An infrared spectroscopic study of the hydrogenation and dehydrogenation of the complexes of aromatic compounds and of fullerene C60 with silica-supported platinum

被引:7
作者
Davydov, VY [1 ]
Sheppard, N
Osawa, E
机构
[1] Moscow MV Lomonosov State Univ, Dept Chem, Moscow 119899, Russia
[2] Univ E Anglia, Sch Chem Sci, Norwich NR4 7TJ, Norfolk, England
[3] Toyohashi Univ Technol, Kept Knowledge Based Informat Engn, Toyohashi, Aichi 4418580, Japan
关键词
fullerene C-60; aromatic hydrocarbons; catalytic hydrogenation and dehydrogenation; complexes with Pt; infrared spectroscopy;
D O I
10.1006/jcat.2002.3694
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
An infrared spectroscopic study has been made of the surface complexes from the chemisorption of the aromatic compounds benzene, toluene, para-xylene (1,4-dimethylbenzene), mesitylene (1,3,5-trimethylbenzene), naphthalene, and anthracene, and also of fullerene C-60, on silica-supported platinum catalysts, and of their subsequent hydrogenation and dehydrogenation reactions. The complexes of the initial adsorbates with platinum can be hydrogenated under relatively low pressures of hydrogen (<1 atm) and then dehydrogenated to considerable degrees by evacuation even at ambient temperatures. In the case of benzene the hydrogenated cyclohexane-like complex gives very extensive reversion to adsorbed benzene on evacuation. The surface complexes gradually diminish in amount during successive cycles of hydrogenation and dehydrogenation, with the generation of gas-phase cyclohexane. For the other compounds, except for C-60, the hydrogenation is also virtually (or actually) complete but the dehydrogenation is only partial and the surface complexes remain present during multiple cycles of hydrogenation and dehydrogenation. The room temperature spectra from the methyl-substituted benzenes under vacuum support chemisorption via methyl-group dissociation. For naphthalene and anthracene the spectra of stable partially dehydrogenated species are consistent with the rearomatization of only one end ring. For fullerene C-60 the spectrum of the hydrogenated species suggests that a five-membered ring is in selective contact with the surface but that some adjacent six-membered rings are also hydrogenated. The hydrogenation and dehydrogenation processes are both slow but the rates, together with the extent of hydrogenation, increase with temperature. The hydrogenated spectra of the fullerene-based complex differ from those reported earlier for C60H18 and C60H36. (C) 2002 Elsevier Science (USA).
引用
收藏
页码:42 / 52
页数:11
相关论文
共 51 条
[1]   ADSORPTION STATES OF BENZENE AND TOLUENE ON PT(111) - A VIBRATIONAL EELS, DELTA-PHI, AES AND TDS STUDY [J].
ABON, M ;
BERTOLINI, JC ;
BILLY, J ;
MASSARDIER, J ;
TARDY, B .
SURFACE SCIENCE, 1985, 162 (1-3) :395-401
[2]   THE USE OF THERMAL-DESORPTION AND ELECTRON-ENERGY LOSS SPECTROSCOPY FOR THE DETERMINATION OF THE STRUCTURES OF UNSATURATED-HYDROCARBONS CHEMISORBED ON METAL SINGLE-CRYSTAL SURFACES .1. ALK-1-ENES ON PT(111) [J].
AVERY, NR ;
SHEPPARD, N .
PROCEEDINGS OF THE ROYAL SOCIETY OF LONDON SERIES A-MATHEMATICAL PHYSICAL AND ENGINEERING SCIENCES, 1986, 405 (1828) :1-25
[4]   HYDROGENATION OF BUCKMINSTERFULLERENE C-60 VIA HYDROZIRCONATION - A NEW WAY TO ORGANOFULLERENES [J].
BALLENWEG, S ;
GLEITER, R ;
KRATSCHMER, W .
TETRAHEDRON LETTERS, 1993, 34 (23) :3737-3740
[5]   BIRCH REDUCTION OF C(60) - A NEW APPRAISAL [J].
BANKS, MR ;
DALE, MJ ;
GOSNEY, I ;
HODGSON, PKG ;
JENNINGS, RCK ;
JONES, AC ;
LECOULTRE, J ;
LANGRIDGESMITH, PRR ;
MAIER, JP ;
SCRIVENS, JH ;
SMITH, MJC ;
SMYTH, CJ ;
TAYLOR, AT ;
THORBURN, P ;
WEBSTER, AS .
JOURNAL OF THE CHEMICAL SOCIETY-CHEMICAL COMMUNICATIONS, 1993, (14) :1149-1152
[6]   Solubility of C-60 [J].
Beck, MT ;
Mandi, G .
FULLERENE SCIENCE AND TECHNOLOGY, 1997, 5 (02) :291-310
[7]  
Bellamy L. J., 1975, INFRARED SPECTRA COM, V1
[8]   A BPTDS AND HREELS STUDY OF THE INTERACTION OF CYCLOHEXANE WITH THE PT(111) SURFACE [J].
BUSSELL, ME ;
HENN, FC ;
CAMPBELL, CT .
JOURNAL OF PHYSICAL CHEMISTRY, 1992, 96 (14) :5978-5982
[9]   THE INFRARED-SPECTRUM OF CYCLOHEXANE ADSORBED ON PT(111) [J].
CHESTERS, MA ;
GARDNER, P .
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY, 1990, 46 (06) :1011-1015
[10]  
Choi HC, 1996, J CATAL, V161, P790