Physisorption energy of successive layers of H2 molecules with a (100) surface of copper

Cilpa, Geraldine; Chambaud, Gilberte

doi:10.1016/j.susc.2006.09.044

Cited by 11 publications

(14 citation statements)

References 35 publications

(50 reference statements)

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“…A rigid unrelaxed cluster model, in which distances between Cu atoms are kept fixed at their solid-state values, has been chosen, since relaxation of such a system could induce spurious effects. This model is similar to the one used in a recent theoretical study [15] whose results are compared to the present ones.…”

Section: Computational Detailsmentioning

confidence: 58%

“…Moreover, we want to notice that it was not possible to compute energies with the same basis used for the MRCI calculations due to problems related to the errors of the numerical integration for the exchange-correlation contribution to the total energy. In addition, the basis set superposition error (BSSE) has not been evaluated in order to make our DFT calculations directly comparable to the MRCI calculations, carried out under similar conditions [15]. In the MRCI ?…”

Section: Computational Detailsmentioning

confidence: 99%

“…These steps are analyzed and discussed separately because they involve electronic effects of different nature. Interaction energies (E), dihydrogen bond lengths [d(H-H)], and distance from the cluster surface (Z) are displayed in Table 1 and compared to available data [7,15].…”

Section: First Layer Interactionmentioning

confidence: 99%

“…From the data given in Table 1 one can see that the MRCI calculations [15] including the Davidson correction (MRCI ? Q) are in excellent agreement with experimental results, and they concluded to the existence of a shallow physisorption minimum located far from the surface, at about 7.0 bohr.…”

Section: Physisorptionmentioning

confidence: 99%

“…Despite the large amount of theoretical works, some questions still remain, especially concerning the energetics of H 2 molecules interacting with a metallic surface already covered with a first layer of hydrogens. In a recent theoretical study on the H 2 /Cu system [15] using a cluster model consisting of 13 Cu atoms, it has been shown that the chemisorption and physisorption of the first H 2 layer and the van der Waals (vdW) interactions responsible for the physisorption of additional H 2 layers can be satisfactorily reproduced by highly correlated electronic wavefunctions. Unfortunately, such refined approaches cannot be easily used in large or extended (2D or 3D) systems and other possibilities must be explored.…”

Section: Introductionmentioning

confidence: 99%

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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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Section: Computational Detailsmentioning

confidence: 58%

Section: Computational Detailsmentioning

confidence: 99%

Section: First Layer Interactionmentioning

confidence: 99%

Section: Physisorptionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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

Cilpa¹,

Colin²,

Labat³

et al. 2012

Vincenzo Barone

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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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Catalytic and kinetic study of the liquid-phase hydrogenation of acetophenone over Cu/SiO2 catalyst

Bertero

Apesteguı́a

Marchi

2008

Applied Catalysis A: General

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Physisorption energy of successive layers of H2 molecules with a (100) surface of copper

Cited by 11 publications

References 35 publications

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

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

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

Catalytic and kinetic study of the liquid-phase hydrogenation of acetophenone over Cu/SiO2 catalyst

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