Adsorption and decomposition of H2S on Pd(111) surface:: a first-principles study

被引：92

作者：

Alfonso, DR

Cugini, AV

Sorescu, DC

机构：

[1] US DOE, Natl Energy Technol Lab, Pittsburgh, PA 15236 USA

[2] Parsons Project Serv Inc, South Pk, PA 15129 USA

来源：

CATALYSIS TODAY | 2005年 / 99卷 / 3-4期

关键词：

density functional calculations; dissociative adsorption; chemisorption; palladium; hydrogen sulfide; sulfuhydryl species (SH); sulfur; metallic surface; low index single crystal surface; GENERALIZED GRADIENT APPROXIMATION; ENERGY ELECTRON-DIFFRACTION; DENSITY-FUNCTIONAL THEORY; HYDROGEN DESORPTION; ADSORBATE STRUCTURE; SULFUR; PALLADIUM; PD; METALS; PSEUDOPOTENTIALS;

D O I：

10.1016/j.cattod.2004.10.006

中图分类号：

O69 [应用化学];

学科分类号：

081704 ;

摘要：

Gradient-corrected density functional theory was used to investigate the adsorption of H2S on Pd(1 1 1) surface. Molecular adsorption was found to be stable with H2S binding preferentially at top sites. In addition, the adsorption of other S moieties (SH and S) was investigated. SH and S were found to be preferentially bind at the bridge and fcc sites, respectively. The reaction pathways and energy profiles for H2S decomposition giving rise to adsorbed S and H were determined. Both H2S(ad) -> SH(ad) + H-(ad) and SH(ad) -> S-(ad) + H-(ad) reactions were found to have low barriers and high exothermicities. This reveals that the decomposition of H2S on Pd(1 1 1) surface is a facile process. (c) 2004 Elsevier B.V. All rights reserved.

引用

页码：315 / 322

页数：8

共 39 条

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