'Shape effects' in metal oxide supported nanoscale gold catalysts

被引:104
作者
Boucher, Matthew B. [1 ]
Goergen, Simone [1 ]
Yi, Nan [1 ]
Flytzani-Stephanopoulos, Maria [1 ]
机构
[1] Tufts Univ, Dept Chem & Biol Engn, Medford, MA 02155 USA
基金
美国国家科学基金会;
关键词
WATER-GAS SHIFT; METHANOL SYNTHESIS; CARBON-MONOXIDE; NANOCRYSTAL SYNTHESIS; AU/FE2O3; CATALYSTS; AU-CEO2; AU(110) SURFACE; ATOMIC OXYGEN; CO OXIDATION; ACTIVE GOLD;
D O I
10.1039/c0cp02009e
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
We report the activity of shape-controlled metal oxide (CeO2, ZnO and Fe3O4) supported gold catalysts for the steam reforming of methanol (SRM) and the water gas shift (WGS) reactions. Metal oxide nanoshapes, prepared by controlled hydrolysis and thermolysis methods, expose different crystal surfaces, and consequently disperse and stabilize gold differently. We observe that similar to gold supported on CeO2 shapes exposing the {110} and {111} surfaces, gold supported on the oxygen-rich ZnO {0001} and Fe3O4 {111} surfaces shows higher activity for the SRM and WGS reactions. While the reaction rates vary among the Au-CeO2, Au-ZnO and Au-Fe3O4 shapes, the apparent activation energies are similar, indicating a common active site. TPR data further indicate that the reaction lightoff coincides with the activation of Au-O-M species on the surface of all three oxide supports evaluated here. Different shapes contain a different number of binding sites for the gold, imparting different overall activity.
引用
收藏
页码:2517 / 2527
页数:11
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