Surface morphology effects on clathrate hydrate wettability
Surface morphology effects on clathrate hydrate wettability
复制标题
DOI：
10.1016/j.jcis.2021.12.083
复制
发表时间：
2022-04-01
影响因子：
9.9
通讯作者：
Striolo, Alberto
中科院分区：
文献类型：
--
作者：
Anh Phan;Stoner, Hannah M.;Striolo, Alberto
假设：笼形水合物优先在界面处形成;因此，润湿性在其形成、生长和附聚中起重要作用。实验证据表明，水合物制备过程会强烈影响接触角测量，导致文献中报道的不同结果。这些差异阻碍了技术进步。我们假设水合物表面形态的变化是负责文献中报道的接触角的广泛变化。实验：我们的假设的实验测试是有问题的，由于水合物的制备历史，其表面性质，和先进的表面表征的困难。因此，我们采用分子动力学模拟，这使我们能够系统地改变界面的功能和系统的组成。实施先进的算法，我们量化的基本热力学性质，以验证我们的观察。结果：我们实现了良好的协议与实验观察原子光滑和粗糙的水合物表面。我们的研究结果表明，接触线钉扎力，增强了表面的异质性，是负责改变水接触角，从而解释报道的实验数据之间的差异。我们的分析和分子水平的见解有助于解释粘附力测量，并更好地了解水合物颗粒之间的团聚，为推进流动保证应用提供微观工具。(c)2022年由Elsevier Inc.出版
Hypothesis: Clathrate hydrates preferentially form at interfaces; hence, wetting properties play an important role in their formation, growth, and agglomeration. Experimental evidence suggests that the hydrate preparation process can strongly affect contact angle measurements, leading to the different results reported in the literature. These differences hamper technological progress. We hypothesize that changes in hydrate surface morphologies are responsible for the wide variation of contact angles reported in the literature. Experiments: Experimental testing of our hypothesis is problematic due to the preparation history of hydrates on their surface properties, and the difficulties in advanced surface characterization. Thus, we employ molecular dynamics simulations, which allow us to systematically change the interfacial features and the system composition. Implementing advanced algorithms, we quantify fundamental thermodynamic properties to validate our observations. Findings: We achieve excellent agreement with experimental observations for both atomically smooth and rough hydrate surfaces. Our results suggest that contact line pinning forces, enhanced by surface heterogeneity, are accountable for altering water contact angles, thus explaining the differences among reported experimental data. Our analysis and molecular level insights help interpret adhesion force measurements and yield a better understanding of the agglomeration between hydrate particles, providing a microscopic tool for advancing flow assurance applications. (c) 2022 Published by Elsevier Inc.