Gold-ceria catalysts for low-temperature water-gas shift reaction

被引:270
作者
Fu, Q [1 ]
Kudriavtseva, S [1 ]
Saltsburg, H [1 ]
Flytzani-Stephanopoulos, M [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
cerium oxide; gold; copper; water-gas shift; nanostructured ceria; oxygen storage capacity;
D O I
10.1016/S1385-8947(02)00107-9
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Nanostructured Au-ceria is a promising new catalyst for low-temperature water-gas shift (LTS). Preparation, characterization, and catalytic properties of this material are reported in this paper. Gold-ceria was prepared by deposition-precipitation (DP), coprecipitation (CP), and gelation methods. The gold loading was varied between 1 and 8.3 at.%, while lanthanum used as a dopant in ceria, was 4 or. 10 at.%. Most gold is in metallic state, but ionic gold was also present as identified by XPS. The average ceria crystallite size in samples prepared by gelation was 4.5 and 7 nm, respectively, after calcination at 400 or 650 degreesC. The gold particle size in samples prepared by DP was <5 nm after 10 h long heating in air at 400degreesC. The gold particle size did not increase with gold loading in these samples. A dramatic effect of gold on the reducibility of the surface oxygen of ceria was found by H-2-temperature-programmed reduction (TPR). All of the available surface oxygen was reduced, while there was no effect on the bulk oxygen of ceria. The enhancement of cerium oxide reducibility by gold is independent of the method of catalyst preparation. Oxygen storage capacity (OSC) measurements using step pulses of CO were in agreement with the TPR results; the presence of gold greatly enhances the OSC of ceria. Similar tests with copper-containing ceria were conduced for comparison. Carbon-containing species left on the surface after the CO step, can be fully removed with O-2 or partially removed with H2O. The high catalytic activity of Au-ceria for LTS reaction correlates well with the ceria structure and oxygen transfer properties. (C) 2002 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:41 / 53
页数:13
相关论文
共 48 条
[21]   PREPARATION OF GOLD IN Y-TYPE ZEOLITE FOR CARBON-MONOXIDE OXIDATION [J].
KANG, YM ;
WAN, BZ .
APPLIED CATALYSIS A-GENERAL, 1995, 128 (01) :53-60
[22]   A new approach to active supported Au catalysts [J].
Kozlov, AI ;
Kozlova, AP ;
Liu, HC ;
Iwasawa, Y .
APPLIED CATALYSIS A-GENERAL, 1999, 182 (01) :9-28
[23]   Reduction characteristics of copper oxide in cerium and zirconium oxide systems [J].
Kundakovic, L ;
Flytzani-Stephanopoulos, M .
APPLIED CATALYSIS A-GENERAL, 1998, 171 (01) :13-29
[24]   Cu- and Ag-modified cerium oxide catalysts for methane oxidation [J].
Kundakovic, L ;
Flytzani-Stephanopoulos, M .
JOURNAL OF CATALYSIS, 1998, 179 (01) :203-221
[25]   Low-temperature water-gas shift reaction over Cu- and Ni-loaded cerium oxide catalysts [J].
Li, Y ;
Fu, Q ;
Flytzani-Stephanopoulos, M .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2000, 27 (03) :179-191
[26]   LOW-TEMPERATURE CO OXIDATION OVER AU/TIO2 AND AU/SIO2 CATALYSTS [J].
LIN, SD ;
BOLLINGER, M ;
VANNICE, MA .
CATALYSIS LETTERS, 1993, 17 (3-4) :245-262
[27]   Transition metal-promoted oxidation catalysis by fluorite oxides: A study of CO oxidation over Cu-CeO2 [J].
Liu, W ;
Flytzani-Stephanopoulos, M .
CHEMICAL ENGINEERING JOURNAL, 1996, 64 (02) :283-294
[28]   TOTAL OXIDATION OF CARBON-MONOXIDE AND METHANE OVER TRANSITION METAL-FLUORITE OXIDE COMPOSITE CATALYSTS .1. CATALYST COMPOSITION AND ACTIVITY [J].
LIU, W ;
FLYTZANI-STEPHANOPOULOS, M .
JOURNAL OF CATALYSIS, 1995, 153 (02) :304-316
[29]   Au iron oxide catalysts: temperature programmed reduction and X-ray diffraction characterization [J].
Neri, G ;
Visco, AM ;
Galvagno, S ;
Donato, A ;
Panzalorto, M .
THERMOCHIMICA ACTA, 1999, 329 (01) :39-46
[30]  
NIEMANTSVERDRIE.J, 1995, SPECTROSCOPY CATALYS