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利用扇形场电感耦合等离子体质谱法测定大土壤样品中痕量(241)Am 的方法:重点关注光谱干扰和基质效应的去除。

Method for Ultratrace Level (241)Am Determination in Large Soil Samples by Sector Field-Inductively Coupled Plasma Mass Spectrometry: With Emphasis on the Removal of Spectral Interferences and Matrix Effect.

机构信息

Biospheric Assessment for Waste Disposal Team, National Institute of Radiological Sciences, National Institutes for Quantum and Radiological Science and Technology , 4-9-1 Anagawa, Inage, Chiba 263-8555, Japan.

School of Geographic and Oceanographic Sciences, Nanjing University , Nanjing 210023, China.

出版信息

Anal Chem. 2016 Jul 19;88(14):7387-94. doi: 10.1021/acs.analchem.6b01934. Epub 2016 Jun 30.

Abstract

A new method using sector field-inductively coupled plasma mass spectrometry (SF-ICPMS) was developed for the determination of (241)Am in large soil samples to provide realistic soil-plant transfer parameter data for dose assessment of nuclear waste disposal plans. We investigated four subjects: extraction behaviors of interfering elements (Bi, Tl, Hg, Pb, Hf, and Pt) on DGA resin (normal type, abbreviated as DGA-N); soil matrix element removal (Mg, Fe, Al, K, Na) using Fe(OH)3, CaF2, and CaC2O4 coprecipitations; Am and rare earth elements (REEs) separation on DGA-N and TEVA resins; and optimization of SF-ICPMS (equipped with a high efficiency nebulizer (HEN)) for Am determination. Our method utilized concentrated HNO3 to leach Am from 2 to 20 g soil samples. The CaC2O4 coprecipitation was used to remove major metals in soil and followed by Am/interfering elements separation using the proposed UTEVA + DGA-N procedure. After a further separation of REEs on TEVA resin, (241)Am was determined by HEN-SF-ICPMS. This method eliminated the matrix effect in ICPMS (241)Am measurement for large soil samples. The high decontamination factors (DFs) of interfering elements enable their thorough removal, and in particular, the DF of Pu (7 × 10(5)) was the highest ever reported in (241)Am studies; thus, this method is capable of analyzing (241)Pu-contaminated Fukushima Daiichi Nuclear Power Plant (FDNPP) sourced soil samples. A low detection limit of 0.012 mBq g(-1) for (241)Am was achieved. The chemical recovery of Am (76-82%) was stable for soil samples. This method can be employed for the low level (241)Am determination in large size soil samples that are contaminated with (241)Pu.

摘要

一种使用扇形场电感耦合等离子体质谱(SF-ICPMS)的新方法被开发用于测定大土壤样品中的(241)Am,以提供核废料处置计划剂量评估的现实土壤-植物转移参数数据。我们研究了四个方面:干扰元素(Bi、Tl、Hg、Pb、Hf 和 Pt)在 DGA 树脂(普通型,缩写为 DGA-N)上的萃取行为;使用 Fe(OH)3、CaF2 和 CaC2O4 共沉淀去除土壤基质元素(Mg、Fe、Al、K、Na);DGA-N 和 TEVA 树脂上的 Am 和稀土元素(REEs)分离;以及优化配备高效雾化器(HEN)的 SF-ICPMS 用于 Am 测定。我们的方法利用浓 HNO3 从 2 到 20 g 土壤样品中浸出 Am。使用 CaC2O4 共沉淀去除土壤中的主要金属,然后使用提议的 UTEVA+DGA-N 程序分离 Am/干扰元素。在 TEVA 树脂上进一步分离 REEs 后,使用 HEN-SF-ICPMS 测定(241)Am。该方法消除了 ICPMS 中(241)Am 测量的基质效应大土壤样品。干扰元素的高去污因子(DF)可彻底去除,特别是 Pu 的 DF(7×10(5))是(241)Am 研究中报道的最高值;因此,该方法能够分析受福岛第一核电站(FDNPP)污染的土壤样品。(241)Am 的检测限低至 0.012 mBq g(-1)。Am 的化学回收率(76-82%)在土壤样品中稳定。该方法可用于测定受(241)Pu 污染的大尺寸土壤样品中的低水平(241)Am。

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