Low translational energy mechanisms in the dissociative chemisorption of methane on iridium and platinum surfaces

被引:21
作者
Reeves, CT [1 ]
Seets, DC [1 ]
Mullins, CB [1 ]
机构
[1] Univ Texas, Dept Chem Engn, Austin, TX 78712 USA
关键词
methane; iridium; platinum; molecular beam; single crystal;
D O I
10.1016/S1381-1169(00)00508-2
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
Recent molecular beam studies of methane dissociative chemisorption on Ir(1 1 0), Ir(1 1 1) and Pt(1 1 0) surfaces show evidence of a low translational energy pathway to dissociation that had not been seen previously for methane dissociation on any transition metal surface. Earlier molecular beam studies on a variety of transition metal surfaces indicated only a direct dissociative mechanism for methane dissociation, which is active only at high translational energies. Recent studies on Ir and Pt show that at low translational energies the dissociative chemisorption probability decreases as the translational energy increases in contrast to the behavior at higher translational energies, where the direct mechanism is known to be dominant and the chemisorption probability increases with increasing translational energy. The exact mechanism of this low energy pathway is under debate and has been described as either a trapping-mediated mechanism or a steering-assisted direct mechanism. (C) 2001 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:207 / 215
页数:9
相关论文
共 76 条
[1]  
ANGER G, 1989, SURF SCI, V219, pL583, DOI 10.1016/0039-6028(89)90504-9
[2]   DYNAMICS OF MOLECULAR CH4 ADSORPTION ON PT(111) [J].
ARUMAINAYAGAM, CR ;
MCMASTER, MC ;
SCHOOFS, GR ;
MADIX, RJ .
SURFACE SCIENCE, 1989, 222 (01) :213-246
[3]   SUBPICOSECOND TRANSIENT INFRARED-SPECTROSCOPY OF ADSORBATES - VIBRATIONAL DYNAMICS OF CO/PT(111) [J].
BECKERLE, JD ;
CAVANAGH, RR ;
CASASSA, MP ;
HEILWEIL, EJ ;
STEPHENSON, JC .
JOURNAL OF CHEMICAL PHYSICS, 1991, 95 (07) :5403-5418
[4]   COLLISION-INDUCED DESORPTION OF PHYSISORBED CH4 FROM NI(111) - EXPERIMENTS AND SIMULATIONS [J].
BECKERLE, JD ;
JOHNSON, AD ;
CEYER, ST .
JOURNAL OF CHEMICAL PHYSICS, 1990, 93 (06) :4047-4065
[5]   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
[6]   ADSORPTION OF HYDROGEN ON TUNGSTEN - A PRECURSOR PATH PLUS DIRECT ADSORPTION [J].
BERGER, HF ;
RESCH, C ;
GROSSLINGER, E ;
EILMSTEINER, G ;
WINKLER, A ;
RENDULIC, KD .
SURFACE SCIENCE, 1992, 275 (1-2) :L627-L630
[7]   PRECURSOR DYNAMICS IN DISSOCIATIVE HYDROGEN ADSORPTION ON W(100) [J].
BUTLER, DA ;
HAYDEN, BE ;
JONES, JD .
CHEMICAL PHYSICS LETTERS, 1994, 217 (04) :423-429
[8]   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
[9]   SURFACE INFRARED-SPECTROSCOPY [J].
CHABAL, YJ .
SURFACE SCIENCE REPORTS, 1988, 8 (5-7) :211-357
[10]   THE KINETICS OF H-2 DISSOCIATIVE CHEMISORPTION - THE ROLE OF TRANSIENTS [J].
CHAKRAVARTY, C ;
METIU, H .
JOURNAL OF CHEMICAL PHYSICS, 1995, 102 (21) :8643-8655