Mixed metal fluorides as doped Lewis acidic catalyst systems:: a comparative study involving novel high surface area metal fluorides

被引:47
作者
Murthy, JK
Gross, U
Rüdiger, S
Ünveren, E
Kemnitz, E
机构
[1] Humboldt Univ, Inst Chem, D-12489 Berlin, Germany
[2] Bundesanstalt Mat Forsch & Prufung, D-12200 Berlin, Germany
关键词
high surface area mixed metal fluorides; doped binary fluoride catalysts; Lewis acidity; heterogeneous catalysis; XPS/XAES; SEM; MAS; XRD;
D O I
10.1016/j.fluchem.2004.01.031
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
MF3-doped/MgF2 systems with enhanced Lewis acidity are reported, which are obtained either by the conventional aqueous route of co-precipitation or, by a novel non-aqueous soft chemistry route. The latter gives outstanding high surface areas and exhibits potent Lewis acid catalyst behaviour. The doped solid metal fluorides with dopant metals such as Ga, In, Fe, V are discussed in terms of the modified Tanabe model, which is adopted for metal fluoride systems. The two doped but differently prepared systems are analysed according to their surface characteristics by BET surface area, pore-size distribution and XPS/XAES as well as for the solid state structure by scanning electron microscopy (SEM), XRD and F-19-MAS-NMR. The surface properties were evaluated by photoacoustic IR-spectroscopy of pyridine adsorbates and selected catalytic reactions. The exemplarily investigated GaF3-doped/MgF2 system reveals modified intrinsic properties of the solid mixture culminating in very high surface areas of a structurally distorted mesoporous solid and electrostatic charge rearrangements causing increased Lewis acid sites. (C) 2004 Elsevier B.V. All rights reserved.
引用
收藏
页码:937 / 949
页数:13
相关论文
共 16 条
[1]   Magnesium- and iron-doped chromium fluoride hydroxyfluoride: Synthesis, characterization and catalytic activity [J].
Adamczyk, B ;
Hess, A ;
Kemnitz, E .
JOURNAL OF MATERIALS CHEMISTRY, 1996, 6 (10) :1731-1735
[2]   On a quantitative scale for Lewis acidity and recent progress in polynitrogen chemistry [J].
Christe, KO ;
Dixon, DA ;
McLemore, D ;
Wilson, WW ;
Sheehy, JA ;
Boatz, JA .
JOURNAL OF FLUORINE CHEMISTRY, 2000, 101 (02) :151-153
[3]   CHARACTERIZATION OF CATALYTICALLY ACTIVE-SITES ON ALUMINUM-OXIDES, HYDROXYFLUORIDES, AND FLUORIDES IN CORRELATION WITH THEIR CATALYTIC BEHAVIOR [J].
HESS, A ;
KEMNITZ, E .
JOURNAL OF CATALYSIS, 1994, 149 (02) :449-457
[4]   Amorphous metal fluorides with extraordinary high surface areas [J].
Kemnitz, E ;
Gross, U ;
Rudiger, S ;
Shekar, CS .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2003, 42 (35) :4251-4254
[5]   Enhanced Lewis acidity by aliovalent cation doping in metal fluorides [J].
Kemnitz, E ;
Zhu, Y ;
Adamczyk, B .
JOURNAL OF FLUORINE CHEMISTRY, 2002, 114 (02) :163-170
[6]  
KEMNITZ E, 1996, J CATAL, V159
[7]   FAST-MAGIC-ANGLE-SPINNING F-19 NMR OF INORGANIC FLUORIDES AND FLUORIDATED APATITIC SURFACES [J].
KREINBRINK, AT ;
SAZAVSKY, CD ;
PYRZ, JW ;
NELSON, DGA ;
HONKONEN, RS .
JOURNAL OF MAGNETIC RESONANCE, 1990, 88 (02) :267-276
[8]  
MANZER LE, 1989, Patent No. 0331991
[9]   STUDY OF CORE ELECTRON BINDING-ENERGIES IN SOME GROUP IIIA, VB, AND VIB COMPOUNDS [J].
MCGUIRE, GE ;
SCHWEITZ.GK ;
CARLSON, TA .
INORGANIC CHEMISTRY, 1973, 12 (10) :2450-2453
[10]  
*NIST, 1989, NIST STAND REF DAT 2