Study of structure-function relationships in platinum-silica catalysts using hydrocarbon hydrogenation as a probe reaction

被引:3
作者
Dias, E
Davies, AT
Mantle, MD
Roy, D
Gladden, LF
机构
[1] Univ Cambridge, Dept Chem Engn, Cambridge CB2 3RA, England
[2] Univ Cambridge, Dept Mat Sci & Met, Cambridge CB2 3RA, England
基金
英国工程与自然科学研究理事会;
关键词
silica-supported catalysts; NMR; Raman; porous media; selectivity; materials;
D O I
10.1016/S0009-2509(02)00587-0
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
In the field of heterogeneous catalysis, the relationship between catalyst synthesis and hence structure, and the resulting catalyst activity and selectivity are not well understood. The focus of this work has been to study the structural and catalytic characteristics of eight silica-supported platinum catalysts containing 0.5 wt% platinum. In particular, we wish to identify the specific characteristics of these materials which determine their. catalytic behaviour. A further aim is to relate these material properties to the method of catalyst synthesis used. This paper highlights the application of 29 Si nuclear magnetic resonance (NMR) and Raman spectroscopies to the characterisation of the hydroxyl and,siloxane ring structure environments on the silica surface. We then investigate how these structures are influenced by catalyst synthesis and the role, if any, they play in the activity and selectivity characteristics of the resulting catalysts. Reactor data are reported for ethene and ethyne hydrogenation reactions. The results suggest that while catalytic activity is determined by metal surface area, which is controlled by the method of metal deposition, for both the ethene and ethyne hydrogenations, the selectivity of the ethyne hydrogenation to ethane production appears to correlate with the structure of the silica surface. (C) 2003 Elsevier Science Ltd. All rights reserved.
引用
收藏
页码:621 / 626
页数:6
相关论文
共 8 条
[1]   SURFACE-STRUCTURE AND CHEMISTRY OF HIGH SURFACE-AREA SILICA-GELS [J].
BRINKER, CJ ;
BROW, RK ;
TALLANT, DR ;
KIRKPATRICK, RJ .
JOURNAL OF NON-CRYSTALLINE SOLIDS, 1990, 120 (1-3) :26-33
[2]   NMR CONFIRMATION OF STRAINED DEFECTS IN AMORPHOUS SILICA [J].
BRINKER, CJ ;
KIRKPATRICK, RJ ;
TALLANT, DR ;
BUNKER, BC ;
MONTEZ, B .
JOURNAL OF NON-CRYSTALLINE SOLIDS, 1988, 99 (2-3) :418-428
[3]   Ab initio calculations of 29Si solid state NMR chemical shifts of silane and silanol groups in silica [J].
Casanovas, J ;
Illas, F ;
Pacchioni, G .
CHEMICAL PHYSICS LETTERS, 2000, 326 (5-6) :523-529
[4]  
CHIARANUSSATI P, 1993, CHEM ENG RES DES, V71, P267
[5]   A detailed model of local structure and silanol hydrogen banding of silica gel surfaces [J].
Chuang, IS ;
Maciel, GE .
JOURNAL OF PHYSICAL CHEMISTRY B, 1997, 101 (16) :3052-3064
[6]   PLANAR RINGS INVITREOUS SILICA [J].
GALEENER, FL .
JOURNAL OF NON-CRYSTALLINE SOLIDS, 1982, 49 (1-3) :53-62
[7]   The fumed silica surface: A study by NMR [J].
Liu, CHC ;
Maciel, GE .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1996, 118 (21) :5103-5119
[8]   HIGH-RESOLUTION NA-23, AL-27, AND SI-29 NMR-SPECTROSCOPY OF FRAMEWORK ALUMINOSILICATE GLASSES [J].
OESTRIKE, R ;
YANG, WH ;
KIRKPATRICK, RJ ;
HERVIG, RL ;
NAVROTSKY, A ;
MONTEZ, B .
GEOCHIMICA ET COSMOCHIMICA ACTA, 1987, 51 (08) :2199-2209