Stability of bimetallic Pd-Zn catalysts for the steam reforming of methanol

被引:159
作者
Conant, Travis [1 ]
Karim, Ayman M. [1 ]
Lebarbier, Vanessa [1 ,2 ]
Wang, Yong [2 ]
Girgsdies, Frank [3 ]
Schloegl, Robert [3 ]
Datye, Abhaya [1 ]
机构
[1] Univ New Mexico, Dept Chem & Nucl Engn, Ctr Microengineered Mat, Albuquerque, NM 87131 USA
[2] Pacific NW Natl Lab, Richland, WA 99352 USA
[3] Max Planck Gesell, Fritz Haber Inst, D-1000 Berlin, Germany
基金
美国国家科学基金会;
关键词
methanol steam reforming; PdZn alloy; STEM; EDS; FTIR; XRD;
D O I
10.1016/j.jcat.2008.04.018
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
ZnO-supported palladium-based catalysts have been shown in recent years to be both active and selective towards the steam reforming of methanol, although they are still considered to be less active than traditional copper-based catalysts. The activity of PdZn catalysts can be significantly improved by supporting them on alumina. Here we show that the Pd/ZnO/Al2O3 catalysts have better long-term stability when compared with commercial Cu/ZnO/Al2O3 catalysts, and that they are also stable under redox cycling. The Pd/ZnO/Al2O3 catalysts can be easily regenerated by oxidation in air at 420 degrees C followed by re-exposure to reaction conditions at 250 degrees C, while the Cu/ZnO based catalysts do not recover their activity after oxidation. Reduction at high temperatures (> 420 degrees C leads to Zn loss from the alloy nanoparticle surface resulting in a reduced catalyst activity. However, even after such extreme treatment, the catalyst activity is regained with time on stream under reaction conditions alone, leading to highly stable catalysts. These findings illustrate that the nanoparticle surface is dynamic and changes drastically depending on the environment, and that elevated reduction temperatures are not necessary to achieve high CO2 selectivity. (c) 2008 Elsevier Inc. All rights reserved.
引用
收藏
页码:64 / 70
页数:7
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