考样品中都准确测定了镅质量分数,具有出色的重现性(2.1%和7.6%)和低检测限(0.4 fg g和0.2 fg g)。获得的相对扩展不确定度(k = 2)分别为17.1%和29.0%。将所提出的程序应用于海洋沉积物和海水样品的总体分析时间估计分别仅约为9小时和6.5小时。它在海洋环境中镅污染应急监测的潜在应用方面显示出巨大优势。

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