The elusive silica/water interface: isolated silanols under water as revealed by vibrational sum frequency spectroscopy

Dalstein, Laetitia; Potapova, Elizaveta; Tyrode, Eric

doi:10.1039/c7cp01507k

Cited by 131 publications

(175 citation statements)

References 46 publications

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“…Although the lowest SFG intensity of free SiOH on polished ISG could be attributed to the lower OH surface concentration, it should be noted that the orientation of OH groups may also contribute to this lowest intensity. 100 The SFG spectrum of fused quartz at 0% RH is in good agreement with SFG spectra at 0% RH reported in the literature. 100,108 SFG spectra of polished ISG, fused quartz, and Vycor at 40% RH are given in Fig.…”

Section: Simulations Of Hydrogen Bonds In Nano-porous Silica Gelssupporting

confidence: 89%

“…These spectral features are also referred as "icelike" (or "solid-like") and "liquid-like" structures, respectively, in the literature. 44,91 The precise assignments of these spectral bands, however, are controversial and still under investigations, 44,90,[92][93][94][95][96][97][98][99][100][101][102] and this study will refer to these spectral features as 3200 cm −1 band and 3400 cm −1 band.…”

Section: Simulations Of Hydrogen Bonds In Nano-porous Silica Gelsmentioning

confidence: 99%

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Hydrogen bonding interactions of H2O and SiOH on a boroaluminosilicate glass corroded in aqueous solution

et al. 2020

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Hydrogen bonding interactions play an important role in many chemical and physical processes occurring in bulk liquids and at interfaces. In this study, hydrous species (H 2 O and Si-OH) on nano-porous alteration layers (gels) formed on a boroaluminosilicate glass called International Simple Glass corroded in aqueous solutions at pH 7 and pH 9, and initially saturated with soluble siliconcontaining species were analyzed using linear and non-linear vibrational spectroscopy in combination with molecular dynamics simulations. The simulation results revealed various possible types of hydrogen bonds among these hydrous species in nanoconfinement environments with their populations depending on pore-size distribution. The nano-porous gels formed on corroded glass surfaces enhance hydrogen bond strength between hydrous species as revealed by attenuated total reflectance infrared spectroscopy. Sum frequency generation spectroscopy showed some significant differences in hydrogen bonding interactions on alteration layers formed at pH 7 and pH 9. The glass dissolution under the leaching conditions used in this study has been known to be ten times faster at pH 7 in comparison to that at pH 9 due to unknown reasons. The simulation and experimental results obtained in this study indicate that the water mobility in the gel formed at pH 9 could be slower than that in the gel formed at pH 7, and as a result, the leaching rate at pH 9 is slower than that at pH 7.npj Materials Degradation (2020) 4:1 ; https://doi.

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Section: Simulations Of Hydrogen Bonds In Nano-porous Silica Gelssupporting

confidence: 89%

Section: Simulations Of Hydrogen Bonds In Nano-porous Silica Gelsmentioning

confidence: 99%

Hydrogen bonding interactions of H2O and SiOH on a boroaluminosilicate glass corroded in aqueous solution

et al. 2020

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“…[6][7][8][9][10][11][12][13][14][15][16][17][18] As such, we employed Vibrational Sum Frequency Generation (V-SFG) spectroscopy for interrogating those interfacial properties, since it allows for probing vibrational states of interfacial molecules with sub-micrometer sensitivity and selectivity towards the symmetry-broken interfacial layers (given by the additional symmetry selection rule underlying V-SFG processes). Using this technique, we study how the presence of ions changes the composition of the EDL for water at a mineral surface.…”

Section: Introductionmentioning

confidence: 99%

Surface-specific vibrational spectroscopy of the water/silica interface: screening and interference

Schaefer

Gonella

Bonn

et al. 2017

Phys. Chem. Chem. Phys.

