Environment-driven reactivity of H2 on PdRu surface alloys

被引：16

作者：

Ramos, M. ^{[1
,2
]}

Minniti, M. ^{[3
,4
]}

Diaz, C. ^{[5
]}

Farias, D. ^{[3
,4
]}

Miranda, R. ^{[3
,4
,6
]}

Martin, F. ^{[5
,6
]}

Martinez, A. E. ^{[1
,2
]}

Busnengo, H. F. ^{[1
,2
]}

机构：

[1] Inst Fis Rosario, Grp Fis Quim Interfases & Nanoestruct, RA-2000 Rosario, Santa Fe, Argentina

[2] Univ Nacl Rosario, RA-2000 Rosario, Santa Fe, Argentina

[3] Univ Autonoma Madrid, Dept Fis Mat Condensada, E-28049 Madrid, Spain

[4] Univ Autonoma Madrid, Inst Nicolas Cabrera, E-28049 Madrid, Spain

[5] Univ Autonoma Madrid, Dept Quim, E-28049 Madrid, Spain

[6] Inst Madrileno Estudios Avanzados Nanociencia IMD, Madrid 28049, Spain

来源：

PHYSICAL CHEMISTRY CHEMICAL PHYSICS | 2013年 / 15卷 / 36期

关键词：

TOTAL-ENERGY CALCULATIONS; BIMETALLIC SURFACES; DISSOCIATION; ADSORPTION; MONOLAYER; DYNAMICS; DIFFRACTION;

D O I：

10.1039/c3cp52001c

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 dissociative adsorption of molecular hydrogen on PdxRu(1-x)/Ru(0001) (0 <= x <= 1) has been investigated by means of He atom scattering, Density Functional Theory and quasi-classical trajectory calculations. Regardless of their surroundings, Pd atoms in the alloy are always less reactive than Ru ones. However, the reactivity of Ru atoms is enhanced by the presence of nearest neighbor Pd atoms. This environment-dependent reactivity of the Ru atoms in the alloy provides a sound explanation for the striking step-like dependence of the initial reactive sticking probability as a function of the Pd concentration observed in experiments. Moreover, we show that these environment-dependent effects on the reactivity of H-2 on single atoms allow one to get around the usual constraint imposed by the Bronsted-Evans-Polanyi relationship between the reaction barrier and chemisorption energy.

引用

页码：14936 / 14940

页数：5

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