CO adsorption on graphite-like ZnO bilayers supported on Cu(111), Ag(111) and Au(111) surfaces

2017 ◽  
Author(s):  
Sergio Tosoni ◽  
Cequn Li ◽  
Philomena Schlexer ◽  
Gianfranco Pacchioni
Keyword(s):  
Density Functional ◽  
Chemical Interaction ◽  
Co Adsorption ◽  
Density Functional Theory Calculations ◽  
Dispersion Interactions ◽  
Oxide Interface ◽  
Functional Theory ◽  
Bilayer Films ◽  
Coinage Metals ◽  
Co Probe

<div> <div> <div> <p>Graphitic-like ZnO bilayer films deposited on coinage metals, Cu(111), Ag(111), and Au(111) have been studied by density functional theory calculations including dispersion corrections. The scope is to compare on an equal footing the properties of the three systems and in particular the nature of the metal/oxide interface. To this end we have considered the adsorption of a CO probe molecule and the vibrational shifts induced by adsorption on ZnO/Cu(111), ZnO/Ag(111), and ZnO/Au(111) compared to adsorption on the unsupported ZnO bilayer and on the wurtzite ZnO surface. We find that while the interaction of ZnO with Ag and Au supports is dominated by dispersion interactions with little or no charge transfer at the interface, in the case of Cu a moderate electron transfer occurs towards the ZnO bilayer. As a consequence, while the stretching frequency of CO on ZnO/Au is blue-shifted, that on ZnO/Cu is red- shifted compared to free CO. CO on ZnO/Ag is intermediate. In all three cases, however, the ZnO bilayer is almost flat, with a modest rumpling found in the case of Cu as a consequence of the stronger chemical interaction. The results fully explain the CO vibrational shifts of CO on ZnO/Cu(111) [Schott, V. et al. Angew. Chem. Int. Ed. 2013, 52, 1-6] without implying major distortions in the supported film. </p> </div> </div> </div>

CO adsorption on graphite-like ZnO bilayers supported on Cu(111), Ag(111) and Au(111) surfaces

2017 ◽  
Author(s):  
Sergio Tosoni ◽  
Cequn Li ◽  
Philomena Schlexer ◽  
Gianfranco Pacchioni
Keyword(s):  
Density Functional ◽  
Chemical Interaction ◽  
Co Adsorption ◽  
Density Functional Theory Calculations ◽  
Dispersion Interactions ◽  
Oxide Interface ◽  
Functional Theory ◽  
Bilayer Films ◽  
Coinage Metals ◽  
Co Probe

<div> <div> <div> <p>Graphitic-like ZnO bilayer films deposited on coinage metals, Cu(111), Ag(111), and Au(111) have been studied by density functional theory calculations including dispersion corrections. The scope is to compare on an equal footing the properties of the three systems and in particular the nature of the metal/oxide interface. To this end we have considered the adsorption of a CO probe molecule and the vibrational shifts induced by adsorption on ZnO/Cu(111), ZnO/Ag(111), and ZnO/Au(111) compared to adsorption on the unsupported ZnO bilayer and on the wurtzite ZnO surface. We find that while the interaction of ZnO with Ag and Au supports is dominated by dispersion interactions with little or no charge transfer at the interface, in the case of Cu a moderate electron transfer occurs towards the ZnO bilayer. As a consequence, while the stretching frequency of CO on ZnO/Au is blue-shifted, that on ZnO/Cu is red- shifted compared to free CO. CO on ZnO/Ag is intermediate. In all three cases, however, the ZnO bilayer is almost flat, with a modest rumpling found in the case of Cu as a consequence of the stronger chemical interaction. The results fully explain the CO vibrational shifts of CO on ZnO/Cu(111) [Schott, V. et al. Angew. Chem. Int. Ed. 2013, 52, 1-6] without implying major distortions in the supported film. </p> </div> </div> </div>

scholarly journals Including dispersion interactions in the ONETEP program for linear-scaling density functional theory calculations

2008 ◽  
Vol 465 (2103) ◽  
pp. 669-683 ◽  
Author(s):  
Quintin Hill ◽  
Chris-Kriton Skylaris
Keyword(s):  
Density Functional Theory ◽  
Density Functional ◽  
Computational Cost ◽  
Density Functional Theory Calculations ◽  
Binding Energies ◽  
Molecular Structures ◽  
Dispersion Interactions ◽  
Biomolecular Systems ◽  
Functional Theory ◽  
High Level

While density functional theory (DFT) allows accurate quantum mechanical simulations from first principles in molecules and solids, commonly used exchange-correlation density functionals provide a very incomplete description of dispersion interactions. One way to include such interactions is to augment the DFT energy expression by damped London energy expressions. Several variants of this have been developed for this task, which we discuss and compare in this paper. We have implemented these schemes in the ONETEP program, which is capable of DFT calculations with computational cost that increases linearly with the number of atoms. We have optimized all the parameters involved in our implementation of the dispersion correction, with the aim of simulating biomolecular systems. Our tests show that in cases where dispersion interactions are important this approach produces binding energies and molecular structures of a quality comparable with high-level wavefunction-based approaches.

scholarly journals Surface and shape modification of mackinawite (FeS) nanocrystals by cysteine adsorption: a first-principles DFT-D2 study

2016 ◽  
Vol 18 (47) ◽  
pp. 32007-32020 ◽  
Author(s):  
N. Y. Dzade ◽  
A. Roldan ◽  
N. H. de Leeuw
Keyword(s):  
Density Functional Theory ◽  
Amino Acid ◽  
First Principles ◽  
Density Functional ◽  
Density Functional Theory Calculations ◽  
Dispersion Interactions ◽  
Shape Modification ◽  
Functional Theory ◽  
Shape Modulation

