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创新的高温氟化氢铵融合技术及核 forensic 价值元素的快速分析。

Innovative high-temperature ammonium bifluoride fusion and rapid analysis of elements with nuclear forensic value.

机构信息

Department of Chemistry, University of Missouri, Columbia, MO, 65211, United States.

Department of Chemistry, University of Missouri, Columbia, MO, 65211, United States; Research Reactor, University of Missouri, Columbia, MO, 65211, United States.

出版信息

Talanta. 2021 Jan 1;221:121622. doi: 10.1016/j.talanta.2020.121622. Epub 2020 Sep 6.

Abstract

High-temperature ammonium bifluoride (ABF) fusions were evaluated for potential use in rapid dissolution of post-detonation nuclear debris. The ABF fusion was carried out in a Pt crucible which allowed evaluation of higher fusion and evaporation temperatures. The high-temperature ABF fusion dissolution method was evaluated using geological reference materials: USGS QLO-1a Quartz Latite, USGS SDC-1 Mica Schist, and NIST 278 Obsidian Rock. The optimized dissolution method involved a 10 min fusion at 540 °C, a 5 min reflux in 8 M HNO an evaporation at 300 °C and final dilution into 45 mL of 2% (v/v) HNO. The final solution was filtered after heating at 105 °C using a hotblock. This dissolution method was simple, requiring only a hotplate or hotblock, filtered samples were available for ICP-MS analysis or radiochemical separation within 150 min, and was found to have high (>90%) recovery for many isotopes of interest in nuclear forensics applications. U and Pu in the dissolved material was separated using TEVA and UTEVA extraction chromatography columns, a process which resulted in >90% recovery. An irradiated U tracer was spiked into the material prior to dissolution and analyzed for recovery of major fission products and Np. The monitored radionuclides had recoveries of greater than 90%, except for the volatile radioiodine isotopes.

摘要

高温氟化铵(ABF)熔融物被评估为用于快速溶解核爆炸后残骸的潜在方法。在 Pt 坩埚中进行 ABF 熔融实验,这使得可以评估更高的熔融和蒸发温度。使用地质参考试样:USGS QLO-1a Quartz Latite、USGS SDC-1 Mica Schist 和 NIST 278 Obsidian Rock 评估了高温 ABF 熔融溶解方法。优化的溶解方法包括在 540°C 下进行 10 分钟熔融、在 8M HNO 中进行 5 分钟回流、在 300°C 下蒸发以及最终稀释至 45mL 2%(v/v)HNO。在 105°C 下加热后,使用热块过滤最终溶液。这种溶解方法简单,只需要热板或热块,过滤后的样品可在 150 分钟内进行 ICP-MS 分析或放射化学分离,并且发现对于核取证应用中许多感兴趣的同位素具有高(>90%)回收率。溶解材料中的 U 和 Pu 使用 TEVA 和 UTEVA 萃取色谱柱进行分离,这一过程导致>90%的回收率。在溶解之前,将辐照的 U 示踪剂掺入材料中,并分析主要裂变产物和 Np 的回收率。监测的放射性核素的回收率均大于 90%,除了挥发性放射性碘同位素。

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