Density Functional Tight-Binding Simulations Reveal the Presence of Surface Defects on the Quartz (101)–Water InterfaceClick to copy article linkArticle link copied!
- Ke Yuan*Ke Yuan*Email: [email protected]. Phone: 865-576-7184.Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United StatesMore by Ke Yuan
- Nikhil RampalNikhil RampalDepartment of Chemical Engineering, Columbia University, New York, New York 10027, United StatesMore by Nikhil Rampal
- Paul FenterPaul FenterChemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, United StatesMore by Paul Fenter
- James D. KubickiJames D. KubickiDepartment of Geological Sciences, University of Texas at El Paso, El Paso, Texas 79968, United StatesMore by James D. Kubicki
- Andrew G. StackAndrew G. StackChemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United StatesMore by Andrew G. Stack
- Stephan Irle*Stephan Irle*Email: [email protected]. Phone: 865-574-7192.Computational Sciences and Engineering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United StatesMore by Stephan Irle
Abstract
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.
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