Distribution of water molecules at Ag(111)/electrolyte interface as studied with surface X-ray scattering

Toney, Michael F.; Howard, Jason N.; Richer, Jocelyn; Borges, Gary L.; Gordon, Judith R.; Melroy, Owen R.; Wiesler, David G.; Yee, Dennis; Sorensen, L. B.

doi:10.1016/0039-6028(95)00455-6

Cited by 173 publications

(140 citation statements)

References 27 publications

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“…3). Our results show that the pronounced water density layering at the mineral surface dissipates within about 9 Å (three times the diameter of a water molecule), in agreement with previous studies of water on flat solid surfaces [30,37,38,94,95]. The z coordinates of the first shoulder and first four peaks of the water density profile are reported in [44,53] of the first shoulder and first two peaks of the water density profile to water molecules that form hydrogen bonds with two (z* ≈ 1.8 Å), one (z* = 2.7 Å), or no surface O atoms (z* = 4.0 Å), respectively (Fig.…”

Section: Interfacial Water Structuresupporting

confidence: 92%

Molecular dynamics simulations of the electrical double layer on smectite surfaces contacting concentrated mixed electrolyte (NaCl–CaCl2) solutions

Bourg

Sposito

2011

Journal of Colloid and Interface Science

254

228

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We report new molecular dynamics results elucidating the structure of the electrical double layer (EDL) on smectite surfaces contacting mixed NaCl-CaCl 2 electrolyte solutions in the range of concentrations relevant to pore waters in geologic repositories for CO 2 or high-level radioactive waste (0.34 to 1.83 mol c dm -3 ). Our results confirm the existence of three distinct ion adsorption planes (0-, β-, and d-planes), often assumed in EDL models, but with two important qualifications: (1) the location of the β-and dplanes are independent of ionic strength or ion type and (2) "indifferent electrolyte" ions can occupy all three planes. Charge inversion occurred in the diffuse ion swarm because of the affinity of the clay surface for CaCl + ion pairs. Therefore, at concentrations ≥ 0.34 mol c dm -3 , properties arising from long-range electrostatics at interfaces (electrophoresis, electro-osmosis, co-ion exclusion, colloidal aggregation) will not be correctly predicted by most EDL models. Co-ion exclusion, typically neglected by surface speciation models, balanced a large part of the clay mineral structural charge in the more concentrated solutions. Water molecules and ions diffused relatively rapidly even in the first statistical water monolayer, contradicting reports of rigid "ice-like" structures for water on clay mineral surfaces.

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Section: Interfacial Water Structuresupporting

confidence: 92%

Molecular dynamics simulations of the electrical double layer on smectite surfaces contacting concentrated mixed electrolyte (NaCl–CaCl2) solutions

Bourg

Sposito

2011

Journal of Colloid and Interface Science

254

228

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“…As discussed in Hiemstra and van Riemsdijk (2006), the double layer structure that emerges can be explained by the alignment of water molecules near the surface in several layers, in which the electrolyte ions can only change stepwise their position. This picture agrees with experimental information obtained by different valuable approaches like force measurements (Pashley and Israelachvili, 1984;Israelachvili and Wennerstrom, 1996), X-ray reflectivity (Toney et al, 1995;Fenter and Sturchio, 2004;Catalano et al, 2006) and Sum Frequency Spectroscopy (Yeganeh et al, 1999;Kataoka et al, 2004;Ostroverkhov et al, 2005;Shen and Ostroverkhov, 2006). These measurements show increase in the ordering of water within a distance of about 0.7-0.9 nm, which is equivalent to about 2-3 layers of water molecules .…”

Section: Extended Stern Layer Modelsupporting

confidence: 89%

Adsorption and surface oxidation of Fe(II) on metal (hydr)oxides

Hiemstra

Riemsdijk

2007

Geochimica et Cosmochimica Acta

143

109

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“…If we identify the location of the silica surface with the Gibbs surface of water obtained from  Ow (z,r) in Figure 3-2, the surfaces of the SiO 2 slab are located at z = 64.3  0.1 and 125.7  0.1 Å (pore length 61.4 Å) and simulated pore radii are r = 4.39 and 9.37 Å. Plots of  Ow and  Hw vs. distance d (measured from Gibbs surface of water O atoms towards the aqueous phase) show density layering up to about three statistical water monolayers (~ 9 Å) from the silica surface ( Figure 3-3), consistent with the behavior of water on a range of solid surfaces (Toney et al, 1995;Schlegel et al, 2002;Bourg and Sposito, 2011). Average water O and H density distributions on the flat external surfaces and concave pore walls of our simulated silica structures (Figure 3-3a, b) are essentially identical beyond the first statistical water monolayer (d > ~ 3 Å).…”

Section: Interfacial Water Structuresupporting

confidence: 64%

Progress toward bridging from atomistic to continuum modeling to predict nuclear waste glass dissolution.

Zapol

Bourg

Criscenti³

et al. 2011

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This report summarizes research performed for the Nuclear Energy Advanced Modeling and Simulation (NEAMS) Subcontinuum and Upscaling Task. The work conducted focused on developing a roadmap to include molecular scale, mechanistic information in continuum-scale models of nuclear waste glass dissolution. This information is derived from molecular-scale modeling efforts that are validated through comparison with experimental data. In addition to developing a master plan to incorporate a subcontinuum mechanistic understanding of glass dissolution into continuum models, methods were developed to generate constitutive dissolution rate expressions from quantum calculations, force field models were selected to generate multicomponent glass structures and gel layers, classical molecular modeling was used to study diffusion through nanopores analogous to those in the interfacial gel layer, and a micro-continuum model (KµC) was developed to study coupled diffusion and reaction at the glass-gel-solution interface. We would also like to acknowledge discussions with the International Corrosion Working Group members including Stéphane Gin,

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Distribution of water molecules at Ag(111)/electrolyte interface as studied with surface X-ray scattering

Cited by 173 publications

References 27 publications

Molecular dynamics simulations of the electrical double layer on smectite surfaces contacting concentrated mixed electrolyte (NaCl–CaCl2) solutions

Molecular dynamics simulations of the electrical double layer on smectite surfaces contacting concentrated mixed electrolyte (NaCl–CaCl2) solutions

Adsorption and surface oxidation of Fe(II) on metal (hydr)oxides

Progress toward bridging from atomistic to continuum modeling to predict nuclear waste glass dissolution.

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