The surface and shape modulation of mackinawite (FeS) nanoparticles by amino acid cysteine adsorption is investigated using a first-principles density functional theory calculations, corrected for dispersion-interactions (DFT-D2).

scholarly journals Theoretical Study of CO Adsorption and Activation on Orthorhombic Fe7C3(001) Surfaces for Fischer–Tropsch Synthesis Using Density Functional Theory Calculations

Energies ◽  
2021 ◽  
Vol 14 (3) ◽  
pp. 563
Author(s):  
Hee-Joon Chun ◽  
Yong Tae Kim
Keyword(s):  
Density Functional Theory ◽  
Density Functional ◽  
Co Adsorption ◽  
Density Functional Theory Calculations ◽  
Tropsch Synthesis ◽  
Fischer Tropsch ◽  
Functional Theory ◽  
Fischer Tropsch Synthesis ◽  
Co Dissociation ◽  
Co Activation

Fischer–Tropsch synthesis (FTS), which converts CO and H2 into useful hydrocarbon products, has attracted considerable attention as an efficient method to replace crude oil resources. Fe-based catalysts are mainly used in industrial FTS, and Fe7C3 is a common carbide phase in the FTS reaction. However, the intrinsic catalytic properties of Fe7C3 are theoretically unknown. Therefore, as a first attempt to understand the FTS reaction on Fe7C3, direct CO* dissociation on orthorhombic Fe7C3(001) (o-Fe7C3(001)) surfaces was studied using density functional theory (DFT) calculations. The surface energies of 14 terminations of o-Fe7C3(001) were first compared, and the results showed that (001)0.20 was the most thermodynamically stable termination. Furthermore, to understand the effect of the surface C atom coverage on CO* activation, C–O bond dissociation was performed on the o-Fe7C3(001)0.85, (001)0.13, (001)0.20, (001)0.09, and (001)0.99 surfaces, where the surface C atom coverages were 0.00, 0.17, 0.33, 0.33, and 0.60, respectively. The results showed that the CO* activation linearly decreased as the surface C atom coverage increased. Therefore, it can be concluded that the thermodynamic and kinetic selectivity toward direct CO* dissociation increased when the o-Fe7C3(001) surface had more C* vacancies.

scholarly journals A dimer path for CO dissociation on PtSn

2019 ◽  
Vol 9 (3) ◽  
pp. 695-701 ◽  
Author(s):  
Matthias Vandichel ◽  
Henrik Grönbeck
Keyword(s):  
Density Functional Theory ◽  
Density Functional ◽  
Co Adsorption ◽  
Density Functional Theory Calculations ◽  
Functional Theory ◽  
Co Dissociation

Density functional theory calculations are used to investigate CO adsorption, dissociation and SnOX formation on Pt3Sn.

Understanding the atomic-level process of CO-adsorption-driven surface segregation of Pd in (AuPd)147 bimetallic nanoparticles

Nanoscale ◽  
2017 ◽  
Vol 9 (33) ◽  
pp. 12077-12086 ◽  
Author(s):  
Hyesung An ◽  
Hyunwoo Ha ◽  
Mi Yoo ◽  
Hyun You Kim
Keyword(s):  
Density Functional Theory ◽  
Density Functional ◽  
Surface Segregation ◽  
Bimetallic Nanoparticles ◽  
Co Adsorption ◽  
Density Functional Theory Calculations ◽  
Atomic Level ◽  
Functional Theory ◽  
Level Process

The atomic-level process of CO-induced surface segregation of Pd in Au–Pd bimetallic nanoparticles is studied through density functional theory calculations.

Formation of Al/CuO bilayer films: Basic mechanisms through density functional theory calculations

2012 ◽  
Vol 520 (14) ◽  
pp. 4768-4771 ◽  
Author(s):  
Cloé Lanthony ◽  
Jean-Marie Ducéré ◽  
Alain Estève ◽  
Carole Rossi ◽  
Mehdi Djafari-Rouhani
Keyword(s):  
Density Functional Theory ◽  
Density Functional ◽  
Density Functional Theory Calculations ◽  
Functional Theory ◽  
Bilayer Films

scholarly journals Assessing the performance of density functional theory in optimizing molecular crystal structure parameters

2014 ◽  
Vol 70 (2) ◽  
pp. 259-267 ◽  
Author(s):  
Jack Binns ◽  
Mary R. Healy ◽  
Simon Parsons ◽  
Carole A. Morrison
Keyword(s):  
Density Functional Theory ◽  
Molecular Crystal ◽  
Density Functional ◽  
Crystal Packing ◽  
Structural Information ◽  
Density Functional Theory Calculations ◽  
Unit Cell ◽  
Dispersion Interactions ◽  
Functional Theory ◽  
Structural Database

This paper assesses the performance of plane-wave density functional theory calculations at returning reliable structural information for molecular crystal structures where the primary intermolecular interactions are either hydrogen bonding or dispersion interactions. The computed structures are compared with input structures obtained from the Cambridge Structural Database, and assessed in terms of crystal packing similarities, unit-cell volume and shape, short contact distances and hydrogen-bond distances. The results demonstrate that the PBE functional [Perdew, Burke & Ernzerhof (1996).Phys. Rev. Lett.77, 3865–3868] with Tkatchenko and Scheffler's `TS' dispersion correction [Tkatchenko & Scheffler (2009).Phys. Rev. Lett.102, 073005] is capable of returning reliable full structural optimizations, in which both atomic positions and unit-cell vectors are free to optimize simultaneously.

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