锆石微量元素同位素组成测定及其在放射成因钼研究中的应用
Measuring the isotopic composition of trace elements in zircon: application to radiogenic molybdenum
摘要:
已经开发了从主要由干扰同位素组成的基质中测量痕量元素的同位素组成的技术。这些技术已被应用于测量由于核衰变而导致的古老锆石样品中钼的质量无关分馏。本文介绍了大型锆石样品的溶出方法和从硅酸锆中分离微量钼所需的离子交换化学方法的改进。研究了TEVA离子交换树脂替代阴离子交换树脂提高分离效率和化学空白的效果。建立了多接收电感耦合等离子体质谱(MC-ICPMS)分析钼的背景校正、干扰校正和质量偏差校正算法。这使得能够通过将Zr含量减少$>$ 9个数量级而保留63%的Mo,从500 mg ZrSiO $_4$回收50 ng Mo,从而进行$<$的同位素组成测量。由于还剩下5 ng Zr,新的数据分析技术使$<$对每种Mo同位素的精确度达到0.1 permil。这种技术提取其他原子物种的相关性也进行了讨论。
英文摘要:
Techniques have been developed to measure the isotopic composition of trace elements from matrices predominantly consisting of interfering isotopes. These techniques have been applied to measuring mass-independent fractionation of molybdenum in ancient zircon samples due to nuclear decays. Improvements to the digestion of large zircon samples and the ion exchange chemistry required to separate trace molybdenum from zirconium silicate are presented. The efficacy of TEVA ion exchange resin as a replacement for anion resin to improve separation efficiency and chemistry blank was studied. An algorithm was established to improve background, interference and mass bias corrections for the data analysis of Mo by multi-collector inductively coupled plasma mass spectrometry (MC-ICPMS). This enabled the isotopic composition measurement of $<$50 ng of Mo recovered from 500 mg ZrSiO$_4$ by reducing the Zr content by $>$9 orders of magnitude while retaining 63% of the Mo. With 5 ng of Zr still remaining, novel data analysis techniques enabled $<$0.1 permil precision on each Mo isotope. The relevance of this technique to extracting other atomic species is also discussed.
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