Advances in Analysis for Halogens in Geological Materials
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摘要: 地质样品中卤素是反演与流体和挥发分相关的地质过程的重要示踪元素.由于卤素含量低和强挥发性,准确测定地质样品中卤素一直是分析地球化学的难点.近年来,针对地质样品卤素的样品前处理技术的开发开展了大量工作.高温热解法、碱熔(溶)法、酸性消解法和碱性提取法能够满足土壤、沉积物和岩石中高含量卤素的分析要求.针对低含量卤素,仅有中子活化法和稀有气体质谱法能够准确定量.随着分析地球化学的发展,地质样品卤素分析技术逐渐向更高效的消解方法、更简便的操作以及更高灵敏度和高精度的分析方向改进.总结了近年来国内外在地质样品卤素分析方面所取得的成果,对比了各类方法的优缺点,展望了地质样品卤素分析方法的发展前景.Abstract: Halogen in geological materials is the key tracer for the fluid/volatile related geological processes. Due to low concentration of halogens and high volatility, it is a challenge for the analysis of halogens in geological materials. Many studies on sample preparation for the analysis of halogens in geological materials have been reported in the last decade. Pyrohydrolysis, alkali fusion, acid digestion and alkali extraction are suitable for the high concentrations of halogens in soils, sediments and most of rocks. Only neutron activation analysis and noble gas technique can be utilized to analyze the low concentrations of halogens in geological materials. With the development of earth science and the analytical geochemistry, the future analysis of halogens will be more effective, more convenients and with higher sensitivity and precision are the future of the analysis of halogens. In this study, we reviewed the development of analysis techniques for halogens and compares the advantages and drawbacks between different methods. Finally, a perspective of the development of analytical method for halogens in geological materials are given.
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Key words:
- halogen /
- geological material /
- sample preparation /
- analytical method /
- geochemistry
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图 1 地球上不同卤素储库的Br/Cl和I/Cl比值与不同矿床类型流体的Br/Cl和I/Cl比值(改自Lecumberri-Sanchez and Bodnar, 2018)
Fig. 1. Characteristic Br/Cl and I/Cl ratios of the different halogen reservoirs on the Earth and fluids in different ore deposit types(revised from Lecimberri-Sanchez and Bodnar, 2018)
图 2 国内土壤(GSS系列)和沉积物(GSD系列)标准物质和国际岩石标准物质(玄武岩BHVO-2、安山岩AGV-2、花岗岩GS-N和橄榄岩JP-1)中Br (a)和I (b)的测定值
Fig. 2. The measured values of Br (a) and I (b) in reference standard materials including soils (GSS series), sediments (GSD series) and rocks (basalt BHVO-2, andesite AGV-2, granite GS-N and peridotite JP-1)
图 3 高温热解法装置(改自Chai and Muramatsu, 2007)
Fig. 3. The schematic diagram of pyrohydrolysis (revised from Chai and Muramatsu, 2007)
图 4 氟化氢铵消解卤素分析方法机理图(改自He et al., 2019)
Fig. 4. The decomposition mechanism of NH4HF2 digestion for halogen analysis (revised from He et al., 2019)
图 5 79Br中子活化过程示意(改自Ruzié-Hamilton et al., 2016)
Fig. 5. The schematic of neutron irradiation for 79Br(revised from Ruzié-Hamilton et al., 2016)
表 1 地球各个储库的卤素丰度
Table 1. Abundances of halogens on Earth
储库类型 储库总质量(1021 kg) F(μg/g) Cl(μg/g) Br(μg/g) I(μg/g) 海水 1.4±0.7 1.30±0.07 19 300±970 66±3.3 0.058±0.006 蒸发盐 0.030±0.005 10±10 550 000±50 000 150±100 1±1 海洋沉积物 0.5±0.1 1 000±300 4 000±3 000 40±20 30±15 沉积岩 1.5±0.3 550±100 700±400 4±3 1.5±1.0 地壳卤水 0.06±0.03 20±15 100 000±50 000 600±400 15±10 地壳 26±3 550±100 300±100 0.60±0.25 0.018±0.009 地幔 2 800±800 12±2 5±2 0.013±0.006 0.000 3±0.000 01 原始地幔 4 040 17±6 26±8 76±25 0.007±0.004 注:数据引自 Kendrick et al.(2017) .表 2 卤素的质谱干扰所需分辨率
Table 2. The resolution to resolve the spectral interferences on halogens
被测元素 干扰离子 所需分辨率(M/ΔM) 19F+ 38Ar2+ 1 116 18O1H+ 1 160 35Cl+ 19F16O+ 1 430 18O18O1H+ 1 059 37Cl+ 36Ar1H+ 4 680 79Br+ 63Cu16O+ 12 790 41K38Ar+ 12 688 39K40Ar+ 10 184 40Ar38Ar1H+ 5 405 81Br+ 65Cu16O+ 12 624 45Sc36Ar+ 11 286 41K40Ar+ 10 217 63Cu18O+ 6 489 40Ar40Ar1H+ 4 965 127I+ 87Sr40Ar+ 3 822 87Rb40Ar+ 3 854 111Cd16O+ 23 545 -
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