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
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  • [1] A NEW FAMILY OF MESOPOROUS MOLECULAR-SIEVES PREPARED WITH LIQUID-CRYSTAL TEMPLATES
    BECK, JS
    VARTULI, JC
    ROTH, WJ
    LEONOWICZ, ME
    KRESGE, CT
    SCHMITT, KD
    CHU, CTW
    OLSON, DH
    SHEPPARD, EW
    MCCULLEN, SB
    HIGGINS, JB
    SCHLENKER, JL
    [J]. 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
    Bonelli, B
    Garrone, E
    Fubini, B
    Onida, B
    Delgado, MR
    Areán, CO
    [J]. 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
    BORADE, RB
    CLEARFIELD, A
    [J]. 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
    Busio, M
    Janchen, J
    vanHooff, JHC
    [J]. MICROPOROUS MATERIALS, 1995, 5 (04): : 211 - 218
  • [7] Towards the Loewenstein limit (Si/Al=1) in thermally stable mesoporous aluminosilicates
    Cabrera, S
    El Haskouri, J
    Mendioroz, S
    Guillem, C
    Latorre, J
    Beltrán-Porter, A
    Beltrán-Porter, D
    Marcos, MD
    Amorós, P
    [J]. CHEMICAL COMMUNICATIONS, 1999, (17) : 1679 - 1680
  • [8] Bronsted acidity of extraframework debris in steamed Y zeolites from the FTIR study of CO adsorption
    Cairon, O
    Chevreau, T
    Lavalley, JC
    [J]. JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1998, 94 (19): : 3039 - 3047
  • [9] Room-temperature formation of thermally stable aluminium-rich mesoporous MCM-41
    Chatterjee, M
    Iwasaki, T
    Hayashi, H
    Onodera, Y
    Ebina, T
    Nagase, T
    [J]. CATALYSIS LETTERS, 1998, 52 (1-2) : 21 - 23
  • [10] STUDIES ON MESOPOROUS MATERIALS .2. SYNTHESIS MECHANISM OF MCM-41
    CHEN, CY
    BURKETT, SL
    LI, HX
    DAVIS, ME
    [J]. MICROPOROUS MATERIALS, 1993, 2 (01): : 27 - 34