Metallic Corner Atoms in Gold Clusters Supported on Rutile Are the Dominant Active Site during Water-Gas Shift Catalysis

被引:172
作者
Williams, W. Damion [1 ]
Shekhar, Mayank [1 ]
Lee, Wen-Sheng [1 ]
Kispersky, Vincent [1 ]
Delgass, W. Nicholas [1 ]
Ribeiro, Fabio H. [1 ]
Kim, Seung Min [2 ,3 ]
Stach, Eric A. [2 ,3 ]
Miller, Jeffrey T. [4 ]
Allard, Lawrence F. [5 ]
机构
[1] Purdue Univ, Sch Chem Engn, W Lafayette, IN 47907 USA
[2] Purdue Univ, Sch Mat Engn, W Lafayette, IN 47907 USA
[3] Birck Nanotechnol Ctr, W Lafayette, IN 47907 USA
[4] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA
[5] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA
关键词
CO OXIDATION; AU; NANOPARTICLES; AU/TIO2; NOBLE;
D O I
10.1021/ja1064262
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Au/TiO2 catalysts used in the water gas shift (WGS) reaction at 120 degrees C, 7% CO, 22% H2O, 9% CO2, and 37% H-2 had rates up to 0.1 moles of CO converted per mole of Au per second. However, the rate per mole of Au depends strongly on the Au particle size. The use of a nonporous, model support allowed for imaging of the active catalyst and a precise determination of the gold size distribution using transmission electron microscopy (TEM) because all the gold is exposed on the surface. A physical model of Au/TiO2 is used to show that corner atoms with fewer than seven neighboring gold atoms are the dominant active sites. The number of corner sites does not vary as particle size increases above 1 nm, giving the surprising result that the rate per gold cluster is independent of size.
引用
收藏
页码:14018 / 14020
页数:3
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