PT PARTICLES FROM THE PT15(CO)302- CLUSTER COMPOUND

被引:18
作者
HANDY, BE [1 ]
DUMESIC, JA [1 ]
LANGER, SH [1 ]
机构
[1] UNIV WISCONSIN,DEPT CHEM ENGN,MADISON,WI 53706
关键词
D O I
10.1016/0021-9517(90)90047-N
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
Highly dispersed platinum particles were prepared by the pyrolysis of Pt15(CO)302- on hydroxylated and dehydroxylated, high surface area γ-Al2O3 Metal carbonyl decomposition was monitored by infrared spectroscopy, transmission electron microscopy, and hydrogen and carbon monoxide chemisorption experiments. The catalytic properties of these materials were examined for isomerization and hydrogenolysis of neopentane at 523-623 K and 1 atm pressure. The metal carbonyl cluster is weakly adsorbed on initial contact with the alumina surface showing CO stretching bands characteristic of the original cluster molecule. After several days of contact, or upon heating, the cluster rearranges to a more bulk-like platinum form. The original cluster compound cannot subsequently be regenerated with exposure to CO or mild reduction treatment. Metal particles originating from the Pt15 cluster are highly dispersed. Preliminary neopentane reaction studies show high selectivity for hydrogenolysis, following treatment in hydrogen at 620 K, consistent with the selectivity of highly dispersed platinum catalysts. Following reduction at 1070 K, the selectivity shifted to favor isomerization. Since electron microscopy results indicated minor particle sintering, the selectivity change may be attributed to surface annealing of the defect crystallite structures from the initial cluster at the higher reduction temperature. © 1990.
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页码:73 / 86
页数:14
相关论文
共 26 条
[1]   PREPARATION OF SOME SUPPORTED METALLIC CATALYSTS FROM METALLIC CLUSTER CARBONYLS [J].
ANDERSON, JR ;
ELMES, PS ;
HOWE, RF ;
MAINWARING, DE .
JOURNAL OF CATALYSIS, 1977, 50 (03) :508-518
[2]   USE OF A BIMETALLIC MOLECULAR CLUSTER COMPOUND FOR PREPARATION OF A DISPERSED BIMETALLIC CATALYST - METHYLCYCLOPENTANE HYDROGENOLYSIS [J].
ANDERSON, JR ;
MAINWARI.DE .
JOURNAL OF CATALYSIS, 1974, 35 (01) :162-165
[3]   ORGANOMETALLIC COMPLEXES ON ALUMINA [J].
BURWELL, RL .
JOURNAL OF CATALYSIS, 1984, 86 (02) :301-314
[4]   SYNTHESIS AND STRUCTURAL CHARACTERIZATION OF PLATINUM CARBONYL CLUSTER DIANIONS, [PT3(CO)3(MU2-CO)3]N2-(N=2,3,4,5) - NEW SERIES OF INORGANIC OLIGOMERS [J].
CALABRESE, JC ;
DAHL, LF ;
CHINI, P ;
LONGONI, G ;
MARTINENGO, S .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1974, 96 (08) :2614-2616
[5]   LARGE METAL-CARBONYL CLUSTERS (LMCC) [J].
CHINI, P .
JOURNAL OF ORGANOMETALLIC CHEMISTRY, 1980, 200 (01) :37-61
[6]   THE GENERATION OF BRONSTED AND LEWIS ACID SITES ON THE SURFACE OF SILICA BY ADDITION OF DOPANT CATIONS [J].
CONNELL, G ;
DUMESIC, JA .
JOURNAL OF CATALYSIS, 1987, 105 (02) :285-298
[7]   ISOMERIZATION OF C-13 LABELED HEXANES ON PT-AL2O3 AND ON ORGANOMETALLIC CLUSTER DERIVED CATALYSTS - EFFECT OF THE METAL-PARTICLE SIZE [J].
GARIN, F ;
ZAHRAA, O ;
CROUZET, C ;
SCHMITT, JL ;
MAIRE, G .
SURFACE SCIENCE, 1981, 106 (1-3) :466-471
[8]   DIRECT EVIDENCE FOR BIMETALLIC CLUSTERS [J].
GARTEN, RL .
JOURNAL OF CATALYSIS, 1976, 43 (1-3) :18-33
[9]  
GATES BC, 1980, CHEMTECH, V10, P248
[10]   INFRARED-SPECTRA OF CARBON-MONOXIDE CHEMISORBED ON SUPPORTED PLATINUM AGGREGATES PREPARED FROM PT CARBONYL CLUSTER COMPOUNDS [J].
ICHIKAWA, M .
CHEMISTRY LETTERS, 1976, (04) :335-338