MOLECULAR-BEAM STUDY OF DISSOCIATIVE STICKING OF METHANE ON NI(100)

被引:165
作者
HOLMBLAD, PM
WAMBACH, J
CHORKENDORFF, I
机构
[1] Physics Department, Technical University of Denmark
关键词
D O I
10.1063/1.468955
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
This paper reports a detailed molecular beam study of the dissociative sticking of methane incident on clean Ni(100). It is demonstrated that the sticking coefficient depends strongly on the translational energy of the molecule. It is also observed that an increase in the vibrational energy of the methane leads to a dramatic enhancement of the sticking, emphasizing that the initial vibrational state is of crucial importance. These results are consistent with a mechanism of direct activated dissociative chemisorption where the dynamics is dominated by a barrier in the potential energy surface mainly located in the vibrational coordinates. Normal-energy scaling is only approximately observed. The effect of surface temperature is also investigated but is found to be smaller than activation by translational or vibrational energy. A simplified analysis in terms of state resolved sticking curves, S v(Ei), considering only the vibrational C-H stretch modes of methane as relevant for the sticking, gives a good description of the data. These sticking curves enables a calculation of the thermal sticking coefficient which is found to be in excellent agreement with bulb experiments directly probing this. © 1995 American Institute of Physics.
引用
收藏
页码:8255 / 8263
页数:9
相关论文
共 24 条
[1]   STATISTICAL-MODELS FOR ENSEMBLE CONTROL BY ALLOYING AND POISONING OF CATALYSTS .2. COMPARISONS WITH MONTE-CARLO SIMULATIONS AND WITH EXPERIMENTAL RESULTS [J].
ALSTRUP, I ;
ANDERSEN, NT .
JOURNAL OF CATALYSIS, 1987, 104 (02) :466-479
[2]   STATISTICAL-MODELS FOR ENSEMBLE CONTROL BY ALLOYING AND POISONING OF CATALYSTS .1. MATHEMATICAL ASSUMPTIONS AND DERIVATIONS [J].
ANDERSEN, NT ;
TOPSOE, F ;
ALSTRUP, I ;
ROSTRUPNIELSEN, JR .
JOURNAL OF CATALYSIS, 1987, 104 (02) :454-465
[3]   KINETICS OF THE ACTIVATED DISSOCIATIVE ADSORPTION OF METHANE ON THE LOW INDEX PLANES OF NICKEL SINGLE-CRYSTAL SURFACES [J].
BEEBE, TP ;
GOODMAN, DW ;
KAY, BD ;
YATES, JT .
JOURNAL OF CHEMICAL PHYSICS, 1987, 87 (04) :2305-2315
[4]   THEORETICAL INVESTIGATION OF THE INSERTION OF NICKEL IN THE CH-BOND OF CH4 - ELECTRONIC-STRUCTURE CALCULATIONS AND DYNAMICS [J].
BURGHGRAEF, H ;
JANSEN, APJ ;
VANSANTEN, RA .
JOURNAL OF CHEMICAL PHYSICS, 1993, 98 (11) :8810-8818
[5]   METHANE ACTIVATION ON CLEAN AND OXIDIZED NI(100) [J].
CAMPBELL, RA ;
SZANYI, J ;
LENZ, P ;
GOODMAN, DW .
CATALYSIS LETTERS, 1993, 17 (1-2) :39-46
[6]   XPS STUDY OF CHEMISORPTION OF CH4 ON NI(100) [J].
CHORKENDORFF, I ;
ALSTRUP, I ;
ULLMANN, S .
SURFACE SCIENCE, 1990, 227 (03) :291-296
[7]   THE ROLE OF PARALLEL MOMENTUM IN THE DISSOCIATIVE ADSORPTION OF H-2 AT HIGHLY CORRUGATED SURFACES [J].
DARLING, GR ;
HOLLOWAY, S .
SURFACE SCIENCE, 1994, 304 (03) :L461-L467
[8]   THE ACTIVATION OF ALKANES ON NI(100) [J].
HAMZA, AV ;
MADIX, RJ .
SURFACE SCIENCE, 1987, 179 (01) :25-46
[9]  
HANLEY L, 1991, SURF SCI, V248, pL265
[10]   MOLECULAR-BEAM INVESTIGATION OF ADSORPTION KINETICS ON BULK METAL TARGETS - NITROGEN ON TUNGSTEN [J].
KING, DA ;
WELLS, MG .
SURFACE SCIENCE, 1972, 29 (02) :454-+