Methanol adsorption on Pd(110) and Ag/Pd(110) studied by high-resolution photoelectron spectroscopy

被引:3
作者
Ramachandran, A. [1 ]
Borck, O. [1 ]
Andersen, T. H. [1 ]
Svenum, I. -H. [1 ]
Walle, L. E. [1 ]
Borg, A. [1 ]
机构
[1] Norwegian Univ Sci & Technol, Dept Phys, NO-7491 Trondheim, Norway
关键词
Methanol; Adsorption; Palladium; Ag-Pd alloy; CO; High-resolution photoelectron spectroscopy; Density functional theory; ENERGY-LOSS SPECTROSCOPY; SINGLE-CRYSTAL SURFACES; THERMAL-DESORPTION SPECTROSCOPY; SUPPORTED PALLADIUM CATALYSTS; CORE-LEVEL PHOTOEMISSION; HYDROGEN CARRIER SYSTEM; PARTIAL OXIDATION; ELECTRONIC-STRUCTURE; POWER APPLICATIONS; XPS SPECTROSCOPY;
D O I
10.1016/j.susc.2009.10.015
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
Adsorption of methanol on clean Pd(1 1 0) and on an alloyed Ag/Pd(1 1 0) surface has been studied by high-resolution photoelectron spectroscopy. On Pd(1 1 0) two different chemisorbed methanol species were observed for temperatures up to 200 K, with the one at lower binding energy remaining at low coverage. These species were attributed to methanol adsorbed in two different adsorption sites on the Pd(1 1 0) surface. As is well established for this system, heating to 250 K resulted in decomposition of methanol into CO. The adsorption and decomposition behaviour of methanol on the Ag/Pd(1 1 0) surface alloy formed by depositing Ag on Pd(1 1 0) at elevated temperature was similar to that of the pure Pd(1 1 0) surface. This suggests that the amount of Ag present in the Pd(1 1 0) surface in this study does not affect the decomposition behaviour of methanol as compared to pure Pd(1 1 0). Complementary density functional theory calculations also show little influence of Ag on the binding of methanol to Pd. These calculations predict an on-top adsorption site for low methanol coverages. (C) 2009 Elsevier B.V. All rights reserved.
引用
收藏
页码:89 / 97
页数:9
相关论文
共 85 条
[1]   Valence-band hybridization and core level shifts in random Ag-Pd alloys [J].
Abrikosov, IA ;
Olovsson, W ;
Johansson, B .
PHYSICAL REVIEW LETTERS, 2001, 87 (17) :176403-176403
[2]   Production of hydrogen by partial oxidation of methanol over ZnO-supported palladium catalysts prepared by microemulsion technique [J].
Agrell, J ;
Germani, G ;
Järås, SG ;
Boutonnet, M .
APPLIED CATALYSIS A-GENERAL, 2003, 242 (02) :233-245
[3]   Partial oxidation of methanol to produce hydrogen over Cu-Zn-based catalysts [J].
Alejo, L ;
Lago, R ;
Pena, MA ;
Fierro, JLG .
APPLIED CATALYSIS A-GENERAL, 1997, 162 (1-2) :281-297
[4]   Alcohol dehydrogenation over Pd versus PdAg membranes [J].
Amandusson, H ;
Ekedahl, LG ;
Dannetun, H .
APPLIED CATALYSIS A-GENERAL, 2001, 217 (1-2) :157-164
[5]   SURFACE CORE-LEVEL SHIFTS OF SOME 4D-METAL SINGLE-CRYSTAL SURFACES - EXPERIMENTS AND AB-INITIO CALCULATIONS [J].
ANDERSEN, JN ;
HENNIG, D ;
LUNDGREN, E ;
METHFESSEL, M ;
NYHOLM, R ;
SCHEFFLER, M .
PHYSICAL REVIEW B, 1994, 50 (23) :17525-17533
[6]   An overview of platinum-based catalysts as methanol-resistant oxygen reduction materials for direct methanol fuel cells [J].
Antolini, E. ;
Lopes, T. ;
Gonzalez, E. R. .
JOURNAL OF ALLOYS AND COMPOUNDS, 2008, 461 (1-2) :253-262
[7]   Valence band studies of Ag and Pd codeposited on Ru(0001) [J].
Bech, L. ;
Li, Z. ;
Onsgaard, J. .
JOURNAL OF ELECTRON SPECTROSCOPY AND RELATED PHENOMENA, 2007, 156 :102-106
[8]   ADSORPTION OF CO ON PD(100) [J].
BEHM, RJ ;
CHRISTMANN, K ;
ERTL, G ;
VANHOVE, MA .
JOURNAL OF CHEMICAL PHYSICS, 1980, 73 (06) :2984-2995
[9]   Dipole correction for surface supercell calculations [J].
Bengtsson, L .
PHYSICAL REVIEW B, 1999, 59 (19) :12301-12304
[10]   THE DECOMPOSITION OF METHANOL ON PD(110) AS STUDIED BY ELECTRON-ENERGY LOSS SPECTROSCOPY - EVIDENCE FOR THE FORMATION OF CH3O AND HCO SURFACE SPECIES [J].
BHATTACHARYA, AK ;
CHESTERS, MA ;
PEMBLE, ME ;
SHEPPARD, N .
SURFACE SCIENCE, 1988, 206 (1-2) :L845-L850