Water Structure, Dynamics and Ion Adsorption at the Aqueous {010} Brushite Surface

Garcia, Natalya A.; Raiteri, Paolo; Vlieg, E.; Gale, Julian D.

doi:10.3390/min8080334

Cited by 12 publications

(13 citation statements)

References 39 publications

(57 reference statements)

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“…Oxide/organic interfaces play a critical role in a wide range of fields, such as heterogeneous catalysis, 1,2 (photo)electrochemistry, 3 biological [4][5][6][7][8][9][10] and geological 11,12 interfaces (with the specific case of nanoconfined liquids 13 ), corrosion 14 and lubrication. 15,16 In this paper, we will focus on modeling the interaction of organic molecules with typical oxide surfaces of utmost importance: the hematite (0001) surface 17 as well as the γ-alumina (100) and (110) surfaces.…”

Section: Introductionmentioning

confidence: 99%

Transferable Gaussian Attractive Potentials for Organic/oxide Interfaces

Rey¹,

Blanck²,

Clabaut³

et al. 2021

Preprint

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Organic/oxide interfaces play an important role in many areas of chemistry, and in particular for lubrication and corrosion. Molecular dynamics simulations are the method of choice for providing complementary insight to experiments. However, the force fields used to simulate the interaction between molecules and oxide surfaces tend to capture only weak physisorption interactions, discarding the stabilizing Lewis acid/base interactions. We here propose an improvement of the usual molecular mechanics description (based on Lennard-Jones and electrostatic interactions) by addition of an attractive Gaussian potential between reactive sites of the surface and heteroatoms of adsorbed organic molecules, leading to the GLJ potential. The interactions of four oxygenated and four amine molecules with the typical and widespread hematite and γ-alumina surfaces are investigated. The total RMSD for all probed molecules decreases from 29.2 to 5.7 kcal/mol, and the corresponding percentage from 107.4 to 22.6% over hematite, while on γ-alumina the RMSD decreases from 21.5 to 7.6 kcal/mol, despite using a single parameter for all five chemically inequivalent surface aluminum atoms. Applying GLJ to the simulation of n-octadecanamine and N-tetradecyldiethanolamine adsorbed films on hematite and alumina respectively demonstrates that mobility of the surfactants is overestimated by the common LJ potential, while GLJ shows a strong structuration and slow dynamics of the surface films, as could be expected from the first-principles adsorption energies for model head-groups.

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Section: Introductionmentioning

confidence: 99%

Transferable Gaussian Attractive Potentials for Organic/oxide Interfaces

Rey¹,

Blanck²,

Clabaut³

et al. 2021

Preprint

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show abstract

“…The combination of diffraction data and simulations has been employed several times, [4][5][6][7][8] but so far this never involved directly fitting all three-dimensional atomic coordinates (i.e. height and lateral position) to the structure factors measured with SXRD.…”

Section: Introductionmentioning

confidence: 99%

The Calcite (104) Surface - Electrolyte Structure: A 3D Comparison of Surface X-Ray Diffraction and Simulations

Raiteri¹,

Accordini²,

Megens³

et al. 2020

Preprint

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<div>Adsorption and incorporation of ions is known to influence the morphology and growth of calcite. Using surface X-ray diffraction, the interfacial structure of calcite in contact with CaCO3, MgCl2, CaCl2</div><div>and BaCl2 solutions was determined. All of these conditions yield a comparable interfacial structure,</div><div>meaning that there is no significant ion adsorption. This allows for the first time a thorough comparison in all three dimensions with state-of-the-art computer simulations, involving molecular dynamics</div><div>based on both DFT and two different force field models. Additionally, the simulated structures are</div><div>used to calculate the corresponding structure factors, which in turn are compared to those obtained</div><div>from experiment, thereby avoiding the need for fitting or subjective interpretation. In general, there</div><div>is a good agreement between experiment and the simulations, though there are some small discrepancies in the atomic positions, which lead to an inadequate fit of certain features characteristic of the</div><div>structure of water at the interface. Of the three simulation methods examined, the DFT results were</div><div>found to agree best with the experimental structure.</div>

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“…Measured oscillatory forces were ascribed to ordering of hydration layers under confinement between the two surfaces. Since then, Xray reflectivity and diffraction techniques have provided information on mineral-aqueous interfaces free from confinement 13 , proving conclusively that ion and solvent distributions within one nanometer of a surface differ drastically from the bulk 14,15,16,17 . However, these techniques are limited to large atomically-smooth surfaces and are often incapable of achieving atomic-scale lateral resolution.…”

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confidence: 99%

Atomic-Scale Variations of Interfacial Water Structure Driven by Site-Specific Chemistry

Nakouzi¹,

Stack²,

Kerisit³

et al. 2020

Preprint

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<p>Although interfacial solution structure impacts environmental, biological and technological phenomena, including colloidal stability, protein assembly, heterogeneous nucleation, and water desalination, its molecular details remain poorly understood. Here, we visualize the three-dimensional (3D) hydration structure at the boehmite(010)-water interface using fast force mapping (FFM). Using a self-consistent scheme to decouple long-range tip-sample interactions from short-range solvation forces, we obtain the solution structure with lattice resolution. The results are benchmarked against molecular dynamics simulations that explicitly include the effects of the tip with different levels of approximation and systematically account for tip size, chemistry, and confinement effects. We find four laterally structured water layers within one nanometer of the surface, with the highest water densities at sites adjacent to hydroxyl groups. The findings reveal a complex relationship between site-specific chemistry, water density, and long-range particle interactions; and represent a major step forward towards quantitative data interpretation and widespread implementation of 3D FFM.</p>

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Water Structure, Dynamics and Ion Adsorption at the Aqueous {010} Brushite Surface

Cited by 12 publications

References 39 publications

Transferable Gaussian Attractive Potentials for Organic/oxide Interfaces

Transferable Gaussian Attractive Potentials for Organic/oxide Interfaces

The Calcite (104) Surface - Electrolyte Structure: A 3D Comparison of Surface X-Ray Diffraction and Simulations

Atomic-Scale Variations of Interfacial Water Structure Driven by Site-Specific Chemistry

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