Formation of gold clusters on TiO2 from adsorbed Au(CH3)2(C5H7O2) characterization by X-ray absorption spectroscopy

被引:41
作者
Guzman, J [1 ]
Kuba, S [1 ]
Fierro-Gonzalez, JC [1 ]
Gates, BC [1 ]
机构
[1] Univ Calif Davis, Dept Chem Engn & Mat Sci, Davis, CA 95616 USA
关键词
CO oxidation; EXAFS; gold; gold clusters; TiO2; XANES; x-ray absorption spectroscopy;
D O I
10.1023/B:CATL.0000023725.13904.cc
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
Gold nanoclusters on TiO2 powder were prepared from adsorbed Au-III(CH3)(2) (C5H7O2) (dimethyl acetylacetonate gold(III)) and characterized by extended X-ray absorption. ne structure (EXAFS) and X-ray absorption near edge structure (XANES) spectroscopies. The samples were tested as catalysts for CO oxidation at 298 K and atmospheric pressure and characterized by EXAFS and XANES with the catalysts in the working state. The XANES results identify Au(III) in the initially prepared sample, and the EXAFS data indicate mononuclear gold complexes as the predominant surface gold species in this sample, consistent with the lack of Au-Au contributions in the EXAFS spectrum. The mononuclear gold complex is bonded to two oxygen atoms of the TiO2 surface at an Au-O distance of 2.16 Angstrom. Treatment of this complex in He or in H-2 at increasing temperatures led to formation of metallic gold clusters of increasing size, ultimately those with an average diameter of about 15 Angstrom. The data demonstrate the presence of metallic gold clusters in the working catalysts and also show these clusters alone are not responsible for the catalytic activity.
引用
收藏
页码:77 / 86
页数:10
相关论文
共 50 条
[1]   γ-Al2O3-supported Pt catalysts with extremely high dispersions resulting from Pt-W interactions [J].
Alexeev, OS ;
Graham, GW ;
Shelef, M ;
Gates, BC .
JOURNAL OF CATALYSIS, 2000, 190 (01) :157-172
[2]  
Ankudinov A. L., 1996, THESIS U WASHINGTON
[3]   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
[4]   Gold-catalysed oxidation of carbon monoxide [J].
Bond, GC ;
Thompson, DT .
GOLD BULLETIN, 2000, 33 (02) :41-51
[5]   Catalysis by gold [J].
Bond, GC ;
Thompson, DT .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1999, 41 (3-4) :319-388
[6]   Cobalt promotion of Au/TiO2 catalysts for the reaction of carbon monoxide with oxygen and nitrogen oxides [J].
Cant, NW ;
Ossipoff, NJ .
CATALYSIS TODAY, 1997, 36 (01) :125-133
[7]   CRITERIA FOR AUTOMATIC X-RAY ABSORPTION FINE-STRUCTURE BACKGROUND REMOVAL [J].
COOK, JW ;
SAYERS, DE .
JOURNAL OF APPLIED PHYSICS, 1981, 52 (08) :5024-5031
[8]   Nature of the active site for CO oxidation on highly active Au/γ-Al2O3 [J].
Costello, CK ;
Kung, MC ;
Oh, HS ;
Wang, Y ;
Kung, HH .
APPLIED CATALYSIS A-GENERAL, 2002, 232 (1-2) :159-168
[9]   On the potential role of hydroxyl groups in CO oxidation over Au/Al2O3 [J].
Costello, CK ;
Yang, JH ;
Law, HY ;
Wang, Y ;
Lin, JN ;
Marks, LD ;
Kung, MC ;
Kung, HH .
APPLIED CATALYSIS A-GENERAL, 2003, 243 (01) :15-24
[10]  
DONNAY JDH, 1973, CRYSTAL DATA DETEMIN, V2, pC88