Superhydrophilicity of <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="si22.svg"><mml:mrow><mml:mi>α</mml:mi></mml:mrow></mml:math>-alumina surfaces results from tight binding of interfacial waters to specific aluminols

Wang, Rui-yu; Zou, Yunqian; Remsing, Richard C.; Ross, Naomi O.; Klein, Michael L.; Carnevale, Vincenzo; Borguet, Eric

doi:10.1016/j.jcis.2022.07.164

Cited by 15 publications

(9 citation statements)

References 94 publications

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“…The formation of the first hydration layer is indicative of a pristine hydrophilic surface. Recent experiments corroborate that appropriate cleaning protocols lead to complete wetting of the sapphire (1120) and (0001) planes, with accompanying computational results suggesting these surfaces are super-hydrophilic . However, other experiments have suggested that hydroxyls increase the hydrophobicity of alumina, , revealing the evolving and often conflicting state of understanding around this surface.…”

Section: Theme 1: Structure and Dynamics Of Solid–aqueous Interfacesmentioning

confidence: 80%

“…Recent experiments corroborate that appropriate cleaning protocols lead to complete wetting of the sapphire (1120) and (0001) planes, with accompanying computational results suggesting these surfaces are super-hydrophilic. 176 However, other experiments have suggested that hydroxyls increase the hydrophobicity of alumina, 177,178 revealing the evolving and often conflicting state of understanding around this surface. Interestingly, in the case of the quartz (0001) surface, simulations show a hydrophobic hexameric water structure consistent with several other oxides, but they do not reveal dangling surface hydroxyls (Figure 11E), 162,179 unlike the alumina surface of kaolinite where dangling surface hydroxyls are located in the center of the adsorbed water hexamers (Figure 11A).…”

Section: Surface Restructuring From Liquidmentioning

confidence: 99%

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Oxide– and Silicate–Water Interfaces and Their Roles in Technology and the Environment

et al. 2023

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Interfacial reactions drive all elemental cycling on Earth and play pivotal roles in human activities such as agriculture, water purification, energy production and storage, environmental contaminant remediation, and nuclear waste repository management. The onset of the 21st century marked the beginning of a more detailed understanding of mineral aqueous interfaces enabled by advances in techniques that use tunable high-flux focused ultrafast laser and X-ray sources to provide near-atomic measurement resolution, as well as by nanofabrication approaches that enable transmission electron microscopy in a liquid cell. This leap into atomic-and nanometer-scale measurements has uncovered scale-dependent phenomena whose reaction thermodynamics, kinetics, and pathways deviate from previous observations made on larger systems. A second key advance is new experimental evidence for what scientists hypothesized but could not test previously, namely, interfacial chemical reactions are frequently driven by "anomalies" or "non-idealities" such as defects, nanoconfinement, and other nontypical chemical structures. Third, progress in computational chemistry has yielded new insights that allow a move beyond simple schematics, leading to a molecular model of these complex interfaces. In combination with surfacesensitive measurements, we have gained knowledge of the interfacial structure and dynamics, including the underlying solid surface and the immediately adjacent water and aqueous ions, enabling a better definition of what constitutes the oxide− and silicate−water interfaces. This critical review discusses how science progresses from understanding ideal solid−water interfaces to more realistic systems, focusing on accomplishments in the last 20 years and identifying challenges and future opportunities for the community to address. We anticipate that the next 20 years will focus on understanding and predicting dynamic transient and reactive structures over greater spatial and temporal ranges as well as systems of greater structural and chemical complexity. Closer collaborations of theoretical and experimental experts across disciplines will continue to be critical to achieving this great aspiration.

