Highly efficient and clean synthesis of verbenone over well ordered two-dimensional mesoporous chromium silicate catalysts

被引:21
|
作者
Selvaraj, M. [1 ]
Kandaswamy, M. [2 ]
Park, D. W. [1 ]
Ha, C. S. [3 ]
机构
[1] Pusan Natl Univ, Sch Chem & Biomol Engn, Pusan 609735, South Korea
[2] Univ Madras, Dept Inorgan Chem, Madras 600025, Tamil Nadu, India
[3] Pusan Natl Univ, Dept Polymer Sci & Engn, Pusan 609735, South Korea
关键词
Two-dimensional CrSBA-15; pH-adjusting direct hydrothermal method; Ammonium fluoride method; alpha-Pinene oxidation; Catalytic stability; alpha-Pinene conversion; V=O selectivity; ALPHA-PINENE; ALLYLIC OXIDATION; MOLECULAR-SIEVES; SBA-15; AUTOXIDATION; OXYGEN;
D O I
10.1016/j.cattod.2010.03.061
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Two-dimensional mesoporous SBA-15 catalysts synthesized by different hydrothermal methods have been used, for the first time, in the liquid-phase oxidation of alpha-pinene with t-butyl hydrogen peroxide (TBHP) for the synthesis of verbenone (V=O). The recyclable CrSBA-15 catalysts have also been reused in this reaction to find their catalytic activities. To investigate the leaching of chromium species on the silica surface, CrSBA-15(8) has been treated with ammonium acetate solution, and it has been also treated with boiling water for the investigation of hydrothermal stability. The treated CrSBA-15(8) catalyst has been used in the catalytic reaction for finding the effects of catalytic stability. The influences of various reaction parameters such as temperature, time, ratios of reactant (alpha-pinene-to-TBHP) have been extensively investigated for the synthesis of V=O. In addition, the liquid-phase oxidation of alpha-pinene has been conducted with different solvents to find the best solvent with a good catalytic activity. On the basis of all investigations with a hypothetical reaction pathway of alpha-pinene oxidation, the CrSBA-15(8) catalyst is found to be a highly active, recyclable and promising heterogeneous catalyst in the liquid-phase oxidation of alpha-pinene for highly selective synthesis of V=O. Furthermore, CrSBA-15(8) catalyst has higher selectivity of V=O (88.2%) than other CrSBA-15 and CrMCM-41. (C) 2010 Elsevier B.V. All rights reserved.
引用
收藏
页码:286 / 295
页数:10
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