Aerobic oxidation of alcohols catalyzed by gold nano-particles confined in the walls of mesoporous silica

被引:82
作者
Hu, Juncheng [1 ]
Chen, Lifang [1 ]
Zhu, Kake [1 ]
Suchopar, Andreas [1 ]
Richards, Ryan [1 ]
机构
[1] Int Jacobs Univ Bremen, Sch Sci & Engn, D-28759 Bremen, Germany
关键词
gold; mesoporous silica; nano-particle; oxidation; alcohol;
D O I
10.1016/j.cattod.2007.01.012
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Gold nano-particles confined in the walls of mesoporous silica (GMS) catalysts were successfully prepared by a novel and simple technique utilizing thioether functional groups in the walls of mesoporous silica to anchor HAuCl4. Calcination of the materials removed organic moieties and reduced the gold salt to gold nano-particles. In this procedure, the thioether groups were introduced into the silica wall via a co-condensation of tetraethyl orthosilicate (TEOS) with 1,4-bis(triethoxysily)propane tetrasulfide. These gold containing mesoporous catalysts have unusually high surface area and pore volume. The catalysts were evaluated for the solvent free liquid phase oxidation of benzyl alcohol by molecular oxygen. High selectivity to benzaldehyde was obtained under the reaction conditions of 403 K, 15 atm and 5 h in an autoclave. The 1.5% GMS catalyst was also evaluated for oxidation of alcohols using toluene as solvent under flowing oxygen at atmospheric pressure at 353 K in a two-necked flask. Under these conditions the conversion of benzyl alcohol reached 100% after 2 h and it was demonstrated that the catalyst can be recycled three times without significant loss of activity. (C) 2007 Elsevier B.V. All rights reserved.
引用
收藏
页码:277 / 283
页数:7
相关论文
共 34 条
[1]   A collaborative effect between gold and a support induces the selective oxidation of alcohols [J].
Abad, A ;
Concepción, P ;
Corma, A ;
García, H .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2005, 44 (26) :4066-4069
[2]   Synthesis and catalytic activity of periodic mesoporous materials incorporating gold nanoparticles [J].
Aprile, C ;
Abad, A ;
Hermenegildo, GA ;
Corma, A .
JOURNAL OF MATERIALS CHEMISTRY, 2005, 15 (41) :4408-4413
[3]   A green process for chlorine-free benzaldehyde from the solvent-free oxidation of benzyl alcohol with molecular oxygen over a supported nano-size gold catalyst [J].
Choudhary, VR ;
Dhar, A ;
Jana, P ;
Jha, R ;
Uphade, BS .
GREEN CHEMISTRY, 2005, 7 (11) :768-770
[4]   Commercial aspects of gold catalysis [J].
Corti, CW ;
Holliday, RJ ;
Thompson, DT .
APPLIED CATALYSIS A-GENERAL, 2005, 291 (1-2) :253-261
[5]   Efficient and selective aerobic oxidation of alcohols into aldehydes and ketones using ruthenium/TEMPO as the catalytic system [J].
Dijksman, A ;
Marino-González, A ;
Payeras, AMI ;
Arends, IWCE ;
Sheldon, RA .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2001, 123 (28) :6826-6833
[6]   Solvent-free oxidation of primary alcohols to aldehydes using supported gold catalysts [J].
Enache, DI ;
Knight, DW ;
Hutchings, GJ .
CATALYSIS LETTERS, 2005, 103 (1-2) :43-52
[7]   Solvent-free oxidation of primary alcohols to aldehydes using Au-Pd/TiO2 catalysts [J].
Enache, DI ;
Edwards, JK ;
Landon, P ;
Solsona-Espriu, B ;
Carley, AF ;
Herzing, AA ;
Watanabe, M ;
Kiely, CJ ;
Knight, DW ;
Hutchings, GJ .
SCIENCE, 2006, 311 (5759) :362-365
[8]   Incorporation of highly dispersed gold nanoparticles into the pore channels of mesoporous silica thin films and their ultrafast nonlinear optical response [J].
Gu, JL ;
Shi, JL ;
You, GJ ;
Xiong, LM ;
Qian, SX ;
Hua, ZL ;
Chen, HR .
ADVANCED MATERIALS, 2005, 17 (05) :557-+
[9]   Highly selective aerobic oxidation of alcohol catalyzed by a Gold(I) complex with an anionic ligand [J].
Guan, BT ;
Xing, D ;
Cai, GX ;
Wan, XB ;
Yu, N ;
Fang, Z ;
Yang, LP ;
Shi, ZJ .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2005, 127 (51) :18004-18005
[10]   Size- and support-dependency in the catalysis of gold [J].
Haruta, M .
CATALYSIS TODAY, 1997, 36 (01) :153-166