Adsorption and decomposition of acetylene on planar and faceted Ir(210)

被引:25
作者
Chen, WH
Ermanoski, I
Wu, QF
Madey, TE
Hwu, HH
Chen, JGG
机构
[1] Rutgers State Univ, Dept Phys & Astron, Piscataway, NJ 08854 USA
[2] Rutgers State Univ, Dept Chem, Piscataway, NJ 08854 USA
[3] Rutgers State Univ, Surface Modificat Lab, Piscataway, NJ 08854 USA
[4] Univ Delaware, Dept Mat Sci & Engn, CCST, Newark, DE 19716 USA
关键词
acetylene; benzene; iridium; surface reaction;
D O I
10.1021/jp0224721
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 adsorption and reaction of acetylene on both planar and faceted Ir(210) have been studied utilizing temperature-programmed desorption TPD), Auger electron spectroscopy (AES), low-energy electron diffraction (LEED), and high-resolution electron energy loss spectroscopy (HREELS). Following adsorption of C2H2 at 300 K or 100 K, TPD data indicate that H-2 is the dominant desorption product, and that decomposition of adsorbed C2H2 occurs in a stepwise fashion. Multiple carbon-containing species are formed on Ir(210) upon adsorption of acetylene at high coverage, which are different from those formed at low coverage. Our HREELS results show that the dominant surface hydrocarbon species formed at high coverage are mainly acetylide and ethylidyne while acetylide dominates at low coverage. In contrast to reaction measurements on an Ir organometallic complex that catalyzes cyclization of C2H2 to C6H6, no evidence for the cyclization reaction is found on Ir(210). The results are compared with adsorption and decomposition of C6H6 on Ir(210); as for C2H2, the dominant desorption product is H2, but there are differences in the reaction sequence. In addition, evidence has been found in TPD measurements for structure sensitivity in decomposition of acetylene over the clean faceted Ir(210) surface versus the clean planar Ir(210) surface, which is attributed to nanometer scale structures on the faceted surface. The HREELS data give complementary information to TPD and AES results and provide insights into the reaction mechanisms for acetylene surface chemistry.
引用
收藏
页码:5231 / 5242
页数:12
相关论文
共 67 条
[41]   COADSORPTION OF CARBON-MONOXIDE AND HYDROGEN ON IRIDIUM SINGLE-CRYSTALS [J].
MARINOVA, TS ;
CHAKAROV, DV .
SURFACE SCIENCE, 1989, 217 (1-2) :65-77
[42]   Atomic structures on faceted W(111) surfaces induced by ultrathin films of Pd [J].
Nien, CH ;
Madey, TE .
SURFACE SCIENCE, 1997, 380 (2-3) :L527-L532
[43]   Coexistence of {011} facets with {112} facets on W(111) induced by ultrathin films of Pd [J].
Nien, CH ;
Madey, TE ;
Tai, YW ;
Leung, TC ;
Che, JG ;
Chan, CT .
PHYSICAL REVIEW B, 1999, 59 (15) :10335-10340
[44]   ADSORPTION OF CARBON-MONOXIDE, OXYGEN, HYDROGEN, NITROGEN, ETHYLENE AND BENZENE ON AN IRIDIUM (110) SURFACE - CORRELATION WITH OTHER IRIDIUM CRYSTAL FACES [J].
NIEUWENHUYS, BE ;
SOMORJAI, GA .
SURFACE SCIENCE, 1978, 72 (01) :8-32
[45]   LEED, AES AND THERMAL DESORPTION STUDIES OF CHEMISORBED HYDROGEN AND HYDROCARBONS (C2H2,C2H4,C6H6,C6H12) ON (111) AND STEPPED [6(111)X(100)] IRIDIUM CRYSTAL-SURFACES - COMPARISON WITH PLATINUM [J].
NIEUWENHUYS, BE ;
HAGEN, DI ;
ROVIDA, G ;
SOMORJAI, GA .
SURFACE SCIENCE, 1976, 59 (01) :155-176
[46]  
NOZOYE H, 1992, SURF SCI, V269, P335
[47]   Thermal conversion of chemisorbed acetylene to vinylidene and hydrogenation to ethylidyne on Rh{111}: A laser induced desorption study [J].
Papageorgopoulos, DC ;
Ge, Q ;
Nimmo, S ;
King, DA .
JOURNAL OF PHYSICAL CHEMISTRY B, 1997, 101 (11) :1999-2005
[48]   MOLECULAR PATHWAYS IN THE CYCLOTRIMERIZATION OF ETHYNE ON PALLADIUM - ROLE OF THE C-4 INTERMEDIATE [J].
PATTERSON, CH ;
LAMBERT, RM .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1988, 110 (20) :6871-6877
[49]   MOLECULAR MECHANISMS IN THE CYCLOTRIMERIZATION OF ACETYLENE TO BENZENE ON PALLADIUM(111) [J].
PATTERSON, CH ;
LAMBERT, RM .
JOURNAL OF PHYSICAL CHEMISTRY, 1988, 92 (05) :1266-1270
[50]   Structural changes of the W(211) surface induced by ultrathin films of Ph, Pt, and Pd [J].
Pelhos, K ;
Abdelrehim, IM ;
Nien, CH ;
Madey, TE .
JOURNAL OF PHYSICAL CHEMISTRY B, 2001, 105 (18) :3708-3717