A method for Si isotope tracer kinetics experiments: Using Q-ICP-MS to obtain 29Si/28Si ratios in aqueous solutions
A method for Si isotope tracer kinetics experiments: Using Q-ICP-MS to obtain 29Si/28Si ratios in aqueous solutions
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Si同位素示踪动力学实验方法：使用Q-ICP-MS获得水溶液中的29Si/28Si比率
DOI：
10.1016/j.chemgeo.2019.119337
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发表时间：
2020
期刊：
影响因子：
3.9
通讯作者：
Zhu, Chen
中科院分区：
文献类型：
--
作者：
Zhang, Yilun;Gong, Lei;Chen, Kaiyun;Burkhart, Joseph;Yuan, Honglin;Zhu, Chen
在这里，我们证明了硅同位素示踪动力学实验可以经济地进行，用四极杆电感耦合等离子体质谱（Q-ICP-MS）测量实验水溶液中的29si /28Si比，具有足够的精度。尽管同位素示踪剂方法有望提高反应的检测灵敏度，但其应用受到多收集器电感耦合等离子体质谱（MC-ICP-MS）用于Si同位素分析的有限可用性的阻碍。然而，在Si同位素示踪动力学实验中，溶解速率通常由同位素分数丰度增量得出，增量可达0.5个单位（相当于50%），该方法主要依赖于一段时间内同位素比率的差异，这使得Si同位素丰度<±0.01分数（或±1%）的不确定性可以容忍。实验室测量的硅酸盐溶解速率通常具有超过±25%的不确定度，并且实验室内和实验室间的重复性更差。这些动力学实验的特殊情况规避了使用Q-ICP-MS测量同位素比率的传统问题。为了验证这个假设，我们进行了两个实验。第一个使用Q-ICP-MS测量一组已知同位素组成的混合溶液或参考溶液。结果表明，两者的平均差值为±0.009 inf29。第二个测试使用MC-ICP-MS和Q-ICP-MS测量钠长石溶解实验溶液中的29si /28Si比率。在50℃、pH 8.8条件下进行了10次钠长石溶蚀实验。学生检验表明，从两个分析数据集计算的比率在95%的置信水平上没有统计学上的显著差异。这些结果表明，Q-ICP-MS测量29si /28Si的比例产生了可容忍的不确定度，以确定硅酸盐溶解速率。然而，成本显著降低，更重要的是，等待时间的减少使同位素示踪实验更加可行。硅酸盐矿物占地壳的90%。硅酸盐-水反应的动力学对许多社会的大型环境企业具有至关重要的意义。该方法进行Si同位素示踪实验，以及将该方法用于其他非传统稳定同位素的可能性，将对地球化学动力学研究产生重大影响。
Here we show that silicon isotope tracer kinetics experiments can be economically conducted with measurements of29Si/28Si ratios in the experimental aqueous solutions using Quadrupole inductively coupled plasma mass spectrometry (Q-ICP-MS) with sufficient precision. Although the isotope tracer method promises orders of magnitude improved detection sensitivity of reactions, its application has been hampered by the limited availability of multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS) for Si isotope analysis. However, in Si isotope tracer kinetics experiments, dissolution rates are often derived from isotope fractional abundance increments by as much as 0.5 unit (equivalent to 50%) and the method essentially relies on the difference in isotope ratios over a period of time, which render uncertainties in < ±0.01 fraction (or ±1%) in Si isotope abundances tolerable. Laboratory-measured silicate dissolution rates typically carry uncertainties of more than ±25% and with even poorer intra- and inter-laboratory replications. These special situations of kinetics experiments circumvent the conventional concerns of using Q-ICP-MS to measure isotope ratios.To test this hypothesis, we conducted two experiments. The first used Q-ICP-MS to measure a set of mixing solutions or reference solutions with known isotope compositions. The results show that the difference is an average of ±0.009 inf29. A second test used both MC-ICP-MS and Q-ICP-MS to measure the29Si/28Si ratios in experimental solutions of albite dissolution. Ten albite dissolution experiments were conducted at 50 °C and pH 8.8. Studentt-test showed that the rates calculated from the two analytical data sets have no statistically significant differences at the 95% confidence level. These results demonstrate that the Q-ICP-MS measurements of29Si/28Si ratios produced tolerable uncertainties for determining silicate dissolution rates. However, the cost is significantly reduced and more significantly, the reduced wait time makes isotope tracer experiments more feasible. Silicate minerals make up 90% of the Earth’s crust. The kinetics of silicate-water reactions is of paramount significance to many society’s mega-environmental enterprises. This method to conduct Si isotope tracer experiments, as well as the possibility to use this approach for other non-traditional stable isotopes, will have significant impact on geochemical kinetics studies.
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