Oxidation of Small Silver Clusters: A Density Functional Theory Study

被引：55

作者：

Klacar, Simon ^{[1
,2
]}

Hellman, Anders ^{[1
,2
]}

Panas, Itai ^{[3
]}

Gronbeck, Henrik ^{[1
,2
]}

机构：

[1] Chalmers Univ Technol, Dept Appl Phys, SE-41296 Gothenburg, Sweden

[2] Chalmers Univ Technol, Competence Ctr Catalysis, SE-41296 Gothenburg, Sweden

[3] Chalmers Univ Technol, Dept Environm Inorgan Chem, SE-41296 Gothenburg, Sweden

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2010年 / 114卷 / 29期

基金：

瑞典研究理事会;

关键词：

SIMPLE METAL-CLUSTERS; MOLECULAR-OXYGEN; BINDING-ENERGY; ADSORPTION; NOX; CHEMISORPTION; HYDROGEN; AG; CO; REACTIVITY;

D O I：

10.1021/jp102715r

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The oxidation of small silver clusters (Ag-n, n <= 9) was investigated through electronic structure calculations based on density functional theory. The adsorption energies of molecular and dissociated adsorption show a pronounced odd/even alternation, with lower energies calculated for even-sized clusters. Molecular adsorption is favored for n <= 5, whereas dissociation is preferred for the larger sizes. Molecular oxygen is adsorbed in atop (Ag, Ag-2, Ag-6, Ag-8) or bridge (Ag-3, Ag-4, Ag-5, Ag-7, Ag-9) configurations, and atomic oxygen is preferably adsorbed in 3-fold hollow positions. Results for stoichiometric (Ag2nOn) clusters were compared to O-2 adsorption on Ag(111), and ab initio thermodynamics was used to estimate the temperature for the oxide-to-metal phase transition. The barrier for O-2 dissociation on Ag-8 was calculated to be higher than the corresponding barrier on Ag(111), which indicates a slower oxidation process. Adsorption of NOx onto the oxidized clusters was found to proceed through a formal reduction of the clusters; that is, NOx is adsorbed as NOx+1 with x = 1, 2.

引用

页码：12610 / 12617

页数：8

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