H2O2 based α-pinene oxidation over Ti-MCM-41. A kinetic study

被引:18
作者
Canepa, Analia L. [1 ]
Herrero, Eduardo R. [1 ]
Crivello, Monica E. [1 ]
Eimer, Griselda A. [1 ]
Casuscelli, Sandra G. [1 ]
机构
[1] Univ Tecnol Nacl, Fac Reg Cordoba, Ctr Invest & Tecnol Quim CITeQ, RA-5016 Cordoba, Argentina
关键词
Kinetic; alpha-Pinene; Hydrogen peroxide; Mesoporous materials; Oxidation; HYDROGEN-PEROXIDE; SELECTIVE OXIDATION; MOLECULAR-SIEVES; ALLYLIC OXIDATION; CATALYTIC-ACTIVITY; LIQUID-PHASE; EPOXIDATION; MCM-41; EFFICIENCY; BEHAVIOR;
D O I
10.1016/j.molcata.2011.06.006
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
alpha-Pinene oxidation with hydrogen peroxide using Ti-MCM-41, prepared by hydrothermal synthesis, with a Ti content of 1.12 wt.% was studied. The major products of reaction observed were: verbenone, verbenol and camnpholenic aldehyde which are used in the pharmaceutical, perfume and cosmetics industry. The effects of various parameters such as the concentration of reagents, catalyst and temperature on the reaction rate have been studied. The experimental results show that the surface chemical reaction onto the catalytic site controls the overall reaction rate. A kinetic model that includes the absorption of reactants, water and solvent on the catalyst was proposed. The analysis of the initial rates allowed to determinate that the reaction is first order regarding to the alpha-pinene, hydrogen peroxide and catalyst amount and zero order with respect to H2O, with apparent activation energy of 67.5 kJ/mol. Under the study conditions, leaching of the active species is not observed. Finally, the catalyst can be used repeatedly without losing activity or selectivity, confirming that the reaction proceeds through a certainly heterogeneous process. (C) 2011 Elsevier B.V. All rights reserved.
引用
收藏
页码:1 / 7
页数:7
相关论文
共 41 条
  • [1] Oxidation of α-pinene over gold containing bimetallic nanoparticles supported on reducible TiO2 by deposition-precipitation method
    Ajaikumar, S.
    Ahlkvist, J.
    Larsson, W.
    Shchukarev, A.
    Leino, A. -R.
    Kordas, K.
    Mikkola, J. -P.
    [J]. APPLIED CATALYSIS A-GENERAL, 2011, 392 (1-2) : 11 - 18
  • [2] ALBERT RM, 1989, FRAGRANCE FLAVOR CHE, P479
  • [3] Bauer K., 1997, COMMON FRAGRANCE FLA
  • [4] REACTIONS OF TITANIUM SILICALITE WITH PROTIC MOLECULES AND HYDROGEN-PEROXIDE
    BELLUSSI, G
    CARATI, A
    CLERICI, MG
    MADDINELLI, G
    MILLINI, R
    [J]. JOURNAL OF CATALYSIS, 1992, 133 (01) : 220 - 230
  • [5] SYNTHESIS, CHARACTERIZATION, AND CATALYTIC ACTIVITY OF TI-MCM-41 STRUCTURES
    BLASCO, T
    CORMA, A
    NAVARRO, MT
    PARIENTE, JP
    [J]. JOURNAL OF CATALYSIS, 1995, 156 (01) : 65 - 74
  • [6] Clean limonene epoxidation using Ti-MCM-41 catalyst
    Cagnoli, MV
    Casuscelli, SG
    Alvarez, AM
    Bengoa, JF
    Gallegos, NG
    Samaniego, NM
    Crivello, ME
    Ghione, GE
    Pérez, CF
    Herrero, ER
    Marchetti, SG
    [J]. APPLIED CATALYSIS A-GENERAL, 2005, 287 (02) : 227 - 235
  • [7] Ti-MCM-41 as catalyst for α-pinene oxidation -: Study of the effect of Ti content and H2O2 addition on activity and selectivity
    Casuscelli, Sandra G.
    Eimer, Griselda A.
    Canepa, Analia
    Heredia, Angelica C.
    Poncio, Carlos E.
    Crivello, Monica E.
    Perez, Celso E.
    Aguilar, Alfredo
    Herrero, Eduardo R.
    [J]. CATALYSIS TODAY, 2008, 133 : 678 - 683
  • [8] Catalysis in the preparation of fragrances and flavours
    Chapuis, C
    Jacoby, D
    [J]. APPLIED CATALYSIS A-GENERAL, 2001, 221 (1-2) : 93 - 117
  • [9] Redox behavior and selective oxidation properties of mesoporous titano- and zirconosilicate MCM-41 molecular sieves
    Chaudhari, K
    Bal, R
    Srinivas, D
    Chandwadkar, AJ
    Sivasanker, S
    [J]. MICROPOROUS AND MESOPOROUS MATERIALS, 2001, 50 (2-3) : 209 - 218
  • [10] CHROMIUM PILLARED CLAY CATALYZED ALLYLIC OXIDATION AND OXIDATIVE DEPROTECTION OF ALLYL ETHERS AND AMINES - A SIMPLE AND CONVENIENT PROCEDURE
    CHOUDARY, BM
    PRASAD, AD
    SWAPNA, V
    VALLI, VLK
    BHUMA, V
    [J]. TETRAHEDRON, 1992, 48 (05) : 953 - 962