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首页> 美国卫生研究院文献>other >Development of a High-Resolution Laser Absorption Spectroscopy Method with Application to the Determination of Absolute Concentration of Gaseous Elemental Mercury in Air
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Development of a High-Resolution Laser Absorption Spectroscopy Method with Application to the Determination of Absolute Concentration of Gaseous Elemental Mercury in Air

机译：高分辨率激光吸收光谱法的发展及其在空气中气态元素汞绝对浓度测定中的应用

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Isotope dilution-cold-vapor-inductively coupled plasma mass spectrometry (ID-CV-ICPMS) has become the primary standard for measurement of gaseous elemental mercury (GEM) mass concentration. However, quantitative mass spectrometry is challenging for several reasons including (1) the need for isotopic spiking with a standard reference material, (2) the requirement for bias-free passive sampling protocols, (3) the need for stable mass spectrometry interface design, and (4) the time and cost involved for gas sampling, sample processing, and instrument calibration. Here, we introduce a high-resolution laser absorption spectroscopy method that eliminates the need for sample-specific calibration standards or detailed analysis of sample treatment losses. This technique involves a tunable, single-frequency laser absorption spectrometer that measures isotopically resolved spectra of elemental mercury (Hg) spectra of 6 1S0 ← 6 3P1 intercombination transition near λ = 253.7 nm. Measured spectra are accurately modeled from first-principles using the Beer–Lambert law and Voigt line profiles combined with literature values for line positions, line shape parameters, and the spontaneous emission Einstein coefficient to obtain GEM mass concentration values. We present application of this method for the measurement of the equilibrium concentration of mercury vapor near room temperature. Three closed systems are considered: two-phase mixtures of liquid Hg and its vapor and binary two-phase mixtures of Hg–air and Hg–N2 near atmospheric pressure. Within the experimental relative standard uncertainty, 0.9–1.5% congruent values of the equilibrium Hg vapor concentration are obtained for the Hg-only, Hg–air, Hg–N2 systems, in confirmation with thermodynamic predictions. We also discuss detection limits and the potential of the present technique to serve as an absolute primary standard for measurements of gas-phase mercury concentration and isotopic composition.
机译：同位素稀释-冷蒸气-电感耦合等离子体质谱法（ID-CV-ICPMS）已成为测量气态元素汞（GEM）质量浓度的主要标准。但是，由于以下几个原因，定量质谱分析具有挑战性：（1）需要使用标准参考物质进行同位素加标；（2）需要无偏差的被动采样方案；（3）需要稳定的质谱接口设计； （4）气体采样，样品处理和仪器校准所需的时间和成本。在这里，我们介绍了一种高分辨率的激光吸收光谱法，无需使用特定于样品的校准标准或对样品处理损失进行详细分析的方法。该技术涉及一种可调谐的单频激光吸收光谱仪，该光谱仪可测量λ附近6 1 S0←6 3 P1结合跃迁的元素汞（Hg）光谱的同位素分辨光谱= 253.7 nm。使用比尔-兰伯特定律和Voigt谱线从第一原理精确地对测得的光谱建模，结合谱线位置，谱线形状参数和自发发射爱因斯坦系数的文献值，即可获得GEM质量浓度值。我们介绍了该方法在室温附近测量汞蒸气平衡浓度的应用。考虑了三个封闭系统：液态Hg及其蒸气的两相混合物，以及接近大气压的Hg-空气和Hg-N2的二元两相混合物。在实验相对标准不确定性范围内，对于仅含汞，含汞空气，含Hg-N2的系统，可获得平衡汞蒸气浓度的0.9-1.5％的全等值，并通过热力学预测得到证实。我们还将讨论检测极限和本技术作为气相汞浓度和同位素组成的绝对绝对标准测量的潜力。

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    Abneesh Srivastava; Joseph T. Hodges;

  • 作者单位
  • 年(卷),期 -1(90),11
  • 年度 -1
  • 页码 6781–6788
  • 总页数 19
  • 原文格式 PDF
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  • 入库时间 2022-08-21 11:07:23

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