Preparation, characterization and catalytic activity towards green reactions of sulfonic functionalized SBA-15

被引:16
作者
Basaldella, Elena I. [1 ,2 ]
Soledad Legnoverde, M. [1 ,2 ]
Jimenez-Morales, Ignacio [3 ]
Rodriguez-Castellon, Enrique [3 ]
Dalla Costa, Bruno O. [4 ]
Querini, Carlos A. [4 ]
机构
[1] Univ Nacl La Plata, Ctr Invest & Desarrollo Ciencias Aplicada Dr JJ R, CCT Plata CONICET, CIC, RA-1900 La Plata, Buenos Aires, Argentina
[2] Univ Tecnol Nacl, Dept Ingn Quim, Fac Reg Plata, RA-1900 La Plata, Buenos Aires, Argentina
[3] Univ Malaga, Fac Ciencias, Dept Quim Inorgan, Unidad Asociada Inst Catalisis CSIC, E-29071 Malaga, Spain
[4] UNL, CONICET, Fac Ingn Quim, Inst Invest Catalisis & Petroquim INCAPE, RA-2654 Santiago Del Estero, Santa Fe, Argentina
来源
ADSORPTION-JOURNAL OF THE INTERNATIONAL ADSORPTION SOCIETY | 2011年 / 17卷 / 03期
关键词
Mesoporous silica; SBA-15; Functionalization; Sulfonation; Acid catalysts; Alkylation; Esterification; SOLID ACID CATALYSTS; ION-EXCHANGE-RESINS; MESOPOROUS SILICA; ISOBUTANE ALKYLATION; DEACTIVATION;
D O I
10.1007/s10450-011-9353-3
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Acidic heterogeneous catalysts based on the anchorage of sulfonic groups on SBA-15 mesoporous silica were synthesized. In a first synthesis step, samples containing mercapto groups were prepared by co-condensation of tetraethylorthosilicate with 3-mercaptopropyltrimethoxysilane, in presence of ethylene-propylene block copolymer as mesoporous silica structure director. In other samples, mercapto groups were introduced by post-functionalization of the traditional calcined SBA-15. In a second step, these mercapto groups were oxidized in order to get sulfonic acid groups on the surface. Characterization of the samples was carried out by N-2 adsorption-desorption, FTIR, XPS and acid-base titration. Spectroscopic techniques showed that the effective incorporation of sulfonic groups depends on the synthesis methodology used. In turn, the SBA-15 post-synthesis functionalization produces changes in structural characteristics like a decrease in BET surface and changes in the pore size distribution. The as-prepared materials were tested as acid catalysts in the alkylation of isobutane with 1-butene, and in the esterification of free fatty acids with methanol. The results obtained show a lack of activity in the alkylation reaction which can be associated with the formation and stabilization of the intermediate carbocation species.
引用
收藏
页码:631 / 641
页数:11
相关论文
共 37 条
  • [1] Mesoporous sulfonic acids as selective heterogeneous catalysts for the synthesis of monoglycerides
    Bossaert, WD
    De Vos, DE
    Van Rhijn, WM
    Bullen, J
    Grobet, PJ
    Jacobs, PA
    [J]. JOURNAL OF CATALYSIS, 1999, 182 (01) : 156 - 164
  • [2] Improved synthesis of some hydroxycoumarins
    Bulut, M
    Erk, C
    [J]. DYES AND PIGMENTS, 1996, 30 (02) : 99 - 104
  • [3] CATIONIC ION-EXCHANGE RESINS AS CATALYST
    CHAKRABARTI, A
    SHARMA, MM
    [J]. REACTIVE POLYMERS, 1993, 20 (1-2): : 1 - 45
  • [4] CHEMISTRY, CATALYSTS, AND PROCESSES FOR ISOPARAFFIN-OLEFIN ALKYLATION - ACTUAL SITUATION AND FUTURE-TRENDS
    CORMA, A
    MARTINEZ, A
    [J]. CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1993, 35 (04): : 483 - 570
  • [5] Isobutane alkylation with solid catalysts based on beta zeolite
    Dalla Costa, B. O.
    Querini, C. A.
    [J]. APPLIED CATALYSIS A-GENERAL, 2010, 385 (1-2) : 144 - 152
  • [6] Dalla Costa B.O., 2009, ACT 16 C ARG CAT BUE
  • [7] Deactivation pathways in zeolite-catalyzed isobutane/butene alkylation
    Feller, A
    Barth, JO
    Guzman, A
    Zuazo, I
    Lercher, JA
    [J]. JOURNAL OF CATALYSIS, 2003, 220 (01) : 192 - 206
  • [8] Engineering nanospaces: ordered mesoporous silicas as model substrates for building complex hybrid materials
    Ford, DM
    Simanek, EE
    Shantz, DF
    [J]. NANOTECHNOLOGY, 2005, 16 (07) : S458 - S475
  • [9] Hybrid materials based on aluminum tungstophosphate or tungstosilicate as catalysts in anisole acylation
    Fuchs, Vanesa A.
    Pizzio, Luis R.
    Blanco, Mirta N.
    [J]. CATALYSIS TODAY, 2008, 133 : 181 - 186
  • [10] Recovery of alkylation activity in deactivated USY catalyst using supercritical fluids: a comparison of light hydrocarbons
    Ginosar, DM
    Thompson, DN
    Burch, KC
    [J]. APPLIED CATALYSIS A-GENERAL, 2004, 262 (02) : 223 - 231