Investigations of water/oxide interfaces by molecular dynamics simulations

Abstract

Water/oxide interfaces are ubiquitous on earth and show significant influence on many chemical processes. For example, understanding water and solute adsorption as well as catalytic water splitting can help build better fuel cells and solar cells to overcome our looming energy crisis; the interaction between biomolecules and water/oxide interfaces is one hypothesis to explain the origin of life. However, knowledge in this area is still limited due to the difficulty of studying water/solid interfaces. As a result, research using increasingly sophisticated experimental techniques and computational simulations has been carried out in recent years. Although it is difficult for experimental techniques to provide detailed microscopic structural information, molecular dynamics (MD) simulations have satisfactory performance. In this review, we discuss classical and ab initio MD simulations of water/oxide interfaces. Generally, we are interested in the following questions: How do solid surfaces perturb interfacial water structure? How do interfacial water molecules and adsorbed solutes affect solid surfaces and how do interfacial environments affect solvent and solute behavior? Finally, we discuss progress in the application of neural network potential based MD simulations, which offer a promising future because this approach has already enabled ab initio level accuracy for very large systems and long trajectories. This article is categorized under: Theoretical and Physical Chemistry > Spectroscopy Molecular and Statistical Mechanics > Molecular Interactions Structure and Mechanism > Molecular Structures

pH dependent reactivity of boehmite surfaces from first principles molecular dynamics

“…ClayFF does not support OH bond breaking, thus dissociative adsorption cannot occur during CMD. This combination of physi- and chemisorption events of H 2 O—a mechanism universally seen at water:metal–(hydr)oxide interfaces 38–40 —stabilizes the surface energy ( vide infra ).…”

Superhydrophilicity of α-alumina surfaces results from tight binding of interfacial waters to specific aluminols

“…Water is one of the most important substances [1,2,3,4] and water/oxide interfaces are ubiquitous on earth, playing important roles in numerous chemical, physical, geological, and biological processes, [5,6,7,8] such as mineral degradation, [9,10] heterogeneous catalysis, [11] phase transitions, [12] solute adsorption [13,14] and wetting. [15,16] Investigating the behavior of interfacial waters is essential to help the design and development of better materials to overcome the energy crisis or increase their biological compatibility.…”

Binding of polar and hydrophobic molecules at the LiCoO2(001)-water interface: force field development and molecular dynamics simulations

“…Since the binding of charged and hydrophobic molecules is expected to perturb the local hydration environment, 14,15 explicit solvent simulations are preferable to implicit solvent models, 16,17 especially for binding kinetics. Explicit solvent simulations with quantum mechanical potential functions are computationally demanding, and state-of-the-art simulations typically reach 10-100 picoseconds of sampling, 18,19 which is usually not sufficient for converging binding free energies. 14 Molecular dynamics simulations using empirical force fields are much more affordable, but parameterization of reliable force fields for metal oxide/water interface requires considerable amount of efforts, although largely automated machine learning techniques have been shown to be promising in recent studies.…”