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Density functional theory studies of the adsorption of hydrogen sulfide on aluminum doped silicane

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Abstract

First principles total energy calculations have been performed to study the hydrogen sulfide (H2S) adsorption on silicane, an unusual one monolayer of Si(111) surface hydrogenated on both sides. The H2S adsorption may take place in dissociative or non-dissociative forms. Silicane has been considered as: (A) non-doped with a hydrogen vacancy, and doped in two main configurations; (B) with an aluminum replacing a hydrogen atom and (C-n; n = 1, 2, 3) with an aluminum replacing a silicon atom at a lattice site. In addition, three supercells; 4x4, 3x3 and 2x2 have been explored for both non-doped and doped silicane. The non-dissociative adsorption takes place in geometries (A), (C-1), (C-2) and (C-3) while the dissociative in (B). Adsorption energies of the dissociative case are larger than those corresponding to the non-dissociated cases. In the dissociative adsorption, the molecule is fragmented in a HS structure and a H atom which are bonded to the aluminum to form a H-S-Al-H structure. The presence of the doping produces some electronic changes as the periodicity varies. Calculations of the total density of states (DOS) indicate that in most cases the energy gap decreases as the periodicity changes from 4x4 to 2x2. The features of the total DOS are explained in terms of the partial DOS. The reported charge density plots explain quite well the chemisorptions and physisorptions of the molecule on silicane in agreement with adsorption energies.

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Acknowledgments

We wish to acknowledge the partial financial support of projects: Cuerpo Académico Física Computacional de la Materia Condensada (BUAP-CA-194) and VIEP-BUAP-EXC11-G. We are also grateful to the technical assistance of L. Rojas and N. Mendes at the computer center, in the Instituto de Física “Luis Rivera Terrazas” of the Universidad Autónoma de Puebla (IFUAP).

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Authors and Affiliations

  1. Instituto de Física “Ing. Luis Rivera Terrazas”, Benemérita Universidad Autónoma de Puebla, Puebla, Mexico

    Francisco Sánchez-Ochoa, Jonathan Guerrero-Sánchez & Gregorio H. Cocoletzi

  2. Centro de Investigación en Corrosión, Universidad Autónoma de Campeche, Campeche, Mexico

    Gabriel I. Canto

  3. Centro de Nanociencias y Nanotecnología, Universidad Nacional Autónoma de México, Mexico, Mexico

    Noboru Takeuchi

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  1. Francisco Sánchez-Ochoa
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  2. Jonathan Guerrero-Sánchez
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  3. Gabriel I. Canto
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  5. Noboru Takeuchi
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Correspondence to Francisco Sánchez-Ochoa.

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Sánchez-Ochoa, F., Guerrero-Sánchez, J., Canto, G.I. et al. Density functional theory studies of the adsorption of hydrogen sulfide on aluminum doped silicane. J Mol Model 19, 2925–2934 (2013). https://doi.org/10.1007/s00894-013-1873-1

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