104

180

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Surface-specific vibrational sum-frequency generation spectroscopy (V-SFG) is frequently used to obtain information about the molecular structure at charged interfaces. Here, we provide experimental evidence that not only screening of surface charges but also interference limits the extent to which V-SFG probes interfacial water at sub-mM salt concentrations. As a consequence, V-SFG yields information about the Bsingle monolayer interfacial region not only at very high ionic strength, where the surface charge is effectively screened, but also for pure water due to the particularly large screening length at this low ionic strength. At these low ionic strengths, the large screening lengths cause destructive interference between contributions in the surface region. A recently proposed theoretical framework near-quantitatively describes our experimental findings by considering only interference and screening. However, a comparison between NaCl and LiCl reveals ion specific effects in the screening efficiency of different electrolytes. Independent of electrolyte, the hydrogen bonding strength of water right at the interface is enhanced at high electrolyte concentrations.

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“…Similarly, the formation of the electric double layer at the electrode/electrolyte interface needs to be considered, which involves not only solvent molecules but also solvated ions. Although some attempts have been made to understand the behavior of solvated ions at the interface with solids, [200][201][202][203][204][205] these types of studies are rather sparse due to limitations in the time and length scales accessible by FPMD approaches. In this regard, coupling FPMD to advanced sampling methods [206][207][208] and continuum solvation models [209,210] offers promising means to alleviate these problems.…”

Section: Discussionmentioning

confidence: 99%

Ab initio simulations of liquid electrolytes for energy conversion and storage

Pham

2018

Int J of Quantum Chemistry

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Understanding physicochemical properties of liquid electrolytes is essential for predicting and optimizing device performance for a wide variety of emerging energy technologies, including photoelectrochemical water splitting, supercapacitors, and batteries. In this work, we review recent progress and open challenges in predicting structural, dynamical, and electronic properties of the liquids using first-principles approaches. We briefly summarize the basic concepts of first-principles molecular dynamics (FPMD), and we discuss how FPMD methods have enriched our understanding of a number of liquids, including aqueous solutions, organic electrolytes and ionic liquids. We also discuss technical challenges in extending FPMD simulations to the study of liquid electrolytes in more complex environments, including the interface between electrolytes and electrodes, which is a key component in many energy storage and conversion systems. K E Y W O R D S energy conversion and storage, first-principles simulations, liquid electrolytes 1 | INTRODUCTIONLiquid electrolytes are essential components in a wide variety of emerging energy and environmental technologies, including hydrogen production through solar-water-splitting, [1,2] supercapacitors, [3][4][5] ion batteries, [6][7][8] and ion-selective membranes. [9][10][11] Within these devices, a large number of liquids have been explored, ranging from aqueous solutions and ionic liquids to organic, redox-type, and solid-state electrolytes. At the same time, continuing progress has been made during the past several decades in the development of novel liquids. For example, recent studies show that the use of highly concentrated aqueous electrolytes could open new opportunities for the design of high-voltage aqueous lithium-ion batteries while also significantly improving battery safety. [12,13] For several energy storage and conversion systems, the understanding of structure, dynamics, and electronic properties of liquid electrolytes is essential for predicting and optimizing device performance. For example, desolvation of ions in sub-nanometer carbon electrodes is known to lead to improved capacitive performance. [14][15][16] Controlling transport of the lithium ion in organic electrolytes and at the interface with the graphite anode is key to the development of next-generation lithium ion batteries. [17][18][19][20] Tailoring the electronic structures of aqueous solutions for facilitated charge transfer at semiconductor/water interfaces in photoelectrochemical cells is critical for improving the efficiency of water-splitting reactions for hydrogen production. [21,22] Last but not least, understanding the electronic properties of liquid electrolytes is one of the prerequisites for manipulating the electrochemical stability of electrode-electrolyte interfaces in ion batteries and supercapacitors. [5,23] Structural, dynamical, and electronic properties of liquid electrolytes are often intertwined. For example, it is now widely accepted that the solvation structure of ions in liquid...

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The elusive silica/water interface: isolated silanols under water as revealed by vibrational sum frequency spectroscopy

Cited by 131 publications

References 46 publications

Hydrogen bonding interactions of H2O and SiOH on a boroaluminosilicate glass corroded in aqueous solution

Hydrogen bonding interactions of H2O and SiOH on a boroaluminosilicate glass corroded in aqueous solution

Surface-specific vibrational spectroscopy of the water/silica interface: screening and interference

Ab initio simulations of liquid electrolytes for energy conversion and storage

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