Direct Prediction of Calcite Surface Wettability with First-Principles Quantum Simulation

Abstract

Prediction of intrinsic surface wettability from first-principles offers great opportunities in probing new physics of natural phenomena and enhancing energy production or transport efficiency. We propose a general quantum mechanical approach to predict the macroscopic wettability of any solid crystal surfaces for different liquids directly through atomic-level density functional simulation. As a benchmark, the wetting characteristics of calcite crystal (10.4) under different types of fluids (water, hexane, and mercury), including either contact angle or spreading coefficient, are predicted and further validated with experimental measurements. A unique feature of our approach lies in its capability of capturing the interactions among various polar fluid molecules and solid surface ions, particularly their charge density difference distributions. Moreover, this approach provides insightful and quantitative predictions of complicated surface wettability alteration problems and wetting behaviors of liquid/liquid/solid triphase systems.

Nonwetting Behavior of Al–Co Quasicrystalline Approximants Owing to Their Unique Electronic Structures

“…30 Besides electronic effects, the consideration of surface energies in our model is essential. Methods based on adsorption energies only, 48,60,61 although they appear well adapted for the determination of water-wetting properties, seems not to be adequate for the determination of wetting properties using a metal as a probe.…”

“…Methods based on free energy calculations are not as straightforward as the droplet simulations but tend to provide more accurate contact angle estimates. 48 Here, the contact angles are determined through the Young equation (Figure 2), 49,50 which involves surface (γ substrate ) and interfacial (γ interface ) energies…”

Wettability Alteration and Enhanced Oil Recovery Induced by Proximal Adsorption of Na+ , Cl− , Liu1, Wani2, Alhassan3 et al. 2018Phys. Rev. Applied485270View full textAdd to dashboardCite

“…This point is especially important when one is considering the effect of additive ions in the liquid. More recently, first-principles quantum MD simulations of such a solid-liquid interface were performed to study the intrinsic water wettability of the calcite surface [38], without considering the effect of brine composition and salinity.…”

The evolution in graphitic surface wettability with first-principles quantum simulations: the counterintuitive role of water

“…We investigate this by means of a DFT-based framework developed by one of the authors that previously demonstrated to be capable of predicting macroscopic surface wettability of solid surface in contact with different liquids 14 . We predict the macroscopic surface wettability of graphite surface without inputting any experimental parameters, including water surface tensions.…”

“…U + − S m L is the total energy of a graphite surface with (m-1) overlaying water layers, U mL is the total energy of the m th water monolayer, and n L is the number of molecules in one water monolayer, which is eight in our DFT simulation domain. Our computational framework 14 allows us to extract the adhesion energy water on graphite is shown in Fig. S1(e).…”