Huang Zhao, Hou Xiaolin, Qiao Jixin, Zhao Xue
Department of Environmental and Resource Engineering, Technical University of Denmark, DTU Risø Campus, Roskilde, 4000, Denmark; State Key Laboratory of Loess and Quaternary Geology, Xi'an AMS Center, Shaanxi Key Laboratory of Accelerator Mass Spectrometry Technology and Application, Institute of Earth Environment, Chinese Academy of Sciences, Xi'an, 710061, China; University of Chinese Academy of Sciences, Beijing, 100049, China.
Department of Environmental and Resource Engineering, Technical University of Denmark, DTU Risø Campus, Roskilde, 4000, Denmark; State Key Laboratory of Loess and Quaternary Geology, Xi'an AMS Center, Shaanxi Key Laboratory of Accelerator Mass Spectrometry Technology and Application, Institute of Earth Environment, Chinese Academy of Sciences, Xi'an, 710061, China; Open Studio for Oceanic-Continental Climate and Environment Changes, Pilot National Laboratory for Marine Science and Technology (Qingdao), Qingdao, 266061, China.
Talanta. 2023 Dec 1;265:124798. doi: 10.1016/j.talanta.2023.124798. Epub 2023 Jun 17.
An analytical method based on triple quadrupole inductively coupled plasma mass spectrometry (ICP-MS/MS) was developed for simultaneous determination of femtogram levels of Np, Pu, and Pu in environmental samples. By carefully controlling the valence states of Np and Pu in the entire separation procedure using a simple single extraction chromatographic column (TK200), the consistent behavior of Np and Pu was achieved, allowing for the reliable application of Pu as the chemical yield tracer for Np, Pu, and Pu. A high decontamination factor of 3.2 × 10 for the most critical interfering element, uranium, was achieved in the chemical separation step. The interferences of UH and peak tailing of U during the measurement of plutonium isotopes were effectively eliminated by utilizing 7.5 mL/min He-1.1 mL/min CO as reaction gases in the octupole collision/reaction cell and employing sequential quadrupole mode for mass separation in ICP-MS/MS. Specifically, the interference of UH was reduced to 10 and the peak tailing of U to 10, surpassing the performance of measurement method without reaction gases by 3 orders of magnitude. The developed method enables the accurate determination of femtogram levels of Np, Pu, and Pu in the samples with U/Np and U/Pu atom ratios of up to 10 and 10, respectively. The developed method was validated by analyzing standard reference materials and spiked soil samples.
建立了一种基于三重四极杆电感耦合等离子体质谱（ICP-MS/MS）的分析方法，用于同时测定环境样品中飞克级水平的镎（Np）、钚（Pu）和钚（此处原文可能有误，疑为其他钚同位素之类）。通过使用简单的单萃取色谱柱（TK200）在整个分离过程中仔细控制Np和Pu的价态，实现了Np和Pu的一致行为，从而能够可靠地将Pu用作Np、Pu和Pu的化学产率示踪剂。在化学分离步骤中，对于最关键的干扰元素铀，实现了3.2×10的高去污因子。在八极杆碰撞/反应池中利用7.5 mL/min He - 1.1 mL/min CO作为反应气体，并在ICP-MS/MS中采用顺序四极杆模式进行质量分离，有效消除了钚同位素测量过程中UH的干扰和U的峰拖尾。具体而言，UH的干扰降低到10，U的峰拖尾降低到10，比无反应气体的测量方法性能提高了3个数量级。所开发的方法能够准确测定U/Np和U/Pu原子比分别高达10和10的样品中飞克级水平的Np、Pu和Pu。通过分析标准参考物质和加标土壤样品对所开发的方法进行了验证。
