Cu-Zn Alloy Formation as Unfavored State for Efficient Methanol Catalysts

被引:51
作者
Frei, Elias [1 ]
Gaur, Abhijeet [2 ,3 ]
Lichtenberg, Henning [2 ,3 ]
Zwiener, Leon [1 ]
Scherzer, Michael [1 ]
Girgsdies, Frank [1 ]
Lunkenbein, Thomas [1 ]
Schloegl, Robert [1 ,4 ]
机构
[1] Max Planck Gesell, Fritz Haber Inst, Dept Inorgan Chem, Faradayweg 4-6, D-14195 Berlin, Germany
[2] Karlsruher Inst Technol, Inst Chem Technol & Polymer Chem, Engesserstr 20, D-76131 Karlsruhe, Germany
[3] Karlsruher Inst Technol, Inst Catalysis Res & Technol, Engesserstr 20, D-76131 Karlsruhe, Germany
[4] Max Planck Inst Chem Energy Convers, Dept Heterogeneous React, Stiftstr 34-36, D-45470 Mulheim, Germany
关键词
methanol synthesis; CuZn-alloy formation; Cu lattice parameter; Cu; ZnO-interface; In-situ XAS; XRD; ALPHA-BRASS FORMATION; ZINC OXIDE CATALYSTS; GAS SHIFT REACTION; CO2; HYDROGENATION; ACTIVE-SITES; COPPER; CU/ZNO; SURFACE; ADSORPTION; INTERFACE;
D O I
10.1002/cctc.202000777
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
The active sites of Cu/ZnO-based catalysts, commercially applied for the hydrogenation of CO(2)or CO2-rich synthesis gas, are still subject of current debates. Generally, the discussion is focused on the nature of the interfacial contact between Cu and ZnO, particularly whether it is rather of oxidic (Cu-ZnO) or alloying (Cu-Zn) character. We report on kinetic investigations on a Cu/ZnO : Al high performance catalyst activated at different temperatures. Incrementally increasing temperature under reductive conditions leads also to increased CuZn-alloy formation, analyzed byin-situX-ray diffraction,in-situX-ray absorption spectroscopy and high resolution transmission electron microscopy. The combination of the catalytic data and the complementary characterization techniques provide valuable insights on the relevant reaction sites for CH3OH formation. Our results highlight the complexity of the interfacial contact with evidence for Cu-ZnO reaction sites and clarify the negative impact of CuZn alloy formation on the nature of the active site.
引用
收藏
页码:4029 / 4033
页数:5
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