In situ study of the formation and stability of supported Pd2Ga methanol steam reforming catalysts

被引:102
作者
Haghofer, Andreas [1 ]
Foettinger, Karin [1 ]
Girgsdies, Frank [2 ]
Teschner, Detre [2 ]
Knop-Gericke, Axel [2 ]
Schloegl, Robert [2 ]
Rupprechter, Guenther [1 ]
机构
[1] Vienna Univ Technol, Inst Mat Chem, A-1060 Vienna, Austria
[2] Max Planck Gesell, Fritz Haber Inst, Dept Inorgan Chem, D-14195 Berlin, Germany
关键词
Palladium; Gallium oxide; Intermetallic compound; Alloy; Methanol steam reforming; Methanol decomposition; In situ X-ray photoelectron spectroscopy; In situ IR spectroscopy; In situ X-ray diffraction; CO adsorption; SURFACE CHARACTERIZATION; SELECTIVE HYDROGENATION; INTERMETALLIC COMPOUNDS; ULTRAHIGH-VACUUM; INFRARED-SPECTRA; DEFECT FORMATION; ALLOY CATALYSTS; MODEL CATALYSTS; PD-ZN; PALLADIUM;
D O I
10.1016/j.jcat.2011.10.007
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
Pd/Ga2O3 methanol steam reforming (MSR) catalysts were characterized in detail by utilizing a range of in situ techniques of varying surface sensitivity. Correlating the nature of the intermetallic Pd-Ga compound (IMC: formed upon reduction) with the corresponding activity/selectivity revealed pronounced differences. Generally, a dynamic response of the catalyst surface to the surrounding gas environment was observed. Special attention was paid to the bulk and surface stability of the Pd-Ga IMCs. Whereas the bulk was stable in O-2, decomposition of the surface occurred resulting in a partial coverage by GaO.), islands. In addition, the main formation mechanism of undesired CO and therefore the reason limiting the selectivity to MSR were identified. CO was shown to have a detrimental effect on the selective Pd-Ga intermetallic compound, causing partial decomposition of the IMC to metallic Pd at the surface. Consequently, patches of Pd metal are present under reaction conditions, catalyzing the unwanted parallel methanol decomposition reaction. (C) 2011 Elsevier Inc. All rights reserved.
引用
收藏
页码:13 / 21
页数:9
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