Effect of the surface model on the theoretical description of the chemisorption of atomic hydrogen on Cu()

Domı́nguez-Ariza, David; Sousa, Carmen; Harrison, N. M.; Ganduglia‐Pirovano, M. V.; Illas, Francesc

doi:10.1016/s0039-6028(02)02347-6

Cited by 26 publications

(18 citation statements)

References 39 publications

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“…These results confirm once more that a given cluster model differently describes different metal surfaces [57]. Later on, it will be shown that the electric field required to induce the ET is proportional to the metal surface U and consequently high Us require lower electric fields.…”

Section: Electron Transfer Related Properties Of the Isolated Systemssupporting

confidence: 73%

Requirements for the generalization of the ab initio two-state model for external electric field induced electron transfer at electrodes

Migani¹,

Illas²

2007

Journal of Electroanalytical Chemistry

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Section: Electron Transfer Related Properties Of the Isolated Systemssupporting

confidence: 73%

Requirements for the generalization of the ab initio two-state model for external electric field induced electron transfer at electrodes

Migani¹,

Illas²

2007

Journal of Electroanalytical Chemistry

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“…Calculations for bulk Cu were conducted with 408 special k points and a cutoff energy of 30 Ry. The total energy convergence with respect to the cutoff energy (25)(26)(27)(28)(29)(30)(31)(32)(33)(34)(35)(36)(37)(38)(39)(40) and the number of the k points (220-570) was within a few tenths of 1 meV per atom. We obtained lattice constants of 3.64Å for bulk Cu, in good agreement with the experimental value of 3.61Å.…”

Section: Resultsmentioning

confidence: 96%

First-principles calculations for the adsorption of water molecules on theCu(100)surface

2004

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First-principles density-functional theory and supercell models are employed to calculate the adsorption of water molecules on the Cu(100) surface. In agreement with the experimental observations, the calculations show that a H2O molecule prefers to bond at a one-fold on-top (T1) surface site with a tilted geometry. At low temperatures, rotational diffusion of the molecular axis of the water molecules around the surface normal is predicted to occur at much higher rates than lateral diffusion of the molecules. In addition, the calculated binding energy of an adsorbed water molecule on the surfaces is significantly smaller than the water sublimation energy, indicating a tendency for the formation of water clusters on the Cu(100) surface.

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“…Alternative studies have also been performed, modeling the surface by a cluster. In such cases, the size of the cluster plays a relevant role since it influences the reactivity of the metal toward H 2 , as demonstrated by Raghavan et al [10] in the case of D 2 /Ni, and also the quality of the results [11]. Moreover, it has been shown that, in the case of Cu, 3D metallic clusters [7] with more than 6 atoms can satisfactorily reproduce the experimental interatomic distances [12].…”

Section: Introductionmentioning

confidence: 89%

Adsorption of successive layers of H2 molecules on a model copper surface: performances of second- to fifth-rung exchange-correlation functionals

et al. 2012

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The interaction of H 2 molecules with a Cu(100) metallic surface has been investigated by DFT approaches using a (H 2 ) n Cu 13 cluster model. Nine exchange-correlation functionals, belonging to the generalized gradient approximations (GGA), meta GGA (mGGA), hybrid Kohn-Sham/Hartree-Fock models, either based on GGAs or mGGAs, range-separated hybrids, and double-hybrid families, have been tested on the chemisorption and physisorption processes involving one or two H 2 layers. The addition of an empirical correction for dispersion has also been tested for some of these functionals. The calculated energies and structural parameters were compared to sophisticated multi reference configuration interaction including Davidson's correction for quadruple excitations (MRCI ? Q). Our results show that among the nine considered exchange-correlation functionals, none can accurately reproduce all processes involved in the successive layers adsorption. Although an hybrid based on a mGGA such as M06-2X can quantitatively describe both the physisorption step and dissociation barriers involved in the adsorption of the first H 2 , it fails to reproduce its chemisorption. On the other hand, significant discrepancies with the reference post-HF data are obtained for the description of the second layer interaction, no matter which functional is considered, outlining the need of improvement and/or development of exchange-correlation functionals suitable for complex systems such as H 2 /H 2 Cu.

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Effect of the surface model on the theoretical description of the chemisorption of atomic hydrogen on Cu()

Cited by 26 publications

References 39 publications

Requirements for the generalization of the ab initio two-state model for external electric field induced electron transfer at electrodes

Requirements for the generalization of the ab initio two-state model for external electric field induced electron transfer at electrodes

First-principles calculations for the adsorption of water molecules on theCu(100)surface

Adsorption of successive layers of H2 molecules on a model copper surface: performances of second- to fifth-rung exchange-correlation functionals

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