期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 125, 期 29, 页码 16246-16255出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.1c03689
关键词
-
资金
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division
- National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility [DE-AC02-05CH11231]
- Office of Science of the U.S. Department of Energy [DE-AC05-00OR22725]
The researchers used density functional tight-binding (DFTB) to simulate the structures of quartz surfaces with different types and densities of defects in water, revealing that the rotation of surface [SiO4] tetrahedra near Si vacancies can lead to outward displacements of Si atoms and inward relaxations of terminal oxygens.
Understanding the structure and reactivity of quartz-water interfaces is critical for numerous applications in the geological, environmental, and biological sciences. However, disagreements on the atomic-level structure of the interfaces between experiments and simulations are hampering our ability to predict the surface reactivity. Here, we used density functional tight-binding (DFTB)-based molecular dynamics to simulate a series of quartz (101) surfaces having different types and densities of surface defects in water and compared them with the structures determined by X-ray reflectivity measurements. The DFTB simulations are able to reproduce previous classical and quantum mechanical predictions of the pristine quartz (101)-water interface that disagree with experimental observations. To remedy this situation, a set of defective quartz surfaces having various surface silicon (Si) vacancies were built as indicated by recent experimental studies. We found that the rotation of surface [SiO4] tetrahedra near Si vacancies can lead to outward displacements of Si atoms similar to those observed in the experiments. The presence of additional surface Si vacancies caused inward relaxations of terminal oxygens through the formation of hydrogen bonds. The overall results indicate that the quartz (101)-water interface may include a mixture of geminal ( Si-(OH)(2))- and vicinal ( Si-OH)-type silanol groups together with the presence of surface Si vacancies.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据