A unified study for water adsorption on metals: meaningful models from structural motifs

Revilla-López, Guillem; López, Núria

doi:10.1039/c4cp02508c

Cited by 17 publications

(25 citation statements)

References 35 publications

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“…Besides, the interface shows low ordering as five‐ and seven‐membered rings appear, in good agreement with experiments done at lower coverages . On Ru, half of the water molecules dissociate, and form a very rigid structure containing mostly hexagonal patters ,. However, there is no explicit pH variation at the interface as protons and hydroxyls are trapped on the surface .…”

Section: Introductionsupporting

confidence: 84%

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Developments in the Atomistic Modelling of Catalytic Processes for the Production of Platform Chemicals from Biomass

Garcı́a-Muelas

Rellán‐Piñeiro

et al. 2018

ChemCatChem

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The transformation of biomass‐derived molecules into platform chemicals that can directly be employed by the chemical industry is one of the challenges in catalysis in this century. While some processes are cost‐effective and industrially available, the molecular insight has been advancing at a slow pace when compared to other areas (like energy conversion). In the present review we describe the main challenges imposed on the theoretical simulations for the study of these complex molecules and how the most crucial issues are typically addressed. In particular, we focus on technical aspects like the need for London dispersion and solvation contributions. We also deal with the complexity of reaction networks, which requires new approaches and ways to compile the results in the form of databases. This allows the study of large reaction networks for the decomposition of C2 alcohols, or the plethora of functional groups of cyclic molecules such as lignin and sugars. Finally, we put forward a few applications that show the potential of atomistic simulations in the field.

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Section: Introductionsupporting

confidence: 84%

“…[98] On Ru, half of the water molecules dissociate, and form a very rigid structure containing mostly hexagonal patters. [99,100] However, there is no explicit pH variation at the interface as protons and hydroxyls are trapped on the surface. [96] On oxide surfaces the situation is more complex.…”

Section: Microkineticsmentioning

confidence: 99%

Developments in the Atomistic Modelling of Catalytic Processes for the Production of Platform Chemicals from Biomass

Garcı́a-Muelas

Rellán‐Piñeiro

et al. 2018

ChemCatChem

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“…29,30 Hybrid methods, where the microsolvation is complemented by an implicit solvent are particularly attractive in terms of computational efficiency, but consistent treatment of the explicit water molecules remains a significant challenge. 9,[31][32][33][34] Another approach is based on ice-like structures, [35][36][37][38][39] which are motivated by low-temperature surface science studies which have evidenced the existence of these arrangements over many transition metal surfaces. [40][41][42] However, these rigid networks are unlikely to be representative at ambient temperature and even less so at the elevated temperatures applied, for instance, in aqueousphase reforming.…”

Section: Introductionmentioning

confidence: 99%

Force Field for Water over Pt(111): Development, Assessment, and Comparison

Steinmann

Morais

Götz

et al. 2018

J. Chem. Theory Comput.

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Metal/water interfaces are key in many natural and industrial processes, such as corrosion, atmospheric, or environmental chemistry. Even today, the only practical approach to simulate large interfaces between a metal and water is to perform force-field simulations. In this work, we propose a novel force field, GAL17, to describe the interaction of water and a Pt(111) surface. GAL17 builds on three terms: (i) a standard Lennard-Jones potential for the bonding interaction between the surface and water, (ii) a Gaussian term to improve the surface corrugation, and (iii) two terms describing the angular dependence of the interaction energy. The 12 parameters of this force field are fitted against a set of 210 adsorption geometries of water on Pt(111). The performance of GAL17 is compared to several other approaches that have not been validated against extensive first-principles computations yet. Their respective accuracy is evaluated on an extended set of 802 adsorption geometries of HO on Pt(111), 52 geometries derived from icelike layers, and an MD simulation of an interface between a c(4 × 6) Pt(111) surface and a water layer of 14 Å thickness. The newly developed GAL17 force field provides a significant improvement over previously existing force fields for Pt(111)/HO interactions. Its well-balanced performance suggests that it is an ideal candidate to generate relevant geometries for the metal/water interface, paving the way to a representative sampling of the equilibrium distribution at the interface and to predict solvation free energies at the solid/liquid interface.

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“…2) is due to the formation of hydrogen bonds between HCHO and the surface hydroxyls [57]. The energy difference can be estimated to the formation of two hydrogen bonds [58]. On (110), A2 binding energy is higher than I2 because the hydroxylated surface presents intrasurface hydrogen bonds (between O lat -H and another O lat ) and formaldehyde adsorbs on the acceptor oxygen disrupting the H-bond surface network.…”

Section: Dehydrogenation Of Formaldehyde To Carbon Monoxide On Ceomentioning

confidence: 99%

Unraveling the structure sensitivity in methanol conversion on CeO2: A DFT+U study

Capdevila‐Cortada

García‐Melchor

López

2015

Journal of Catalysis

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108

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Highlights:-Structure sensitivity correlates with the surface oxygen content in the methanol decomposition on ceria.-Methanol selectively converts to formaldehyde on ceria (111) and (110) facets.-The CeO 2 (100) facet traps formaldehyde and ultimately enables its oxidation to produce CO+H 2 .-Hydrogen evolution is permitted on (100) due to its ability to stabilize a hydrogen precursor.-Formaldehyde can easily exchange its oxygen with the lattice in all facets. 2 ABSTRACTMethanol decomposes on oxides, in particular CeO 2 , producing either formaldehyde or CO as main products. This reaction presents structure sensitivity to the point that the major product obtained depends on the facet exposed in the ceria nanostructures. Our Density Functional Theory (DFT) calculations illustrate how the control of the surface facet and its inherent stoichiometry determine the sole formation of formaldehyde on the closed surfaces or the more degraded byproducts on the open facets (CO and hydrogen). In addition, we found that the regular (100) termination is the only one that allows hydrogen evolution via a hydride-hydroxyl precursor. The fundamental insights presented for the differential catalytic reactivity of the different facets agree with the structure sensitivity found for ceria catalysts in several reactions and provide a better understanding on the need of shape control in selective processes.3

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A unified study for water adsorption on metals: meaningful models from structural motifs

Cited by 17 publications

References 35 publications

Developments in the Atomistic Modelling of Catalytic Processes for the Production of Platform Chemicals from Biomass

Developments in the Atomistic Modelling of Catalytic Processes for the Production of Platform Chemicals from Biomass

Force Field for Water over Pt(111): Development, Assessment, and Comparison

Unraveling the structure sensitivity in methanol conversion on CeO2: A DFT+U study

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