Water at Interfaces

Björneholm, Olle; Hansen, Martin Hangaard; Hodgson, A.; Liu, Limin; Limmer, David T.; Michaelides, Angelos; Pedevilla, Philipp; Rossmeisl, Jan; Shen, Huaze; Tocci, Gabriele; Tyrode, Eric; Walz, Marie‐Madeleine; Werner, Josephina; Bluhm, Hendrik

doi:10.1021/acs.chemrev.6b00045

Cited by 647 publications

(631 citation statements)

References 299 publications

(629 reference statements)

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“…29 The present AIMD simulations predict three to four ordered water layers (L 1 to L 4 ) near the TiO 2 surfaces (Fig. 5), in agreement with the literature.…”

Section: Hard and Soft Hydration Layerssupporting

confidence: 90%

“…19 Considerable research efforts have been devoted to sorting out the molecular mechanisms behind water dissociation and diffusion on TiO 2 surfaces 20,21 and nanoparticles, 22,23 as well as adsorption of biological molecules on TiO 2 24-28 under ambient conditions. The TiO 2 water interface 29 can be probed with a range of experimental techniques. Important examples include determining the amount of surface OH groups with x-ray photoelectron spectroscopy (XPS), 30 measuring the water oxygen-to-surface bond length with xray photoelectron diffraction (XPD), 31 and/or imaging the interface with scanning tunneling microscopy (STM).…”

Section: Introductionmentioning

confidence: 99%

“…29 However, biological environments are usually fully hydrated. Experiments 32 and computations 49,50 have shown that the structure of the hydration layer changes as the water amount is increased beyond monolayer coverage, presumably because of hydrogen bonding between the first and second water layers.…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Diffusion and reaction pathways of water near fully hydrated TiO2 surfaces from ab initio molecular dynamics

Agosta

Brandt

Lyubartsev

2017

The Journal of Chemical Physics

104

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Ab initio molecular dynamics simulations are reported for water-embedded TiO2 surfaces to determine the diffusive and reactive behavior at full hydration. A three-domain model is developed for six surfaces [rutile (110), (100), and (001), and anatase (101), (100), and (001)] which describes waters as “hard” (irreversibly bound to the surface), “soft” (with reduced mobility but orientation freedom near the surface), or “bulk.” The model explains previous experimental data and provides a detailed picture of water diffusion near TiO2 surfaces. Water reactivity is analyzed with a graph-theoretic approach that reveals a number of reaction pathways on TiO2 which occur at full hydration, in addition to direct water splitting. Hydronium (H3O+) is identified to be a key intermediate state, which facilitates water dissociation by proton hopping between intact and dissociated waters near the surfaces. These discoveries significantly improve the understanding of nanoscale water dynamics and reactivity at TiO2 interfaces under ambient conditions.

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“…29 The present AIMD simulations predict three to four ordered water layers (L 1 to L 4 ) near the TiO 2 surfaces (Fig. 5), in agreement with the literature.…”

Section: Hard and Soft Hydration Layerssupporting

confidence: 90%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Diffusion and reaction pathways of water near fully hydrated TiO2 surfaces from ab initio molecular dynamics

Agosta

Brandt

Lyubartsev

2017

The Journal of Chemical Physics

104

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“…Hence, recent thermodynamical calculations suggested transition metal oxides as being universally unstable under OER conditions [87]. However, these calculations neither take into account specific interactions with water and counterions on the surface [88], nor reflect the orientation dependence for the stability of the oxides [89], as reported for SrRuO 3 perovskites for instance [86], which can largely modify the stability of transition metal oxides under OER conditions. Nevertheless, as a general trend, while triggering surface oxygen as an active site for OER might be seen as a blessing due to the enhanced OER kinetics, drastic instabilities must be anticipated.…”

Section: Low Temperature Oxygen Evolution Reactionmentioning

confidence: 98%

Factors Controlling the Redox Activity of Oxygen in Perovskites: From Theory to Application for Catalytic Reactions

Yang

Grimaud

2017

Catalysts

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Abstract:Triggering the redox reaction of oxygens has become essential for the development of (electro) catalytic properties of transition metal oxides, especially for perovskite materials that have been envisaged for a variety of applications such as the oxygen evolution or reduction reactions (OER and ORR, respectively), CO or hydrocarbons oxidation, NO reduction and others. While the formation of ligand hole for perovskites is well-known for solid state physicists and/or chemists and has been widely studied for the understanding of important electronic properties such as superconductivity, insulator-metal transitions, magnetoresistance, ferroelectrics, redox properties etc., oxygen electrocatalysis in aqueous media at low temperature barely scratches the surface of the concept of oxygen ions oxidation. In this review, we briefly explain the electronic structure of perovskite materials and go through a few important parameters such as the ionization potential, Madelung potential, and charge transfer energy that govern the oxidation of oxygen ions. We then describe the surface reactivity that can be induced by the redox activity of the oxygen network and the formation of highly reactive surface oxygen species before describing their participation in catalytic reactions and providing mechanistic insights and strategies for designing new (electro) catalysts. Finally, we give a brief overview of the different techniques that can be employed to detect the formation of such transient oxygen species.

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“…Water is an important component of atmospheric dispersoids such as fog, mist, dew, and rain. Atmospheric water not only retains pollutants via both adsorption and absorption, but also facilitates and participates in their transformation to other species [1] [2] [3] [4]. Specifically, the uptake of organic and inorganic gases leads to transformations in atmospheric water films that lead to more polar and less volatile compounds.…”

Section: Introductionmentioning

confidence: 99%

An Experimental Study of the Atmospheric Oxidation of a Biogenic Organic Compound (Methyl Jasmonate) in a Thin Water Film as in Fog or Aerosols

Heath¹,

Valsaraj²

2017

OJAP

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Experiments on the reactions of OH radicals in thin films of water were conducted in a photochemical reactor. The OH radical reactivity of a biogenic molecule (methyl jasmonate) was observed to be much larger in thin films of water than in the bulk aqueous phase. The pseudo-first order reaction rate was enhanced by an order of magnitude on a 38-micron film compared to the bulk liquid. However, the first order rate constant increased by 349%. This has implications in atmospheric systems like fog and mist which have large specific surface areas. The enhanced reactivity is attributable to both the partial solvation and faster diffusion at the air-water interface compared to the bulk liquid.

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Water at Interfaces

Cited by 647 publications

References 299 publications

Diffusion and reaction pathways of water near fully hydrated TiO2 surfaces from ab initio molecular dynamics

Diffusion and reaction pathways of water near fully hydrated TiO2 surfaces from ab initio molecular dynamics

Factors Controlling the Redox Activity of Oxygen in Perovskites: From Theory to Application for Catalytic Reactions

An Experimental Study of the Atmospheric Oxidation of a Biogenic Organic Compound (Methyl Jasmonate) in a Thin Water Film as in Fog or Aerosols

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