Electronic structure of aqueous-phase anatase titanium dioxide nanoparticles probed by liquid jet photoelectron spectroscopy

Ali, Hebatallah; Seidel, Robert; Bergmann, Arno; Winter, Bernd

doi:10.1039/c8ta09414d

Cited by 26 publications

(36 citation statements)

References 86 publications

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“…For example, much experiment and theory demonstrates that, to describe electron transfer across (charged) solid-water interfaces, such as for the photocatalytic water splitting into hydrogen and oxygen at an electrode-solution interface, details of the interfacial molecular arrangement of water are quintessential. The interface can act to align water molecules, but the water molecules can act back on the interface, through both protonation and deprotonation, and dissociative adsorption at the interface 59,60 , thus changing the local charge and surface potential (Fig. 1; Box 1).…”

Section: Nature Reviews | Chemistrymentioning

confidence: 99%

Water at charged interfaces

et al. 2021

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The ubiquity of aqueous solutions in contact with charged surfaces and the realization that the molecular-level details of water-surface interactions often determine interfacial functions and properties relevant in many natural processes have led to intensive research. Even so, many open questions remain regarding the molecular picture of the interfacial organization and preferential alignment of water molecules, as well as the structure of water molecules and ion distributions at different charged interfaces. While water, solutes and charge are present in each of these systems, the substrate can range from living tissues to metals. This diversity in substrates has led to different communities considering each of these types of aqueous interface. In this Review, by considering water in contact with metals, oxides and biomembranes, we show the essential similarity of these disparate systems. While in each case the classical mean-field theories can explain many macroscopic and mesoscopic observations, it soon becomes apparent that such theories fail to explain phenomena for which molecular properties are relevant, such as interfacial chemical conversion. We highlight the current knowledge and limitations in our understanding and end with a view towards future opportunities in the field.

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Section: Nature Reviews | Chemistrymentioning

confidence: 99%

Water at charged interfaces

et al. 2021

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“…The A 101 active sites for molecule adsorption are Ti 5c and O 2c . 10,22,26,27,55 Ti 5c can bind to the oxygen atom of H 2 O and the OH radicals as well as to CH 3 CH 2 OH and CH 3 CH 2 O groups. O 2c binds to the protons generated by dissociative adsorptions.…”

Section: Water and Ethanol Adsorption At The A 101 Surfacementioning

confidence: 99%

“…21 Resolving the atomic structure of the A 101 /solvent interface is experimentally challenging. 11,16,22 Ab initio simulations are particularly valuable in this context, allowing for the accurate modeling of these systems as a function of varying external conditions. 23 In fact, Density Functional Theory (DFT) has become the main workhorse for atomistic simulations, providing a high predictive power for structural properties in materials science at an affordable computational cost.…”

Section: Introductionmentioning

confidence: 99%

Wet Environment Effects for Ethanol and Water Adsorption on Anatase TiO₂ (101) Surfaces

et al. 2019

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Titanium dioxide exhibits superior photocatalytic properties, mainly occurring in liquid environments through molecular adsorptions and dissociations at the solid/liquid interface. The presence of these wet environments is often neglected when performing ab initio calculations for the interaction between the adsorbed molecules and the TiO 2 1 surface. In this study we consider two solvents, i.e. water and ethanol, and show that the proper inclusion of the wet environment in the methodological scheme is fundamental for obtaining reliable results. Our calculations are based on structure predictions at a density functional theory level for molecules interacting with the perfect and defective anatase (1 0 1) surface under both vacuum and wet conditions. A soft-sphere implicit solvation model is used to describe the polar character of the two solvents. As a result, we find that surface oxygen vacancies become energetically favorable with respect to subsurface vacancies at the solid/liquid interface. This aspect is confirmed by ab initio molecular dynamics simulations with explicit water molecules. Ethanol molecules are able to strongly passivate these vacancies, whereas water molecules only weakly interact with the (1 0 1) surface, allowing the coexistence of surface vacancy defects and adsorbed species. Infrared and photoluminescence spectra of anatase nanoparticles exposing predominantly (1 0 1) surfaces dispersed in water and ethanol support the predicted molecular-surface interactions, validating the whole computational paradigm. The combined analysis allows for a better interpretation of TiO 2 processes in wet environments based on improved computational models with implicit solvation features.

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“…Water interaction with curved TiO 2 surfaces is of utmost importance because water can compete with any other chemical species for the adsorption on surface sites as a donor on low-coordinated Ti atoms and as an H-bonding species on lowcoordinated O atoms. 24,25 Also, dissociation of water on the surface sites or defects leads to the formation of OH species, which are crucial functional groups for surface chemistry, functionalization and molecular anchoring. 26 Additionally, mono-or multi-layered water adsorption may alter the surface electronic properties and work function, as well as the surface energy leading to different reconstructions than in ultra-high vacuum conditions.…”

Section: Introductionmentioning

confidence: 99%

Reactive molecular dynamics simulations of hydration shells surrounding spherical TiO₂nanoparticles: implications for proton-transfer reactions

Soria

Valentin

2021

Nanoscale

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Electronic structure of aqueous-phase anatase titanium dioxide nanoparticles probed by liquid jet photoelectron spectroscopy

Abstract: Proposed pH-dependent mechanism of TiO2–water interaction.

Cited by 26 publications

References 86 publications

Water at charged interfaces

Water at charged interfaces

Wet Environment Effects for Ethanol and Water Adsorption on Anatase TiO₂ (101) Surfaces

Reactive molecular dynamics simulations of hydration shells surrounding spherical TiO₂nanoparticles: implications for proton-transfer reactions

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Electronic structure of aqueous-phase anatase titanium dioxide nanoparticles probed by liquid jet photoelectron spectroscopy

Abstract: Proposed pH-dependent mechanism of TiO2–water interaction.

Cited by 26 publications

References 86 publications

Water at charged interfaces

Water at charged interfaces

Wet Environment Effects for Ethanol and Water Adsorption on Anatase TiO2 (101) Surfaces

Reactive molecular dynamics simulations of hydration shells surrounding spherical TiO2nanoparticles: implications for proton-transfer reactions

Contact Info

Product

Resources

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Wet Environment Effects for Ethanol and Water Adsorption on Anatase TiO₂ (101) Surfaces

Reactive molecular dynamics simulations of hydration shells surrounding spherical TiO₂nanoparticles: implications for proton-transfer reactions