Poisoning of hydrogen dissociation at Pd (100) by adsorbed sulfur studied by ab-initio quantum dynamics and ab-initio molecular dynamics

被引：43

作者：

Gross, A

Wei, CM

Scheffler, M

机构：

[1] Acad Sinica, Inst Phys, Taipei 11529, Taiwan

[2] Max Planck Gesell, Fritz Haber Inst, D-14195 Berlin, Germany

来源：

SURFACE SCIENCE | 1998年 / 416卷 / 1-2期

关键词：

chemisorption; density functional calculations; hydrogen; models of surface chemical reactions; molecular dynamics; molecule-solid reactions; palladium; quantum effects; sulfur;

D O I：

10.1016/S0039-6028(98)00649-9

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：

We report calculations of the dissociative adsorption of H-2 at Pd (100) covered with 1/4 monolayer of sulfur using quantum dynamics as well as molecular dynamics and taking all six degrees of freedom of the two H atoms fully into account. The ab-initio potential-energy surface (PES) is found to be very strongly corrugated. In particular, we discuss the influence of tunneling, zero-point vibrations due to the localization of the wave function of the nuclei when narrow valleys of the PES are passed, steering of the approaching H-2 molecules towards low-energy barrier configurations, and the important role of subsurface absorbates for the hydrogen dissociation. It is shown that "established" concepts derived from low-dimensional dynamical studies are not necessarily valid in a high-dimensional treatment. (C) 1998 Elsevier Science B.V. All rights reserved.

引用

页码：L1095 / L1100

页数：6

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