ISOLATING THE REACTION STEPS IN THE FORMATION OF METHOXY ON CU(100)

被引:24
作者
ELLIS, TH
WANG, H
机构
[1] Département de Chimie, Université de Montréal, Québec, H3C 3J7, C.P. 6128, Succ. centre-ville, Montréal
关键词
D O I
10.1021/la00023a030
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The adsorption and reaction of methanol on clean and oxygen-precovered Cu(100) has been studied using high-resolution electron energy loss spectroscopy (HREELS). On the clean Cu(100) surface, methanol is molecularly adsorbed and forms an ordered layer at around a monolayer coverage. Preadsorbed oxygen promotes the dissociation of methanol via a two-step process. The first reaction step (CH3OH2 + O-2 --> CH3Oa + OHa) occurs below 120 K. Most importantly, for the first time, a stable OH intermediate is directly observed by HREELS. Furthermore, OH subsequently reacts with excess methanol to form gaseous H2O and additional methoxy at 180 K (the second reaction step CH3OHa + OHa --> CH3Oa + H2Og). We have also studied the reaction between methanol and a preadsorbed OH layer on Cu(100), in order to confirm this reaction process occurring at 180 K. These results show that the activation barrier for the second reaction is higher than that of the first reaction on Cu(100).
引用
收藏
页码:4083 / 4088
页数:6
相关论文
共 25 条
[1]   A STATIC SIMS TPD STUDY OF THE KINETICS OF METHOXY FORMATION AND DECOMPOSITION ON O/PT(111) [J].
AKHTER, S ;
WHITE, JM .
SURFACE SCIENCE, 1986, 167 (01) :101-126
[2]   THE EFFECTS OF PREADSORBED OXYGEN ON THE ADSORPTION AND DECOMPOSITION OF METHANOL ON NI(110) [J].
BARE, SR ;
STROSCIO, JA ;
HO, W .
SURFACE SCIENCE, 1985, 155 (2-3) :L281-L291
[3]   WATER-ADSORPTION ON CU(100) - THE EFFECT OF DEFECTS [J].
BROSSEAU, R ;
BRUSTEIN, MR ;
ELLIS, TH .
SURFACE SCIENCE, 1993, 294 (03) :243-250
[4]   THE ADSORPTION AND REACTION OF METHANOL ON OXIDIZED COPPER(111) STUDIED BY FOURIER-TRANSFORM REFLECTION ABSORPTION INFRARED-SPECTROSCOPY [J].
CHESTERS, MA ;
MCCASH, EM .
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY, 1987, 43 (12) :1625-1630
[5]   THE ADSORPTION AND REACTION OF METHANOL ON PD(100) .1. CHEMISORPTION AND CONDENSATION [J].
CHRISTMANN, K ;
DEMUTH, JE .
JOURNAL OF CHEMICAL PHYSICS, 1982, 76 (12) :6308-6317
[6]   FLUORINE SUBSTITUENT EFFECTS ON ALKOXIDE CHEMISTRY AND ORIENTATION ON THE CU(100) SURFACE [J].
DAI, Q ;
GELLMAN, AJ .
JOURNAL OF PHYSICAL CHEMISTRY, 1993, 97 (41) :10783-10789
[7]   A HREELS STUDY OF C1-C5 STRAIGHT CHAIN ALCOHOLS ON CLEAN AND PRE-OXIDIZED AG(110) SURFACES [J].
DAI, Q ;
GELLMAN, AJ .
SURFACE SCIENCE, 1991, 257 (1-3) :103-112
[8]  
Davis R., 1992, CATALYSIS SURFACE CH, P213
[9]   ADSORPTION AND REACTION OF WATER ON OXYGEN PRECOVERED CU(100) [J].
ELLIS, TH ;
KRUUS, EJ ;
WANG, H .
JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A-VACUUM SURFACES AND FILMS, 1993, 11 (04) :2117-2121
[10]   INFRARED SPECTRA OF METHANOL AND DEUTERATED METHANOLS IN GAS, LIQUID, AND SOLID PHASES [J].
FALK, M ;
WHALLEY, E .
JOURNAL OF CHEMICAL PHYSICS, 1961, 34 (05) :1554-&