Supported Au catalysts prepared from Au phosphine complexes and As-precipitated metal hydroxides: Characterization and low-temperature CO oxidation

被引:174
作者
Yuan, YZ
Kozlova, AP
Asakura, K
Wan, HL
Tsai, K
Iwasawa, Y
机构
[1] UNIV TOKYO, GRAD SCH SCI, DEPT CHEM, BUNKYO KU, TOKYO 113, JAPAN
[2] XIAMEN UNIV, DEPT CHEM, XIAMEN 361005, PEOPLES R CHINA
[3] XIAMEN UNIV, STATE KEY LAB PHYS CHEM SOLID SURFACE, XIAMEN 361005, PEOPLES R CHINA
[4] UNIV TOKYO, FAC SCI, RES CTR SPECTROCHEM, BUNKYO KU, TOKYO 113, JAPAN
关键词
D O I
10.1006/jcat.1997.1752
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
Supported Au catalysts were prepared by attaching Au phosphine complexes, Au(PPh3)(NO3) (1) and [Au-9(PPh3)(8)](NO3)(3) (2), on as-precipitated metal hydroxides M(OH)(x)* (*, as-precipitated; M = Mn2+, Co2+, Fe3+, Ni2+, Zn2+, Mg2+, Cu2+, Ti4+, Ce4+, and La3+), followed by temperature-programmed calcination in a flow of dry air. The obtained Au catalysts showed high catalytic activities in low-temperature CO oxidation. Among the obtained Au catalysts 1/Mn(OH)(2)* and 1/Co(OH)(2)* were most highly active even at 203 K. 1/Fe(OH)(3)* and 1/Ti(OH)(4)* also catalyzed CO oxidation at low temperatures 203-273 K, whereas 1/Fe2O3 and 1/TiO2 prepared by supporting 1 on conventional Fe2O3 and TiO2 showed negligible activity under the similar reaction conditions. It was estimated by TEM and XRD that the mean diameter of Au particles in 1/Fe(OH)(3)* was about 2.9 nm, which was about 10 times smaller than that for 1/Fe2O3. EXAFS for 1/Ti(OH)(4)* revealed that the coordination number of Au-Au bond was 8-10, while that for 1/TiO2 was 11.0, which also indicates that Au particle size for 1/Ti(OH)(4)* is smaller than that for 1/TiO2. The catalysts obtained by attaching the Au complexes on commercially available metal hydroxides also showed negligible activity for the low-temperature CO oxidation under identical conditions. These results demonstrate that supported Au catalysts with small Au particles, tremendously active for the low-temperature CO oxidation, can be prepared by attaching the Au phosphine complexes on the as-precipitated metal hydroxides. Sodium cations exhibited positive effect on the Au catalysis, whereas chloride anions drastically decreased the CO oxidation activity. (C) 1997 Academic Press.
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页码:191 / 199
页数:9
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