Spectroscopic characterisation of the strength and stability of the acidic sites of Al-rich microporous micelle-templated silicates

被引:33
作者
Bonelli, B
Onida, B
Chen, JD
Galarneau, A
Di Renzo, F
Fajula, F
Garrone, E
机构
[1] Politecn Torino, Dipartimento Sci Mat Ingn Chim, I-10129 Turin, Italy
[2] CNRS, UMR 5618, ENSCM, Lab Mat Catalyt & Catalyse Chim Organ, F-34296 Montpellier 05, France
[3] Politecn Torino, INFM, UdR, Turin, Italy
关键词
micelle-templated materials; Bronsted acidity; Lewis acidity; FT-IR;
D O I
10.1016/j.micromeso.2003.10.007
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
A micelle-templated material with Si/Al = 2.5 has been synthesised, then either calcined to provide the H form of the sample or partially exchanged with Li+ and Na+ ions. After surfactant removal, all samples were microporous, with average diameter around 18 Angstrom. In the H form, sizeable formation of octahedral and pentacoordinated Al was found, whereas, with Na sample, Al-27 NMR spectra showed minimal occurrence of octahedral Al, so indicating that Na+ cations, in contrast with protons, do compensate tetrahedral Al in the silicate structure. All samples have been characterised via FT-IR spectroscopy of surface hydroxyl species and adsorbed probe molecules acting as Lewis bases (carbon monoxide, ammonia, propene). Although the Si/Al ratio is close to that of Y zeolites, these systems showed definitely weaker acidity, similar to that of amorphous silica-aluminas of low Al content. With H sample, no zeolite-like Bronsted site has been observed, the more acidic hydroxyls being those absorbing at 3660 cm(-1), ascribed to Si-O-Al(OH)-O-Si groups, able to transfer a proton to ammonia, but not to propene, and undergoing with CO a shift of about 220 cm(-1). With Na sample, the nearly complete exchange caused the disappearance of more acidic hydroxyls and of Al3+ Lewis sites; a fraction of Na+ cations resulted not accessible to probe molecules, being probably buried into the thick walls. With Li sample, some AI-OH species and Al3+ Lewis sites are at the surface, as a consequence of the lower degree of exchange. (C) 2003 Elsevier Inc. All rights reserved.
引用
收藏
页码:95 / 106
页数:12
相关论文
共 50 条
[1]   A NEW FAMILY OF MESOPOROUS MOLECULAR-SIEVES PREPARED WITH LIQUID-CRYSTAL TEMPLATES [J].
BECK, JS ;
VARTULI, JC ;
ROTH, WJ ;
LEONOWICZ, ME ;
KRESGE, CT ;
SCHMITT, KD ;
CHU, CTW ;
OLSON, DH ;
SHEPPARD, EW ;
MCCULLEN, SB ;
HIGGINS, JB ;
SCHLENKER, JL .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1992, 114 (27) :10834-10843
[2]   Two distinguishable lithium sites in the zeolite Li-ZSM-5 as revealed by adsorption of CO:: an infrared spectroscopic and thermodynamic characterisation [J].
Bonelli, B ;
Garrone, E ;
Fubini, B ;
Onida, B ;
Delgado, MR ;
Areán, CO .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2003, 5 (13) :2900-2905
[3]  
BONELLI B, 2000, MICROPOR MESOPOR MAT, V53, P305
[4]   SYNTHESIS OF ALUMINUM-RICH MCM-41 [J].
BORADE, RB ;
CLEARFIELD, A .
CATALYSIS LETTERS, 1995, 31 (2-3) :267-272
[5]  
BURNEAU A, 1999, SURFACE PROPERTIES S, P194
[6]   Aluminum incorporation in MCM-41 mesoporous molecular sieves [J].
Busio, M ;
Janchen, J ;
vanHooff, JHC .
MICROPOROUS MATERIALS, 1995, 5 (04) :211-218
[7]   Towards the Loewenstein limit (Si/Al=1) in thermally stable mesoporous aluminosilicates [J].
Cabrera, S ;
El Haskouri, J ;
Mendioroz, S ;
Guillem, C ;
Latorre, J ;
Beltrán-Porter, A ;
Beltrán-Porter, D ;
Marcos, MD ;
Amorós, P .
CHEMICAL COMMUNICATIONS, 1999, (17) :1679-1680
[8]   Bronsted acidity of extraframework debris in steamed Y zeolites from the FTIR study of CO adsorption [J].
Cairon, O ;
Chevreau, T ;
Lavalley, JC .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1998, 94 (19) :3039-3047
[9]   Room-temperature formation of thermally stable aluminium-rich mesoporous MCM-41 [J].
Chatterjee, M ;
Iwasaki, T ;
Hayashi, H ;
Onodera, Y ;
Ebina, T ;
Nagase, T .
CATALYSIS LETTERS, 1998, 52 (1-2) :21-23
[10]   STUDIES ON MESOPOROUS MATERIALS .2. SYNTHESIS MECHANISM OF MCM-41 [J].
CHEN, CY ;
BURKETT, SL ;
LI, HX ;
DAVIS, ME .
MICROPOROUS MATERIALS, 1993, 2 (01) :27-34