Study of textural properties and nucleation phenomenon in Pd/SiO2, Ag/SiO2 and Cu/SiO2 cogelled xerogel catalysts

被引:31
作者
Lambert, S [1 ]
Alie, C [1 ]
Pirard, JP [1 ]
Heinrichs, B [1 ]
机构
[1] Univ Liege, Lab Genie Chim, B-4000 Cointe Ougree, Belgium
关键词
D O I
10.1016/j.jnoncrysol.2004.06.005
中图分类号
TQ174 [陶瓷工业]; TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
Pd/SiO2, Ag/SiO2 and CU/SiO2 xerogel catalysts have been synthesized by cogelation of tetraethoxysilane (TEOS) and chelates of Pd, Ag and Cu with 3-(2-aminoethylamino)propyltrimethoxysilane (EDAS). The resulting materials are composed of completely accessible metallic crystallites with a diameter of about 3 nm, located inside silica particles exhibiting a monodisperse microporous distribution centered on a pore width of about 0.8 nm. Voids between silica particles and between aggregates of silica particles constitute the material meso- and macroporous texture. The EDAS/TEOS ratio is the main operating variable to tailor the material morphology. When the EDAS/TEOS ratio decreases, metallic particle size decreases, whereas silica particle size increases. Thus the meso- and macropores between silica particles are larger. So the total pore volume can reach 5 cm(3)/g when the EDAS/TEOS ratio decreases. The remarkable morphology of these materials can be explained by the rule in which the EDAS metal complex acts as a nucleation agent in the formation of silica particles. A nucleation mechanism by EDAS-metal complex based on mass equations and the nuclei formation kinetics allows fitting the entire results. (C) 2004 Elsevier B.V. All rights reserved.
引用
收藏
页码:70 / 81
页数:12
相关论文
共 22 条
[1]   Preparation of low-density xerogels from mixtures of TEOS with substituted alkoxysilanes.: I.: 17O NMR study of the hydrolysis-condensation process [J].
Alié, C ;
Pirard, JP .
JOURNAL OF NON-CRYSTALLINE SOLIDS, 2003, 320 (1-3) :21-30
[2]   Preparation of low-density xerogels from mixtures of TEOS with substituted alkoxysilanes.: II.: Viscosity study of the sol-gel transition [J].
Alié, C ;
Pirard, R ;
Pirard, JP .
JOURNAL OF NON-CRYSTALLINE SOLIDS, 2003, 320 (1-3) :31-39
[3]   The use of additives to prepare low-density xerogels [J].
Alié, C ;
Pirard, R ;
Lecloux, AJ ;
Pirard, JP .
JOURNAL OF NON-CRYSTALLINE SOLIDS, 2001, 285 (1-3) :135-141
[4]   Preparation of low-density xerogels by incorporation of additives during synthesis [J].
Alié, C ;
Ferauche, F ;
Pirard, R ;
Lecloux, AJ ;
Pirard, JP .
JOURNAL OF NON-CRYSTALLINE SOLIDS, 2001, 289 (1-3) :88-96
[5]   Preparation of low-density xerogels through additives to TEOS-based alcogels [J].
Alié, C ;
Pirard, R ;
Lecloux, AJ ;
Pirard, JP .
JOURNAL OF NON-CRYSTALLINE SOLIDS, 1999, 246 (03) :216-228
[6]   HYDROGEN-OXYGEN TITRATION METHOD FOR MEASUREMENT OF SUPPORTED PALLADIUM SURFACE-AREAS [J].
BENSON, JE ;
HWANG, HS ;
BOUDART, M .
JOURNAL OF CATALYSIS, 1973, 30 (01) :146-153
[7]  
Bergeret G., 1997, Handb. Heterog.Catal, V2, P439
[8]   METAL-COMPLEXES IN INORGANIC MATRICES .7. NANOMETER-SIZED, UNIFORM METAL PARTICLES IN A SIO2 MATRIX BY SOL-GEL PROCESSING OF METAL-COMPLEXES [J].
BREITSCHEIDEL, B ;
ZIEDER, J ;
SCHUBERT, U .
CHEMISTRY OF MATERIALS, 1991, 3 (03) :559-566
[9]  
Brinker C.J., 1990, SOL GEL SCI
[10]   Irreversible volume shrinkage of silica aerogels under isostatic pressure [J].
Duffours, L ;
Woignier, T ;
Phalippou, J .
JOURNAL OF NON-CRYSTALLINE SOLIDS, 1996, 194 (03) :283-290