Deuterium analysis by inductively coupled plasma mass spectrometry using polyatomic species: An experimental study supported by plasma chemistry modeling

被引:7
作者
Galbacs, Gabor [1 ]
Keri, Albert [1 ]
Kalomista, Ildiko [1 ]
Kovacs-Szeles, Eva [2 ]
Gornushkin, Igor B. [3 ]
机构
[1] Univ Szeged, Dept Inorgan & Analyt Chem, Dom Sq 7, H-6720 Szeged, Hungary
[2] MTA Ctr Energy Res, Nucl Secur Dept, Konkoly Thege Miklos St 29-33, H-1121 Budapest, Hungary
[3] BAM Fed Inst Mat Res & Testing, Richard Willstaetter Str 11, D-12489 Berlin, Germany
关键词
Deuterium; Deuterium-enriched water; Deuterium-depleted water; Inductively coupled plasma-mass spectrometry; Hydrogen; Polyatomic species; RATIO INFRARED-SPECTROSCOPY; POTENTIAL-ENERGY SURFACE; HYDRIDE MOLECULE-IONS; AB-INITIO; HIGH-RESOLUTION; ICP-MS; PARTITION-FUNCTIONS; HYDROGEN-PEROXIDE; ELECTRONIC STATES; ISOTOPE ANALYSIS;
D O I
10.1016/j.aca.2020.01.011
中图分类号
O65 [分析化学];
学科分类号
070302 ; 081704 ;
摘要
A new analytical method is proposed for the determination of deuterium (D) by ICP-MS. The method is based on the use of the signal from hydrogen-containing polyatomic ions formed in the inductively coupled plasma. Prior to analytical experiments, a theoretical study was performed to assess the concentration of polyatomic species present in an equilibrium Ar-O-D-H plasma, as a function of temperature and stoichiometric composition. It was established that the highest sensitivity and linearity measurement of D concentration in a wide range can be achieved by monitoring the ions of D-2 and ArD, at masses 4 and 42, respectively. Results of the calculations are in good agreement with the experiments. Signal stability, spectral interferences, as well as the effect of plasma parameters were also assessed. Under optimized conditions, the limit of detection (LOD) was found to be 3 ppm atom fraction for deuterium when measured as ArD (in calcium and potassium free water), or 78 ppm when measured as D2. The achieved LOD values and the 4 to 5 orders of magnitude dynamic range easily allow the measurement of deuterium concentrations at around or above the natural level, up to nearly 100% (or 1 Mio ppm) in a standard quadrupole ICP-MS instrument. An even better performance is expected from the method in high resolution ICP-MS instruments equipped with low dead volume sample introduction systems. (C) 2020 Elsevier B.V. All rights reserved.
引用
收藏
页码:28 / 37
页数:10
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