Kinetics and mechanism of o-aminophenol oxidation by the supported mesoporous silica (HISiO2) in the binary system with Amberlite resin

被引:15
作者
El-Safty, SA
Evans, J
El-Sheikh, MY
Zaki, AB
机构
[1] Tanta Univ, Fac Sci, Dept Chem, Tanta, Egypt
[2] Univ Southampton, Dept Chem, Southampton SO17 1BJ, Hants, England
关键词
hexagonal mesoporous silica; amberlite anion-exchanger; o-aminophenol; copper-complexes; synthesis; oxidation; kinetics;
D O I
10.1016/S0927-7757(01)01102-5
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
H1SiO2 (hexagonal mesoporous silica) was synthesized with a high concentration of a non-ionic template. The synthesized H1SiO2 materials have a well defined porous architecture with surface area (760 m(2) g(-1)), and pore size = 35 Angstrom. Cu(II)-aquo complex was anchored onto silica (S-Cu-II) through the coordination with amino-functionalized H1SiO2 (S-NH2) without impregnation on the surface, The oxidation of omicron-aminophenol (omicron-AP) with (S-Cu-II), Cu(II)-oxalate complex supported on Amberlite resin (R-Cu-II), (R-Cu-II)/S-NH2 (0.05 g), and a mixture (1:1) of (R-Cu-II)/(S-Cu-II), has been studied at different temperatures (25-40 degreesC) +/- 0.1. The oxidation product has been monitored kinetically and spectrophotometrically. All redox reactions were characterized by first-order kinetics. The rate constant of the oxidation reaction of omicron-AP decreases in the following order; (S-Cu-II) > (R-Cu-II)/(S-Cu-II) > (R-Cu-II)/(S-NH2) > (R-Cu-II). This sequence reflects the role of the effective surface area of H1SiO2 on the redox reaction. The activation parameters for the amine oxidation have been estimated. Besides, a mechanism of the oxidation process of omicron-AP has been proposed. (C) 2002 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:217 / 228
页数:12
相关论文
共 53 条
  • [1] LIQUID-CRYSTALLINE PHASES AS TEMPLATES FOR THE SYNTHESIS OF MESOPOROUS SILICA
    ATTARD, GS
    GLYDE, JC
    GOLTNER, CG
    [J]. NATURE, 1995, 378 (6555) : 366 - 368
  • [2] Attard GS, 1998, STUD SURF SCI CATAL, V117, P89
  • [3] Liquid-crystal templates for nanostructured metals
    Attard, GS
    Goltner, CG
    Corker, JM
    Henke, S
    Templer, RH
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION IN ENGLISH, 1997, 36 (12): : 1315 - 1317
  • [4] TEMPLATING OF MESOPOROUS MOLECULAR-SIEVES BY NONIONIC POLYETHYLENE OXIDE SURFACTANTS
    BAGSHAW, SA
    PROUZET, E
    PINNAVAIA, TJ
    [J]. SCIENCE, 1995, 269 (5228) : 1242 - 1244
  • [5] Mesoporous alumina molecular sieves
    Bagshaw, SA
    Pinnavaia, TJ
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION IN ENGLISH, 1996, 35 (10): : 1102 - 1105
  • [6] BANSCH B, 1991, INORG CHEM, V30, P4555
  • [7] 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
  • [8] Brunel D, 1995, STUD SURF SCI CATAL, V97, P173
  • [9] Monoglyceride synthesis by heterogeneous catalysis using MCM-41 type silicas functionalized with amino groups
    Cauvel, A
    Renard, G
    Brunel, D
    [J]. JOURNAL OF ORGANIC CHEMISTRY, 1997, 62 (03) : 749 - 751
  • [10] Synthesis and characterization of the gallosilicate mesoporous molecular sieve MCM-41
    Cheng, CF
    He, HY
    Zhou, WZ
    Klinowski, J
    Goncalves, JAS
    Gladden, LF
    [J]. JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (01) : 390 - 396