Role of gold cations in the oxidation of carbon monoxide catalyzed by iron oxide-supported gold

被引:373
作者
Hutchings, Graham J.
Hall, Matthew S.
Carley, Albert F.
Landon, Philip
Solsona, Benjamin E.
Kiely, Christopher J.
Herzing, Andrew
Makkee, Michiel
Moulijn, Jacob A.
Overweg, Arian
Fierro-Gonzalez, Juan Carlos
Guzman, Javier
Gates, Bruce C.
机构
[1] Cardiff Univ, Sch Chem, Cardiff CF10 3AT, Wales
[2] Lehigh Univ, Ctr Adv Mat & Nanotechnol, Bethlehem, PA 18015 USA
[3] Delft Univ Technol, Fac Sci Appl, DelftChemTech, NL-2628 BL Delft, Netherlands
[4] Delft Univ Technol, Fac Sci Appl, Dept Radiat Radionuclides & Reactors, NL-2629 JB Delft, Netherlands
[5] Univ Calif Davis, Dept Chem Engn & Mat Sci, Davis, CA 95616 USA
基金
美国国家科学基金会;
关键词
gold; oxidation state; catalysis; XANES; STEM-XEDS; Mossbauer spectroscopy; XPS; CO oxidation;
D O I
10.1016/j.jcat.2006.06.001
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 [物理化学]; 081704 [应用化学];
摘要
Recent intense interest in catalysis by supported gold has focused mainly on the oxidation of CO at low temperatures, which offers the potential for many important applications, including the purification of hydrogen for automotive fuel cells. Numerous, contradictory proposals have been made concerning the nature of the active sites in supported gold catalysts. We now present evidence from a set of complementary experimental methods characterizing Au/alpha-Fe2O3 catalysts, demonstrating that cationic gold plays a crucial role in catalyzing CO oxidation at 298 K, as well as in the hydrogenation of crotonaldehyde. A series of catalysts based on a co-precipitated 5-wt% Au/Fe2O3 precursor heat treated in different ways were compared for CO oxidation at ambient temperature. The catalysts were structurally and chemically analyzed by HREM and STEM-XEDS. A combination of EXAFS, in situ XANES, XPS, and Mossbauer effect spectroscopy demonstrates the important role of cationic gold in the activity of these iron oxide-supported gold catalysts. (c) 2006 Elsevier Inc. All rights reserved.
引用
收藏
页码:71 / 81
页数:11
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