C-O bond scission on "defect-rich and perfect" Pd(111)?

被引:45
作者
Kaichev, VV
Morkel, M
Unterhalt, H
Prosvirin, IP
Bukhtiyarov, VI
Rupprechter, G
Freund, HJ
机构
[1] Max Planck Gesell, Fritz Haber Inst, D-14195 Berlin, Germany
[2] Boreskov Inst Catalysis, Novosibirsk 630090, Russia
关键词
carbon monoxide; alcohols; palladium; sum frequency generation; X-ray photoelectron spectroscopy; catalysis; low index single crystal surfaces;
D O I
10.1016/j.susc.2004.06.100
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
To investigate the influence of surface defects on CO adsorption and dissociation, well-annealed and "defect-rich" Pd(111) were examined by sum frequency generation (SFG) and X-ray photoelectron spectroscopy (XPS) within the pressure range 10(-6)-1 mbar. Ar+ ion sputtering was employed to produce surface defects which exhibited vibrational and photoemission characteristics different from the regular adsorption sites on Pd(111). Even under high-pressure, SFG and XPS indicated that no CO dissociation occurred on both surfaces at 300-400 K. By contrast, C-O bond scission was observed during methanol decomposition producing carbonaceous deposits beside CO and H-2. A possible relationship between the adsorption geometry and C-O bond scission is discussed. (C) 2004 Elsevier B.V. All rights reserved.
引用
收藏
页码:1024 / 1029
页数:6
相关论文
共 29 条
[21]   ANGLE-RESOLVED PHOTOEMISSION AS A TOOL FOR THE STUDY OF SURFACES [J].
PLUMMER, EW ;
EBERHARDT, W .
ADVANCES IN CHEMICAL PHYSICS, 1982, 49 :533-656
[22]   Sum frequency generation vibrational spectroscopy at solid-gas interfaces: CO adsorption on Pd model catalysts at ambient pressure [J].
Rupprechter, G ;
Unterhalt, H ;
Morkel, M ;
Galletto, P ;
Hu, LJ ;
Freund, HJ .
SURFACE SCIENCE, 2002, 502 :109-122
[23]   Surface vibrational spectroscopy from ultrahigh vacuum to atmospheric pressure: adsorption and reactions on single crystals and nanoparticle model catalysts monitored by sum frequency generation spectroscopy [J].
Rupprechter, G .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2001, 3 (21) :4621-4632
[24]   The molecular origins of selectivity in methanol decomposition on Pd nanoparticles [J].
Schauermann, S ;
Hoffmann, J ;
Johánek, V ;
Hartmann, J ;
Libuda, J ;
Freund, HJ .
CATALYSIS LETTERS, 2002, 84 (3-4) :209-217
[25]   Adsorption and desorption of methanol on Pd (111) and on a Pd/V surface alloy [J].
Schennach, R ;
Eichler, A ;
Rendulic, KD .
JOURNAL OF PHYSICAL CHEMISTRY B, 2003, 107 (11) :2552-2558
[26]   CO CHEMISORPTION ON CR(110) - EVIDENCE FOR A PRECURSOR TO DISSOCIATION [J].
SHINN, ND ;
MADEY, TE .
JOURNAL OF CHEMICAL PHYSICS, 1985, 83 (11) :5928-5944
[27]   CO adsorption on Pd(111): a high-resolution core level photoemission and electron energy loss spectroscopy study [J].
Surnev, S ;
Sock, M ;
Ramsey, MG ;
Netzer, FP ;
Wiklund, M ;
Borg, M ;
Andersen, JN .
SURFACE SCIENCE, 2000, 470 (1-2) :171-185
[28]   Vibrational sum frequency spectroscopy on Pd(111) and supported Pd nanoparticles: CO adsorption from ultrahigh vacuum to atmospheric pressure [J].
Unterhalt, H ;
Rupprechter, G ;
Freund, HJ .
JOURNAL OF PHYSICAL CHEMISTRY B, 2002, 106 (02) :356-367
[29]   OPTICAL PARAMETRIC GENERATION AND AMPLIFICATION IN BARIUM BORATE AND LITHIUM TRIBORATE CRYSTALS [J].
ZHANG, JY ;
HUANG, JY ;
SHEN, YR ;
CHEN, C .
JOURNAL OF THE OPTICAL SOCIETY OF AMERICA B-OPTICAL PHYSICS, 1993, 10 (09) :1758-1764