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Section: Theme 1: Structure and Dynamics Of Solid–aqueous Interfacesmentioning

confidence: 80%

Section: Surface Restructuring From Liquidmentioning

confidence: 99%

Oxide– and Silicate–Water Interfaces and Their Roles in Technology and the Environment

et al. 2023

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“…θ is the angle between the water orientation (defined by the sum of OH vectors) and the surface normal (Figure S5f). , As plotted in Figure a, χ zzz (2) increases when the surface potential becomes more negative regardless of the cation type. At the same potential, χ zzz (2) decreases in the order K + > Li + > Ba 2+ .…”

Section: Resultsmentioning

confidence: 95%

“…θ is the angle between the water orientation (defined by the sum of OH vectors) and the surface normal (Figure S5f). 44,45 As plotted in Figure 3a, χ zzz…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Cation Modifies Interfacial Water Structures on Platinum during Alkaline Hydrogen Electrocatalysis

Xu,

Wang,

Zhang

et al. 2024

J. Am. Chem. Soc.

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The molecular details of an electrocatalytic interface play an essential role in the production of sustainable fuels and value-added chemicals. Many electrochemical reactions exhibit strong cation-dependent activities, but how cations affect reaction kinetics is still elusive. We report the effect of cations (K+, Li+, and Ba2+) on the interfacial water structure using second-harmonic generation (SHG) and classical molecular dynamics (MD) simulation. The second- (χH2O (2)) and third-order (χH2O (3)) optical susceptibilities of water on Pt are smaller in the presence of Ba2+ compared to those of K+, suggesting that cations can affect the interfacial water orientation. MD simulation reproduces experimental SHG observations and further shows that the competition between cation hydration and interfacial water alignment governs the net water orientation. The impact of cations on interfacial water supports a cation hydration-mediated mechanism for hydrogen electrocatalysis; i.e., the reaction occurs via water dissociation followed by cation-assisted hydroxide/water exchange on Pt. Our study highlights the role of interfacial water in electrocatalysis and how innocent additives (such as cations) can affect the local electrochemical environment.

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“…Understanding the forces driving crystallization is relevant from a fundamental scientific perspective and for a wide range of practical applications. − In natural environments, crystalline solids are major components of rocks in the form of feldspar containing Si, Al, O, and other ions − with implications for climate change. In industrial scenarios, understanding crystallization processes is essential for improvement of material design and synthesis.…”

Section: Introductionmentioning

confidence: 99%

Is the Local Ion Density Sufficient to Drive NaCl Nucleation from the Melt and Aqueous Solution?

Wang,

Mehdi,

Zou

et al. 2024

J. Phys. Chem. B

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Even though nucleation is ubiquitous in different science and engineering problems, investigating nucleation is extremely difficult due to the complicated ranges of time and length scales involved. In this work, we simulate NaCl nucleation in both molten and aqueous environments using enhanced sampling of all-atom molecular dynamics with deep-learning-based estimation of reaction coordinates. By incorporating various structural order parameters and learning the reaction coordinate as a function thereof, we achieve significantly improved sampling relative to traditional ad hoc descriptions of what drives nucleation, particularly in an aqueous medium. Our results reveal a one-step nucleation mechanism in both environments, with reaction coordinate analysis highlighting the importance of local ion density in distinguishing solid and liquid states. However, although fluctuations in the local ion density are necessary to drive nucleation, they are not sufficient. Our analysis shows that near the transition states, descriptors such as enthalpy and local structure become crucial. Our protocol proposed here enables robust nucleation analysis and phase sampling and could offer insights into nucleation mechanisms for generic small molecules in different environments.

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Superhydrophilicity of α-alumina surfaces results from tight binding of interfacial waters to specific aluminols

Cited by 15 publications

References 94 publications

Oxide– and Silicate–Water Interfaces and Their Roles in Technology and the Environment

Oxide– and Silicate–Water Interfaces and Their Roles in Technology and the Environment

Cation Modifies Interfacial Water Structures on Platinum during Alkaline Hydrogen Electrocatalysis

Is the Local Ion Density Sufficient to Drive NaCl Nucleation from the Melt and Aqueous Solution?

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