Nanoporous Au: An Unsupported Pure Gold Catalyst?

被引:217
作者
Wittstock, Arne [2 ]
Neumann, Bjoern [2 ]
Schaefer, Andreas [2 ]
Dumbuya, Karifala [1 ]
Kuebel, Christian [4 ]
Biener, Monika M. [3 ]
Zielasek, Volkmar [2 ]
Steinrueck, Hans-Peter [1 ]
Gottfried, J. Michael [1 ]
Biener, Juergen
Hamza, Alex [3 ]
Baeumer, Marcus [2 ]
机构
[1] Univ Erlangen Nurnberg, Lehrstuhl Phys Chem 2, D-91058 Erlangen, Germany
[2] Univ Bremen, Inst Appl & Phys Chem, D-28359 Bremen, Germany
[3] Lawrence Livermore Natl Lab, Nanoscale Synth & Characterizat Lab, Livermore, CA 94550 USA
[4] Fraunhofer Inst Mfg Technol & Appl Mat Sci IFAM, Adhes Bonding & Surfaces Div, D-28359 Bremen, Germany
关键词
CO OXIDATION; CARBON-MONOXIDE; BIMETALLIC NANOPARTICLES; SURFACE CHARACTERIZATION; MECHANICAL-BEHAVIOR; AG; ADSORPTION; OXYGEN; O-2; EPOXIDATION;
D O I
10.1021/jp808185v
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
The unique properties of gold especially in low temperature CO oxidation have been ascribed to a combination of various effects. In particular, particle sizes below a few nanometers and specific particle-support interactions have been shown to play important roles. In contrast, recent reports revealed that monolithic nanoporous gold (npAu) prepared by leaching a less noble metal, such as Ag, out of the corresponding alloy can also exhibit a remarkably high catalytic activity for CO oxidation, even though no support is present. Therefore, it was claimed to be a pure and unsupported gold catalyst. We investigated npAu with respect to its morphology, surface composition, and catalytic properties. In particular, we studied the reaction kinetics for low temperature CO oxidation in detail, taking the mass transport limitation due to the porous structure of the material into account. Our results reveal that Ag, even if removed almost completely from the bulk, segregates to the surface, resulting in surface concentrations of up to 10 atom %. Our data suggest that this Ag plays a significant role in activating of molecular oxygen. Therefore, npAu should be considered a bimetallic catalyst rather than a pure Au catalyst.
引用
收藏
页码:5593 / 5600
页数:8
相关论文
共 58 条
[31]   Synergistic effect in an Au-Ag alloy nanocatalyst: CO oxidation [J].
Liu, JH ;
Wang, AQ ;
Chi, YS ;
Lin, HP ;
Mou, CY .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (01) :40-43
[32]   Identifying an O2 supply pathway in CO oxidation on Au/TiO2(110):: A density functional theory study on the intrinsic role of water [J].
Liu, LM ;
McAllister, B ;
Ye, HQ ;
Hu, P .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2006, 128 (12) :4017-4022
[33]   Surface chemistry of catalysis by gold [J].
Meyer, R ;
Lemire, C ;
Shaikhutdinov, SK ;
Freund, H .
GOLD BULLETIN, 2004, 37 (1-2) :72-+
[34]   ALUMINA-SILICA AEROGEL CATALYSTS PREPARED BY 2 SUPERCRITICAL DRYING METHODS FOR METHANE COMBUSTION [J].
MIZUSHIMA, Y ;
HORI, M .
JOURNAL OF MATERIALS SCIENCE, 1995, 30 (06) :1551-1555
[35]   Activation of O-2 on Cu, Ag, and Au surfaces for the epoxidation of ethylene: dipped adcluster model study [J].
Nakatsuji, H ;
Hu, ZM ;
Nakai, H ;
Ikeda, K .
SURFACE SCIENCE, 1997, 387 (1-3) :328-341
[36]   On the transient gas flow through catalytically active micromachined channels [J].
Norberg, P ;
Ackelid, U ;
Lundstrom, I ;
Petersson, LG .
JOURNAL OF APPLIED PHYSICS, 1997, 81 (05) :2094-2100
[37]   New setup for in situ x-ray photoelectron spectroscopy from ultrahigh vacuum to 1 mbar -: art. no. 014102 [J].
Pantförder, J ;
Pöllmann, S ;
Zhu, JF ;
Borgmann, D ;
Denecke, R ;
Steinrück, HP .
REVIEW OF SCIENTIFIC INSTRUMENTS, 2005, 76 (01) :014102-1
[38]   A GENERAL CRITERION FOR DIFFUSION INFLUENCED CHEMICAL REACTIONS IN POROUS SOLIDS [J].
PETERSEN, EE .
CHEMICAL ENGINEERING SCIENCE, 1965, 20 (06) :587-&
[39]   Active role of buried ultrathin oxide layers in adsorption of O2 on Au films [J].
Quek, Su Ying ;
Friend, Cynthia M. ;
Kaxiras, Efthimios .
SURFACE SCIENCE, 2006, 600 (17) :3388-3393
[40]   Water-gas shift activity of Au and Cu nanoparticles supported on molybdenum oxides [J].
Rodriguez, J. A. ;
Liu, R. ;
Hrbek, J. ;
Perez, M. ;
Evans, J. .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2008, 281 (1-2) :59-65