Mechanism of selective alcohol oxidation to aldehydes on gold catalysts: Influence of surface roughness on reactivity

被引：110

作者：

Boronat, Mercedes ^{[1
]}

Corma, Avelino ^{[1
]}

Illas, Francesc ^{[2
,3
]}

Radilla, Juan ^{[2
,3
,4
]}

Rodenas, Tania ^{[1
]}

Sabater, Maria J. ^{[1
]}

机构：

[1] Univ Politecn Valencia, Inst Tecnol Quim, CSIC, Valencia 46022, Spain

[2] Univ Barcelona, Dept Quim Fis, E-08028 Barcelona, Spain

[3] Univ Barcelona, Inst Quim Teor & Computac IQTCUB, E-08028 Barcelona, Spain

[4] Univ Autonoma Metropolitana Azcapotzalco, Dept Ciencias Basicas, Area Quim, Mexico City 02200, DF, Mexico

来源：

JOURNAL OF CATALYSIS | 2011年 / 278卷 / 01期

关键词：

Catalysis; Au; DFT; Alcohol oxidation; Selectivity; ACTIVE HETEROGENEOUS CATALYST; TOTAL-ENERGY CALCULATIONS; AEROBIC OXIDATION; DIMER METHOD; NANOPARTICLES; PALLADIUM; PHASE; ACID; DEHYDROGENATION; NANOCLUSTERS;

D O I：

10.1016/j.jcat.2010.11.013

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 complete reaction pathway for the selective alcohol oxidation to aldehyde has been obtained from periodic density functional theory (DFT) calculations on a series of catalyst models having Au atoms with different coordination number. A clear trend exists in the reactivity of the surfaces: it increases with decreasing the Au coordination number, suggesting that a distribution of Au sites with different activity might exist on the surface of real catalysts. This hypothesis emerging from the theoretical study has been experimentally confirmed by measuring the kinetics of benzyl alcohol oxidation on a series of Au/MgO catalysts having different particle diameter and therefore different concentration and distribution of low coordinated Au sites. (C) 2010 Elsevier Inc. All rights reserved.

引用

页码：50 / 58

页数：9

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