Laser induced breakdown spectroscopy tandem with laser ablation

激光诱导击穿光谱与激光烧蚀串联

• 批准号: NE/T009187/1
• 负责人: Monica Felipe-Sotelo
• 金额: $ 18.97万
• 依托单位: University of Surrey
• 依托单位国家: 英国
• 项目类别: Research Grant
• 财政年份: 2019
• 资助国家: 英国
• 起止时间: 2019 至 无数据
• 项目状态: 已结题
• 来源: https://gtr.ukri.org/projects?ref=NE%2FT009187%2F1
• 关键词: Laser; induced; breakdown; spectroscopy; tandem

The government is committed to deliver sustainable, low-carbon energy and this strategic goal requires a cross-disciplinary effort to advance the current understanding of the interaction of radionuclides with earth materials, including minerals, soils and rocks. The data generated will be employed to monitor and minimise the environmental impact from the leaching of radioactive materials, and to predict their migration rate. This could be built into the safety case for storage and geological disposal of radioactive waste.Current research at the University of Surrey focuses on the safety of radioactive waste disposal. In particular; (1) characterisation of natural uranium-bearing minerals to investigate the evolution of radioactive wastes; (2) mechanisms of interaction of radionuclides with rocks and soils; and (3) effect of natural organic matter and concomitant pollutants on the retardation of radionuclides. One of the biggest challenges encountered by this investigation is the determination of the migration profiles of key elements and radionuclides and their association to specific mineral phases. For this purpose, the tandem LIBS-LA (laser-induced breakdown spectroscopy with laser ablation) would offer the elemental range, sensitivity and spatial resolution necessary to support this research.Many conventional techniques of analysis only provide average concentration of the elements present in the bulk material and require intensive sample preparation, while others can obtain information on the distribution and specific interactions of some elements (elemental mapping), for example XRF (X-ray fluorescence) or EDX (energy-dispersive X-ray). However, due to their low sensitivity they can only be applied to a limited range of elements. Both laser-induced breakdown spectroscopy (LIBS) and laser ablation-inductively coupled plasma-mass spectrometry (LA-ICP-MS) are techniques that enable elemental mapping for solid sample and can provided isotopic information, with minimum sample preparation requirements, and they are well-established analytical techniques with their own unique advantages and disadvantages. The combination of the two analytical methods in one unique instrumentation, as proposed here, is a very promising way to overcome the challenges faced by each method individually.Despite the advances in sensitivity and resolution of LA-ICP-MS, there are certain elements and isotopes that still cannot be measured. These include among others F, O, H and N. This is due to interferences, saturation of the detector (for major elements) and problems with the ionisation potential (either too high or too low). On the other hand, while LIBS can successfully provide quantitative and distribution information of these light and bulk components, it suffers from precision limitations due to temporal and spatial variations generated by the physical and chemical heterogeneity of the solid samples (matrix effects). LIBS and LA can be combined, as the same laser pulse used to ablate small particles from the solid samples to be carried into the ICP-MS can also generate a laser- induced plasma that can be detected and analysed spectroscopically. Thus, the combination of LIBS and LA-ICP-MS not only expands the coverage of elements that can be measured simultaneously, but also it will lead to improved precision and reduction of spectral interferences by using the signals from both the MS and spectroscopy detectors applying a multivariate approach to calibration and signal processing.This proposed unique analytical facility in the UK will have the capability to determine simultaneously the distribution and association of radionuclides with mineral and other major components in soils, rocks and structural materials contaminated by accidental leaks. This will provide knowledge of the pathways of radioisotopes into the environment and mechanisms of interaction with the natural media, to evaluate and minimise the impact of human activities.

政府致力于提供可持续的低碳能源，这一战略目标需要跨学科的努力，以促进目前对放射性核素与地球材料(包括矿物、土壤和岩石)相互作用的理解。所产生的数据将被用来监测和减少放射性物质浸出对环境的影响，并预测它们的迁移率。这可以建立在放射性废物储存和地质处置的安全案例中。萨里大学目前的研究重点是放射性废物处置的安全性。特别是：(1)研究放射性废物演化的天然含铀矿物的特征；(2)放射性核素与岩石和土壤相互作用的机制；(3)天然有机物和伴随污染物对放射性核素延缓作用的影响。这项调查遇到的最大挑战之一是确定关键元素和放射性核素的迁移分布及其与特定矿物相的联系。为此，串联式激光诱导击穿光谱(LIBS-LA)将提供支持这项研究所需的元素范围、灵敏度和空间分辨率。许多传统的分析技术只能提供块状材料中存在的元素的平均浓度，需要密集的样品制备，而其他技术可以获得某些元素的分布和特定相互作用的信息(元素图谱)，例如XRF(X射线荧光)或EDX(能量色散X射线)。然而，由于它们的灵敏度较低，它们只能应用于有限范围的元素。激光诱导击穿光谱(LIBS)和激光烧蚀-电感耦合等离子体质谱(LA-ICPMS)都是能够对固体样品进行元素测绘的技术，可以提供同位素信息，而且样品制备要求最低，这两种技术都是成熟的分析技术，各有其独特的优缺点。将这两种分析方法结合在一个独特的仪器中，是一种非常有希望的方法，可以克服每种方法各自面临的挑战。尽管LA-ICPMS在灵敏度和分辨率方面取得了进展，但仍有某些元素和同位素无法测量。其中包括F、O、H和N。这是由于干扰、探测器饱和(对于主要元素)和电离势(太高或太低)的问题。另一方面，虽然LIBS可以成功地提供这些轻组分和体积组分的定量和分布信息，但由于固体样品的物理和化学不均一性(基质效应)产生的时间和空间变化，LIBS的精度受到限制。LIBS和LA可以结合在一起，因为用于从固体样品中烧蚀小颗粒的同一激光脉冲也可以产生激光诱导的等离子体，可以用光谱分析来检测和分析。因此，LIBS和LA-ICP-MS的结合不仅扩大了可以同时测量的元素的覆盖范围，而且通过使用来自MS和光谱探测器的信号，应用多变量方法进行校准和信号处理，从而提高了精度并减少了光谱干扰。这一拟议的英国独一无二的分析设施将能够同时确定放射性核素与意外泄漏污染的土壤、岩石和结构材料中的矿物和其他主要成分的分布和结合。这将提供放射性同位素进入环境的途径和与自然介质相互作用的机制的知识，以评估和最大限度地减少人类活动的影响。

项目成果

Characterisation of carnotite and tyuyamunite using Raman, luminescence and laser-induced breakdown spectroscopy

使用拉曼、发光和激光诱导击穿光谱表征卡诺石和秋亚铝石

• DOI: 10.1016/j.apgeochem.2022.105503
• 发表时间: 2022
• 期刊: Applied Geochemistry
• 影响因子: 3.4
• 作者: Frankland V

Characterisation of andersonite by Raman, luminescence and laser-induced breakdown spectroscopy

通过拉曼、发光和激光诱导击穿光谱表征红钙石

• DOI: 10.1016/j.apgeochem.2022.105353
• 发表时间: 2022
• 期刊: Applied Geochemistry
• 影响因子: 3.4
• 作者: Frankland V