Theoretical and experimental studies of Ag-Pt interactions for supported Ag-Pt bimetallic catalysts

被引：40

作者：

Schaal, Melanie T. ^{[1
]}

Hyman, Matthew P. ^{[2
]}

Rangan, Meghana ^{[3
]}

Ma, Shuguo ^{[1
]}

Williams, Christopher T. ^{[1
]}

Monnier, John R. ^{[1
]}

Medlin, J. Will ^{[3
]}

机构：

[1] Univ S Carolina, Dept Chem Engn, Columbia, SC 29208 USA

[2] Univ Penn, Dept Chem & Biomol Engn, Philadelphia, PA 19104 USA

[3] Univ Colorado, Dept Chem & Biol Engn, Boulder, CO 80309 USA

来源：

SURFACE SCIENCE | 2009年 / 603卷 / 04期

基金：

美国国家科学基金会;

关键词：

X-ray photoelectron spectroscopy; Ab-initio quantum chemical methods and calculations; Silver; Platinum; Bimetallic surfaces; Electronic effect; Core level shifts; DENSITY-FUNCTIONAL THEORY; AB-INITIO CALCULATIONS; CHEMICAL-PROPERTIES; ELECTROLESS DEPOSITION; METAL-SURFACES; ADSORPTION; PT(111); CO; SPECTROSCOPY; TRANSITION;

D O I：

10.1016/j.susc.2009.01.011

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 electronic structure and chemical properties of catalysts prepared by the electroless deposition (ED) of Ag onto Pt/SiO2 were studied using a combination of X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations. XPS studies revealed a negative shift (up to -0.75 eV) in the Ag 3d binding energy (BE) relative to bulk Ag. Both the magnitude and direction of the shift are consistent with DFT calculations of model Ag/Pt(111) surfaces. DFT calculations have also been employed to study the adsorption of two probe molecules, carbon monoxide and 1-epoxy-3-butene (EpB), on the model surfaces. Combined with previously published reports, the results presented here suggest that (1) the AgPt/SiO2 catalysts that are most active for hydrogenation of the EpB olefin function consist of an adlayer of Ag on Pt rather than a surface or bulk alloy and that (2) the higher activity and selectivity of ED-prepared Ag-Pt/SiO2 catalysts for C=C hydrogenation of EpB to 1-epoxybutane are consistent with computed electronic (ligand) and bifunctional effects. (C) 2009 Elsevier B.V. All rights reserved.

引用

页码：690 / 696

页数：7

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