Microstructural comparison of calcined and uncalcined gold/iron-oxide catalysts for low-temperature CO oxidation

被引:192
|
作者
Hodge, NA
Kiely, CJ
Whyman, R
Siddiqui, MRH
Hutchings, GJ
Pankhurst, QA
Wagner, FE
Rajaram, RR
Golunski, SE
机构
[1] Univ Liverpool, Dept Mat Sci & Engn, Liverpool L69 3BX, Merseyside, England
[2] Univ Liverpool, Dept Chem, Liverpool L69 7ZD, Merseyside, England
[3] Cardiff Univ, Dept Chem, Cardiff CF10 3TB, S Glam, Wales
[4] UCL, Dept Phys, London W1CE 6BT, England
[5] Tech Univ Munich, Dept Phys, D-85747 Garching, Germany
[6] Johnson Matthey Technol Ctr, Reading RG4 9NH, Berks, England
关键词
low-temperature CO oxidation; Au-MO; Au oxyhydroxide; ferrihydrite;
D O I
10.1016/S0920-5861(01)00487-4
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
A series of gold/iron-oxide catalysts has been prepared by an inverse co-precipitation method from a mixture of HAuCl(4)(.)3H(2)O and Fe(NO(3))(3)(.)9H(2)O. Samples calcined at 400 degreesC for 3h exhibited poor activity towards CO oxidation, whereas uncalcined materials that had only been dried at 120 degreesC for 16 h exhibited a far superior catalytic activity. The most active material of this latter type is shown to have 100% CO conversion at 20 degreesC for at least 10 h. Detailed characterisation of the dried and the calcined materials using ICP and BET analysis, XRD, HREM, STEM-EDX and Mossbauer spectroscopy has shown significant differences in their microstructure. The dried materials consist of micron scale agglomerates of 4-8 nm disordered Fe(5)HO(8)(.)4H(2)O particles on which the An is uniformly dispersed in the form of a mixture AuOOH(.)xH(2)O and Au(0). By comparison, the calcined materials are comprised solely of 3-5 nm cuboctahedral metallic Au particles supported on 20 nm diameter well-crystalline alpha-Fe(2)O(3) particles. Our microstructural observations and catalytic measurements are discussed in the context of the Bond-Thompson mixed Au(x+)/Au(0) model for the low-temperature CO oxidation catalyst. (C) 2002 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:133 / 144
页数:12
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