Synthesis and Characterisation of a Highly Active Cu/ZnO:Al Catalyst

被引:95
作者
Schumann, Julia [1 ]
Lunkenbein, Thomas [1 ]
Tarasov, Andrey [1 ]
Thomas, Nygil [1 ]
Schloegl, Robert [1 ,2 ]
Behrens, Malte [1 ,3 ,4 ]
机构
[1] Max Planck Gesell, Fritz Haber Inst, Dept Inorgan Chem, D-14195 Berlin, Germany
[2] Max Planck Inst Chem Energiekonvers, Dept Heterogeneous React, Mulheim, Germany
[3] Univ Duisburg Essen, Fac Chem, D-45141 Essen, Germany
[4] Ctr Nanointegrat Duisburg Essen CENIDE, D-45141 Essen, Germany
关键词
aluminum; copper; hydrogenation; microporous materials; zinc; METHANOL SYNTHESIS CATALYSTS; REDUCTION CONDITIONS; COPPER; CU; NANOPARTICLES; CU/ZNO/AL2O3; SUPPORT; ZN; HYDROXYCARBONATES; HYDROGENATION;
D O I
10.1002/cctc.201402278
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
We report the application of an optimised synthesis protocol of a Cu/ZnO:Al catalyst. The different stages of synthesis are all well-characterised by using various methods with regard to the (micro-)structural, textural, solid-state kinetic, defect and surface properties. The low amount of the Al promoter (3%) influences but does not generally change the phase evolution known for binary Cu/ZnO catalysts. Its main function seems to be the introduction of defect sites in ZnO by doping. These sites as well as the large Cu surface area are responsible for the large N2O chemisorption capacity. Under reducing conditions, the Al promoter, just as Zn, is found enriched at the surface suggesting an active role in the strong metal-support interaction between Cu and ZnO:Al. The different stages of the synthesis are comprehensively analysed and found to be highly reproducible in the 100g scale. The resulting catalyst is characterised by a uniform elemental distribution, small Cu particles (8nm), a porous texture (pore size of approximately 25nm), high specific surface area (approximately 120m(2)g(-1)), a high amount of defects in the Cu phase and synergetic Cu-ZnO interaction. A high and stable performance was found in methanol synthesis. We wish to establish this complex but well-studied material as a benchmark system for Cu-based catalysts.
引用
收藏
页码:2889 / 2897
页数:9
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