TDS study of the bonding of CO and NO to vacuum-cleaved NiO(100)

Wichtendahl, Ralph; Rodriguez-Rodrigo, M.; Härtel, U.; Kuhlenbeck, Helmut; Freund, Hans‐Joachim

doi:10.1016/s0039-6028(98)00915-7

Cited by 123 publications

(92 citation statements)

References 14 publications

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“…[33] Recent experimental studies result in a desorption enthalpy of 3.2 kcal mol À1 . [33,57] Dispersion has a crucial contribution of 50 % or more to the interaction energy. [29,30] A correct description of such a weak interaction is still a challenge for DFT.…”

Section: Adsorption Of Carbon Monoxide On Magnesium Oxidementioning

confidence: 99%

System‐Dependent Dispersion Coefficients for the DFT‐D3 Treatment of Adsorption Processes on Ionic Surfaces

et al. 2011

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Dispersion-corrected density functional theory calculations (DFT-D3) were performed for the adsorption of CO on MgO and C(2) H(2) on NaCl surfaces. An extension of our non-empirical scheme for the computation of atom-in-molecules dispersion coefficients is proposed. It is based on electrostatically embedded M(4)X(4) (M=Na, Mg) clusters that are used in TDDFT calculations of dynamic dipole polarizabilities. We find that the C(MM)(6) dispersion coefficients for bulk NaCl and MgO are reduced by factors of about 100 and 35 for Na and Mg, respectively, compared to the values of the free atoms. These are used in periodic DFT calculations with the revPBE semi-local density functional. As demonstrated by calculations of adsorption potential energy curves, the new C(6) coefficients lead to much more accurate energies (E(ads)) and molecule-surface distances than with previous DFT-D schemes. For NaCl/C(2) H(2) we obtained at the revPBE-D3(BJ) level a value of E(ads) =-7.4 kcal mol(-1) in good agreement with experimental data (-5.7 to -7.1 kcal mol(-1)). Dispersion-uncorrected DFT yields an unbound surface state. For the MgO/CO system, the computed revPBE-D3(BJ) value of E(ads) =-4.1 kcal mol(-1) is also in reasonable agreement with experimental results (-3.0 kcal mol(-1)) when thermal corrections are taken into account. Our new dispersion correction also improves computed lattice constants of the bulk systems significantly compared to plain DFT or previous DFT-D results. The extended DFT-D3 scheme also provides accurate non-covalent interactions for ionic systems without empirical adjustments and is suggested as a general tool in surface science.

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Section: Adsorption Of Carbon Monoxide On Magnesium Oxidementioning

confidence: 99%

System‐Dependent Dispersion Coefficients for the DFT‐D3 Treatment of Adsorption Processes on Ionic Surfaces

et al. 2011

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“…In fact, the presence of appreciable concentrations of defects can completely change the chemical behavior of the MgO surface. For instance, while a single crystal, nearly defect-free, (100) MgO surface is totally inert towards carbon monoxide, [12] the surface of a polycrystalline MgO sample reacts at low temperature with the same molecule, with formation of complex carbonate species. [13] Among all the defects identified at the surface of MgO, (see Table 1), the oxygen vacancy is one of the most important and is supposed to be the prevalent defect in many oxides.…”

Section: Defects In Bulk Materialsmentioning

confidence: 99%

Oxygen Vacancy: The Invisible Agent on Oxide Surfaces

Pacchioni¹

2003

ChemPhysChem

463

340

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“…Adsorption on defect-free oxides is generally weak given the high degree of bond saturation at their surface and the large gap, in particular, that governs their electronic structure [14,15,24,26,31,38,44,45,[52][53][54]58]. Metal atoms deposited onto pristine oxides have essentially two means to interact with the surface [58].…”

Section: Introductionmentioning

confidence: 99%

Oxygen activation on oxide surfaces: A perspective at the atomic level

Freund

2014

Catalysis Today

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a b s t r a c tThin oxide films have been used as model supports to unravel the influence of the oxide-metal and oxide-gas interface. We discuss the influence of defects in the oxide lattice and the oxide surface on properties of adsorbed species, in particular the formation of oxide particles from a deposited transition metal onto ceria and of adsorbed oxygen from the gas phase. Here we correlate the structure of the particles, as revealed by a combination of STM and spectroscopic as well as theoretical calculations, with their reactive properties. The nature of the involved defects is characterized by adsorption of Au as a way to correlate the influence of various defects of different structure on the Au charge state. In a second case study, we demonstrate the influence of dopants within the supporting oxide on the adsorption of oxygen on a defect free surface. This is shown to be potentially relevant for the activation of methane in oxidative methane coupling reactions, as recently demonstrated.

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TDS study of the bonding of CO and NO to vacuum-cleaved NiO(100)

Cited by 123 publications

References 14 publications

System‐Dependent Dispersion Coefficients for the DFT‐D3 Treatment of Adsorption Processes on Ionic Surfaces

System‐Dependent Dispersion Coefficients for the DFT‐D3 Treatment of Adsorption Processes on Ionic Surfaces

Oxygen Vacancy: The Invisible Agent on Oxide Surfaces

Oxygen activation on oxide surfaces: A perspective at the atomic level

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