Thermal stability and catalytic activity of gold nanoparticles supported on silica

被引:166
作者
Veith, Gabriel M. [1 ]
Lupini, Andrew R. [1 ]
Rashkeev, Sergey [1 ,2 ]
Pennycook, Stephen J. [1 ]
Mullins, David R. [3 ]
Schwartz, Viviane [3 ,4 ]
Bridges, Craig A. [3 ]
Dudney, Nancy J. [1 ]
机构
[1] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA
[2] Vanderbilt Univ, Dept Phys, Nashville, TN 37235 USA
[3] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA
[4] Oak Ridge Natl Lab, Ctr Nanophase, Div Mat Sci, Oak Ridge, TN 37831 USA
关键词
Gold catalyst; Silica; Sputtering; Thermal stability; Tammann temperature; Titania; Gold reference catalyst; DFT calculations; Gold-support interaction; TEMPERATURE CO OXIDATION; METAL-CLUSTERS; AU; AU/TIO2; ADSORPTION; DEPOSITION; PARTICLES; SURFACE; SIO2; SIZE;
D O I
10.1016/j.jcat.2008.12.005
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
2.5 nm gold nanoparticles were grown on a fumed silica support, using the physical vapor deposition technique of magnetron sputtering, that are thermally stable when annealed in an oxygen containing environment up to at least 500 degrees C. Traditional Au/TiO2 catalysts rapidly sinter to form large 13.9 nm gold clusters under these annealing conditions. This surprising stability of Au/SiO2 is attributed to the absence of residual impurities (ensured by the halide-free production method) and a strong bond between gold and defects at the silica surface (about 3 eV per bond) estimated from density functional theory (DFT) calculations. The Au/SiO2 catalysts are less active for CO oxidation than the prototypical Au/TiO2 catalysts, however they can be regenerated far more easily, allowing the activity of a catalyst to be fully recovered after deactivation. (C) 2008 Elsevier Inc. All rights reserved.
引用
收藏
页码:92 / 101
页数:10
相关论文
共 71 条
[1]   X-ray absorption spectroscopic studies on gold nanoparticles in mesoporous and microporous materials [J].
Akolekar, DB ;
Foran, G ;
Bhargava, SK .
JOURNAL OF SYNCHROTRON RADIATION, 2004, 11 :284-290
[2]  
[Anonymous], IMPACT ELECT SCANNIN
[3]  
[Anonymous], 1992, Handbook of X-Ray Photoelectron Spectroscopy: A Reference Book of Standard Spectra for Identification and Interpretation of XPS Data 1992
[4]   Structure and bonding of gold metal clusters, colloids, and nanowires studied by EXAFS, XANES, and WAXS [J].
Benfield, RE ;
Grandjean, D ;
Kröll, M ;
Pugin, R ;
Sawitowski, T ;
Schmid, G .
JOURNAL OF PHYSICAL CHEMISTRY B, 2001, 105 (10) :1961-1970
[5]   Depth sectioning with the aberration-corrected scanning transmission electron microscope [J].
Borisevich, AY ;
Lupini, AR ;
Pennycook, SJ .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2006, 103 (09) :3044-3048
[6]   Gold-organic-inorganic high-surface-area materials as precursors of highly active catalysts [J].
Budroni, Gerolamo ;
Corma, Avelino .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2006, 45 (20) :3328-3331
[7]   New method for analysis of nanoparticle geometry in supported fee metal catalysts with scanning transmission electron microscopy [J].
Carlsson, A ;
Puig-Molina, A ;
Janssens, TVW .
JOURNAL OF PHYSICAL CHEMISTRY B, 2006, 110 (11) :5286-5293
[8]   Metal-support and preparation influence on the structural and electronic properties of gold catalysts [J].
Casaletto, MP ;
Longo, A ;
Venezia, AM ;
Martorana, A ;
Prestianni, A .
APPLIED CATALYSIS A-GENERAL, 2006, 302 (02) :309-316
[9]   Interaction of Au with titania: the role of reduced Ti [J].
Chen, M. S. ;
Goodman, D. W. .
TOPICS IN CATALYSIS, 2007, 44 (1-2) :41-47
[10]   High catalytic activity for CO oxidation of gold nanoparticles confined in acidic support Al-SBA-15 at low temperatures [J].
Chiang, CW ;
Wang, AQ ;
Wan, BZ ;
Mou, CY .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (38) :18042-18047