Preparation and characterization of zirconium containing mesoporous silicas. II. Grafting reaction of tetraneopentyl zirconium on MCM-41 and characterization of the grafted species and of the resulting materials

被引:27
作者
Wang, XX
Veyre, L
Lefebvre, F
Patarin, J
Basset, JM
机构
[1] CNRS, Lab Chim Organomet Surface, UMR 9986, CPE, F-69616 Villeurbanne, France
[2] Ecole Natl Super Chim, Lab Mat Mineraux, CNRS, URA 428, F-68093 Mulhouse, France
关键词
mesoporous silica; zirconium; solid-state NMR; organometallic complex; acidity;
D O I
10.1016/j.micromeso.2003.09.004
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Hydroxyl groups of MCM-41 dehydroxylated under vacuum at 500 degreesC react with tetraneopentyl zirconium, leading to the evolution of neopentane and the formation of organometallic species with the mean formula (dropSi-O)(2)ZrNp2 which were fully characterized by physicochemical methods such as solid-state NMR, infrared spectroscopy, quantification of evolved gases and microanalysis. Decomposition of the resulting materials under vacuum, oxygen, water and hydrogen has been studied. The acid properties of the Zr-MCM-41 solids obtained by this way compare well to those of Zr-MCM-41 materials obtained by direct synthesis. (C) 2003 Elsevier Inc. All rights reserved.
引用
收藏
页码:169 / 179
页数:11
相关论文
共 19 条
[1]   Surface organometallic chemistry of zirconium.: Chemical reactivity of the Si-O-ZrNP3 surface complex synthesized on dehydroxylated silica and application to the modification of mordenite [J].
Adachi, M ;
Nédez, C ;
Wang, XX ;
Bayard, F ;
Dufaud, V ;
Lefebvre, F ;
Basset, JM .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2003, 204 (204-205) :443-455
[2]   Surface organometallic chemistry: some fundamental features including the coordination effects of the support [J].
Basset, JM ;
Lefebvre, F ;
Santini, C .
COORDINATION CHEMISTRY REVIEWS, 1998, 178 :1703-1723
[3]   Synthesis and characterization of mesostructured materials [J].
Biz, S ;
Occelli, ML .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1998, 40 (03) :329-407
[4]  
CHOPLIN A, 1998, SUPPORTED REAGENTS C, P150
[5]   Catalytic cleavage of the C-H and C-C bonds of alkanes by surface organometallic chemistry: An EXAFS and IR characterization of a Zr-H catalyst [J].
Corker, J ;
Lefebvre, F ;
Lecuyer, C ;
Dufaud, V ;
Quignard, F ;
Choplin, A ;
Evans, J ;
Basset, JM .
SCIENCE, 1996, 271 (5251) :966-969
[6]   SILICA-SUPPORTED ZIRCONIA .1. CHARACTERIZATION BY INFRARED-SPECTROSCOPY, TEMPERATURE-PROGRAMMED DESORPTION, AND X-RAY-DIFFRACTION [J].
DANG, Z ;
ANDERSON, BG ;
AMENOMIYA, Y ;
MORROW, BA .
JOURNAL OF PHYSICAL CHEMISTRY, 1995, 99 (39) :14437-14443
[7]   Novel zirconium containing mesoporous silicas for oxidation reactions in the liquid phase [J].
Gontier, S ;
Tuel, A .
APPLIED CATALYSIS A-GENERAL, 1996, 143 (01) :125-135
[8]  
Jones D.J., 1997, J CHEM SOC CHEM COMM, P431
[9]   CHEMISTRY OF (SILICA)ZIRCONIUM DIHYDRIDE [J].
KING, SA ;
SCHWARTZ, J .
INORGANIC CHEMISTRY, 1991, 30 (19) :3771-3774
[10]   ORDERED MESOPOROUS MOLECULAR-SIEVES SYNTHESIZED BY A LIQUID-CRYSTAL TEMPLATE MECHANISM [J].
KRESGE, CT ;
LEONOWICZ, ME ;
ROTH, WJ ;
VARTULI, JC ;
BECK, JS .
NATURE, 1992, 359 (6397) :710-712