Preparation of highly active silica-supported Au catalysts for CO oxidation by a solution-based technique

被引:189
作者
Zhu, Haoguo [1 ]
Liang, Chengdu [1 ]
Yan, Wenfu [1 ]
Overbury, Steven H. [1 ]
Dai, Sheng [1 ]
机构
[1] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA
关键词
D O I
10.1021/jp060637q
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
Although Au catalysts can be readily prepared on titania via the deposition-precipitation (DP) method, the direct application of the method similar to the preparation of silica-supported Au catalysts only results in diminished success. This paper reports a novel, efficient method to synthesize highly active Au catalysts supported on mesoporous silica (SBA-15) through a gold cationic complex precursor [Au(en)(2)](3+) (en = ethylenediamine) via a wet chemical process. The gold cationic precursor was immobilized on negatively charged surfaces of silica by a unique DP method that makes use of the deprotonation reaction of ethylenediamine ligands. The resulting mesoporous catalyst has been demonstrated to be highly active for CO oxidation at room temperature and even below 273 K, the activity of which is much superior to that of silica-supported Au catalysts previously prepared by various solution techniques. The pH value of the gold precursor solution plays a key role in determining the catalytic activity through the regulation of [Au(en)(2)](3+) deprotonation reaction and the surface interaction of silica with the gold precursor. This mesoporous gold silica catalyst has also been shown to be highly resistant to sintering because of the stabilization of Au nanoparticles inside mesopores.
引用
收藏
页码:10842 / 10848
页数:7
相关论文
共 38 条
[1]   THE REACTION OF GOLD(III) WITH SOME BIDENTATE COORDINATING GROUPS [J].
BLOCK, BP ;
BAILAR, JC .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1951, 73 (10) :4722-4725
[2]   Catalysis by gold [J].
Bond, GC ;
Thompson, DT .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1999, 41 (3-4) :319-388
[3]   CO oxidation over gold nanocatalyst confined in mesoporous silica [J].
Chi, YS ;
Lin, HP ;
Mou, CY .
APPLIED CATALYSIS A-GENERAL, 2005, 284 (1-2) :199-206
[4]   Hierarchically imprinted sorbents for the separation of metal ions [J].
Dai, S ;
Burleigh, MC ;
Ju, YH ;
Gao, HJ ;
Lin, JS ;
Pennycook, SJ ;
Barnes, CE ;
Xue, ZL .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2000, 122 (05) :992-993
[5]   Vital role of moisture in the catalytic activity of supported gold nanoparticles [J].
Daté, M ;
Okumura, M ;
Tsubota, S ;
Haruta, M .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2004, 43 (16) :2129-2132
[6]   CHEMICAL REACTIVITY OF SUPPORTED GOLD .4. REDUCTION OF NO BY H-2 [J].
GALVAGNO, S ;
PARRAVANO, G .
JOURNAL OF CATALYSIS, 1978, 55 (02) :178-190
[7]   Gold nanoparticles deposited on SiO2/Si(100):: Correlation between size, electron structure, and activity in CO oxidation [J].
Guczi, L ;
Petö, G ;
Beck, A ;
Frey, K ;
Geszti, O ;
Molnár, G ;
Daróczi, C .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2003, 125 (14) :4332-4337
[8]   Surface characterization of Au/HY by Xe-129 NMR and diffuse reflectance IR spectroscopy of adsorbed CO. Formation of electron-deficient gold particles inside HY cavities [J].
Guillemot, D ;
Borovkov, VY ;
Kazansky, VB ;
PolissetThfoin, M ;
Fraissard, J .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1997, 93 (19) :3587-3591
[9]   Advances in the catalysis of Au nanoparticles [J].
Haruta, M ;
Daté, M .
APPLIED CATALYSIS A-GENERAL, 2001, 222 (1-2) :427-437
[10]   NOVEL GOLD CATALYSTS FOR THE OXIDATION OF CARBON-MONOXIDE AT A TEMPERATURE FAR BELOW 0-DEGREES-C [J].
HARUTA, M ;
KOBAYASHI, T ;
SANO, H ;
YAMADA, N .
CHEMISTRY LETTERS, 1987, (02) :405-408