Kinetic study on gas phase zinc reduction of silicon tetrachloride
Kinetic study on gas phase zinc reduction of silicon tetrachloride
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四氯化硅气相锌还原动力学研究
DOI：
10.1016/j.cej.2011.02.028
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发表时间：
2011
影响因子：
15.1
通讯作者：
Y. Yamaguchi
中科院分区：
文献类型：
--
作者：
Norihisa Uesawa;P. Shen;S. Inasawa;A. Miyoshi;Y. Yamaguchi
本文对四氯化硅气相锌还原反应进行了动力学分析。尽管这种反应已经被知道了至少几十年，并且预计将提供用于光伏电池的硅材料的新的低成本生产路线，但是由于处理锌蒸气的困难，关于详细的反应动力学知之甚少。在此，使用石英管反应器在870°C至1020°C的温度范围内在各种停留时间下实验测量反应产率。在970°C下，反应产率从约50%增加到大于50%。当停留时间为10 s时，在870°C下为20%。可能的基元反应步骤也已通过量子化学计算进行了研究。提出了以SiCl2为中间物种的两步反应模型。该模型较好地描述了实验数据。此外，从实验数据和我们的反应模型的解析解，得到了总的反应速率常数。总活化能为3.2×102kJmol−1。
This report details a kinetic analysis on gas phase zinc reduction of silicon tetrachloride. Although this reaction has been known for at least several decades, and is expected to provide a new low cost production route for silicon materials for photovoltaic cells, little is known about the detailed reaction kinetics due to the difficulties in handling zinc vapor. Here, the reaction yields have been experimentally measured at various residence times using a quartz tube reactor over a range of temperatures from 870°C to 1020°C. Reaction yields increased to greater than 50% at 970°C from ca. 20% at 870°C when the residence time was 10s. Possible elementary reaction steps have also been investigated by quantum chemical calculations. A two-step reaction model with SiCl2as an intermediate species has been proposed. This model describes the experimental data well. Furthermore, from experimental data and analytical solution of our reaction model, the overall reaction rate constants were obtained. The overall activation energy was 3.2×102kJmol−1.