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
  • [11] ION-EXCHANGE RESINS AS CATALYSTS IN THE HYDROLYSIS OF ESTERS
    DAVIES, CW
    THOMAS, GG
    [J]. JOURNAL OF THE CHEMICAL SOCIETY, 1952, (MAY): : 1607 - 1610
  • [12] Engelhardt G., 1987, HIGH RESOLUTION SOLI
  • [13] Incorporation of transition-metal complexes in functionalized mesoporous silica and their activity toward the oxidation of aromatic amines
    Evans, J
    Zaki, AB
    El-Sheikh, MY
    El-Safty, SA
    [J]. JOURNAL OF PHYSICAL CHEMISTRY B, 2000, 104 (44) : 10271 - 10281
  • [14] Functionalized monolayers on ordered mesoporous supports
    Feng, X
    Fryxell, GE
    Wang, LQ
    Kim, AY
    Liu, J
    Kemner, KM
    [J]. SCIENCE, 1997, 276 (5314) : 923 - 926
  • [15] FREI E, 1974, CANCER CHEMOTH REP 1, V58, P49
  • [16] THE INTERACTION OF NO WITH COPPER IONS IN ZSM5 - AN EPR AND IR INVESTIGATION
    GIAMELLO, E
    MURPHY, D
    MAGNACCA, G
    MORTERRA, C
    SHIOYA, Y
    NOMURA, T
    ANPO, M
    [J]. JOURNAL OF CATALYSIS, 1992, 136 (02) : 510 - 520
  • [17] THE ABSORPTION SPECTRA OF COMPLEX OXALATES
    GRADDON, DP
    [J]. JOURNAL OF INORGANIC & NUCLEAR CHEMISTRY, 1956, 3 (05): : 308 - 322
  • [18] Gregg S.J., 1992, Adsorption, Surface area, and Porosity
  • [19] Helferich F., 1962, ION EXCHANGE
  • [20] ACTINOMYCIN - CHEMISTRY AND MECHANISM OF ACTION
    HOLLSTEIN, U
    [J]. CHEMICAL REVIEWS, 1974, 74 (06) : 625 - 652