LaMer爆裂数据的成核和生长动力学,The Journal of Physical Chemistry A

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LaMer爆裂数据的成核和生长动力学
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2017-10-03 00:00:00 , DOI: 10.1021/acs.jpca.7b08368
Daniel B. K. Chu ₁ , Jonathan S. Owen ₂ , Baron Peters _{1,

3}

Affiliation

在LaMer爆发形核中，单个形核事件大量发生，几乎同时，并且在几乎相同的均质条件下。这些特性使LaMer爆裂成核对于需要单分散颗粒的应用以及理论分析都很重要。Sugimoto及其同事预测，LaMer爆发期间产生的核数仅取决于溶质供给速率和生长速率，而与成核动力学无关。一些实验证实溶质供给动力学控制着核的数量，但是原始理论分析中的缺陷引起了有关生长和成核动力学的预测作用的疑问。我们对控制原子核和溶质浓度的耦合方程式进行了严格的分析。我们的分析证实，核的数量在很大程度上取决于溶质的供应和增长率，但是我们的预测关系不同于Sugimoto等人的关系。此外，我们发现在生长动力学缓慢的系统中应出现更多依赖于核尺寸的校正。最后，我们展示了成核动力学如何确定粒度分布。我们建议测得的粒度分布可能因此提供了测试均相成核动力学理论模型的方法。

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Nucleation and Growth Kinetics from LaMer Burst Data

In LaMer burst nucleation, the individual nucleation events happen en masse, quasi-simultaneously, and at nearly identical homogeneous conditions. These properties make LaMer burst nucleation important for applications that require monodispersed particles and also for theoretical analyses. Sugimoto and co-workers predicted that the number of nuclei generated during a LaMer burst depends only on the solute supply rate and the growth rate, independent of the nucleation kinetics. Some experiments confirm that solute supply kinetics control the number of nuclei, but flaws in the original theoretical analysis raise questions about the predicted roles of growth and nucleation kinetics. We provide a rigorous analysis of the coupled equations that govern concentrations of nuclei and solutes. Our analysis confirms that the number of nuclei is largely determined by the solute supply and growth rates, but our predicted relationship differs from that of Sugimoto et al. Moreover, we find that additional nucleus size dependent corrections should emerge in systems with slow growth kinetics. Finally, we show how the nucleation kinetics determine the particle size distribution. We suggest that measured particle size distributions might therefore provide ways to test theoretical models of homogeneous nucleation kinetics.

更新日期：2017-10-04

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