Kinetic Monte Carlo Study on the Role of Heterogeneity in the Dissolution Kinetics of Glasses
Kinetic Monte Carlo Study on the Role of Heterogeneity in the Dissolution Kinetics of Glasses
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DOI：
10.1021/acs.jpcc.3c01123
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发表时间：
2023-04
期刊：
影响因子：
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通讯作者：
Luis Ruiz Pestana;Swathi Shantha Raju;Chaitanya Guntoorkar;P. Suraneni
中科院分区：
文献类型：
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作者：
Luis Ruiz Pestana;Swathi Shantha Raju;Chaitanya Guntoorkar;P. Suraneni
硅酸盐和其他氧化物玻璃的溶解调节许多自然过程，并在许多技术应用中发挥重要作用。尽管这些玻璃本质上是异质的，但目前的玻璃溶解理论完全依赖于玻璃结构或化学性质的平均描述符。玻璃的局部结构和化学组成的空间波动对其溶解动力学的影响还没有得到很好的理解。在这里，我们使用动力学蒙特卡罗（KMC）模拟阐明的作用，异质性发挥溶解动力学的玻璃模型系统。在单相颗粒中，我们发现，异质性，远离单调的效果，可以减缓或加速溶解取决于平均程度的无序的玻璃。在两相颗粒中，我们发现相分离系统的溶解动力学由不太可溶的相控制，而对于良好混合的系统，溶解可以比等效的单相系统更快，因为随着更可溶的相溶解，它留下了稀疏的结构，不太可溶的相，然后可以更快地溶解。我们解释我们的研究结果的基础上观察到的KMC模拟和理论论据的溶解机制。
The dissolution of silicate and other oxide glasses regulates many natural processes and plays an important role in many technological applications. Despite the fact that these glasses are inherently heterogeneous, current theories of glass dissolution exclusively rely on average descriptors of the structure or chemistry of the glass. The effect that spatial fluctuations in the local structure and chemical composition of a glass has on its dissolution kinetics is not well understood. Here, we use kinetic Monte Carlo (KMC) simulations to elucidate the role that heterogeneity plays in the dissolution kinetics of a glass model system. In single-phase particles, we find that heterogeneity, far from having a monotonic effect, can slow down or speed up the dissolution depending on the average extent of disorder of the glass. In two-phase particles, we find that the dissolution kinetics of phase-separated systems is governed by the less-soluble phase, while for well-mixed systems, the dissolution can be faster than that of the equivalent single-phase system because as the more soluble phase dissolves, it leaves behind a sparse structure of the less soluble phase which can then dissolve faster. We explain our findings based on both the mechanisms of dissolution observed in the KMC simulations and theoretical arguments.