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WIREs Comput Mol Sci
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Investigations of water/oxide interfaces by molecular dynamics simulations

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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
The structure of α‐alumina (0001) and () surfaces. Water is not shown for clarity and gray, purple and white color represent aluminum, oxygen and hydrogen atoms, respectively. The top two figures show the top view of (0001) (a) and () (b) surfaces; the bottom two show the side view of (0001) (c) and () (d) surfaces. The numbers in figure (b) and (d) represent how many aluminum atoms are connected with each oxygen, that is, the “x” of AlxOH. The figures only show one simulation box so the periodic boundary condition is broken
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The mechanism of how strained silica become unstrained silica. (a) Strained silica, the initial state. (b–d) Intermediate defect structures. (e) Unstrained silica, the final state. Reprinted with permission from Ref. 118. Copyright (2016) American Chemical Society
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The calculation of ΔpKa of pyruvic acid at an interface. The structures are the protonated acid (HA) and the deprotonated ion (A). (a) Initial state with HA at the surface and A in the bulk. (b) Final state with A at the surface and HA in the bulk. Reprinted with permission from Ref. 102. Copyright (2018) American Chemical Society
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Classification of silanols on amorphous silica surfaces. “Isolated” silanols are not hydrogen bonded with other silanols; “vicinal” silanols share one common oxygen atoms and “geminal” silanols have two OH groups connected with one silicon atom. Reprinted with permission from Ref. 101. Copyright (2015) American Chemical Society
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Different ion binding modes between ions and the β‐crystabolite (001) surface. Yellow, red, white, blue, orange and green balls represent Si, O, H, Na, Mg, and Cu atoms(ions), respectively. (a,b) Na+ binding modes, (c) Mg2+ directly binds to the surface, (d) Mg2+ with completed hydration shell. (e) Cu2+ binds to the surface, (f,g) Cu(OH)(H2O)3 complex ion. Reprinted with permission from Ref. 87. Copyright (2018) American Chemical Society
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Influence of ions on water orientation at the water/silica interface. θ is the angle between the opposite of the water dipole and silica surface normal. The silica surface is negatively charged. (a) after adding NaCl, the surface potential and <cos θ> in the diffuse layer become positive (oxygen close to the surface). (b) CsCl follows the Gouy–Chapman–Stern model. The surface potential and <cos θ> in diffuse layer remain negative (hydrogen close to the surface). Reprinted with permission from Ref. 18. Copyright (2014) American Chemical Society
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Number of articles published since 2010 by searching “water,” “interface,” and “molecular dynamics simulations” as key words. Source: “Web of Science”
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A snapshot of a surface following the Gouy–Chapman–Stern model. At the interface, cations are in excess because the mineral surface is negatively charged. Legend: Blue and green balls represent positive and negative ions, respectively; red and white sticks represent the hydration shells of ions
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Free energy profile of proton transfer from NNP‐MD simulations at the (a) ZnO interface and (b,c) ZnO interface. For the ZnO interface, proton transfer along the (0001) direction has a high barrier (3.5 kBT, green in (a)), but that along the is more accessible. For the ZnO interface, proton transfer is along both two directions. Reprinted from Ref. 193—Published by The Royal Society of Chemistry
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Comparison of vSFG spectra of the water/α‐alumina (0001) interface from experiments and AIMD simulations. The spectrum predicted by SCAN agrees best with experiments in this work. Spectra from PBE or PBE‐TS overestimate intensities at low frequency while features at low frequency are missing in RPBE. Reprinted with permission from Ref. 131. Copyright (2019) American Chemical Society
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BMP‐2 adsorption modes at different water/TiO2 interfaces. Purple color highlights the wrist epitope, which shows different orientations depending on the surface terminated groups. (a,b) at the OH‐terminated anatase(101) surface, the wrist epitope either points down or stays flat, (c) at the phosphite‐terminated anatase(101) surface, the orientation of the BMP‐2 changed and its wrist epitope points up. It also points down (d) or stays flat (e) at the OH‐terminated and points up (f) at the phosphite‐terminated rutile(110) surface. Reprinted with permission from Ref. 168. Copyright (2018) American Chemical Society
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Water dissociative adsorption on TiO2 surfaces: (a) the structure of anatase (101) and (b) rutile (110) surfaces with atom labels; (c) before and (d) after water dissociation at the anatase (101) surface; (e) before and (f) after water dissociation at the rutile (110) surface. Reprinted with permission from Ref. 151. Copyright (2017) American Chemical Society
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Comparison of experimental and simulated electron density profiles of the water/α‐alumina (0001) interface. The “zz0” is the distance of Z direction (surface normal) and 0 is set to the surface outmost oxygen plane. Black curve (“best fit”) is the fitted electron density from XRR measurements. Blue (“PBE”) and green (“optB88”) curves are results directly calculated from AIMD simulations using different functionals. Red curve (“CMD”) is results from classical simulations. Reprinted from Ref. 139
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Surface excess ions per unit surface area, Γ(Z), profile of F and I near the water/α‐alumina (0001) interface. The counter‐ion is Na+. Comparing to results with the Al‐O‐H angle bending potential, simulations without it underestimate ion adsorption. Reprinted with permission from Ref. 125. Copyright (2019) American Chemical Society
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Structure and Mechanism > Molecular Structures
Molecular and Statistical Mechanics > Molecular Interactions
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