Isotope Studies in Oxidation of Propane over Vanadium Oxide

被引：30
作者：
Kube, Pierre [1 ]
Frank, Benjamin [1 ,2 ]
Schloegl, Robert [1 ]
Trunschke, Annette [1 ]
机构：
[1] Max Planck Gesell, Fritz Haber Inst, Dept Inorgan Chem, Faradayweg 4-6, D-14195 Berlin, Germany
[2] TU Berlin, BasCat UniCat BASF Joint Lab, EW K 01 Hardenbergstr 36, D-10623 Berlin, Germany
来源：
CHEMCATCHEM | 2017年 / 9卷 / 18期
关键词：
kinetic isotope effect; oxidation; propane; reaction network; vanadium oxide; DENSITY-FUNCTIONAL THEORY; REACTION-PATH ANALYSIS; SELECTIVE OXIDATION; ALKANE OXIDATION; DEHYDROGENATION; CATALYSTS; KINETICS; PROPENE; SURFACE; PROPYLENE;
D O I：
10.1002/cctc.201700847
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 oxidation of propane has been studied over silica-supported vanadium oxide and polycrystalline, bulk MoVTeNb oxide with M1 structure. Temperature-programmed reaction experiments were performed, and the reactivity of propane molecules labeled with deuterium and C-13, respectively, was analyzed under steady-state conditions. The measurement of kinetic isotope effects reveals fundamental differences in the activation of propane over the two catalysts. The reaction network of consecutive and parallel reactions of the formed propylene is comparable. However, oxygen insertion into the CHO group of acrolein under formation of acrylic acid is faster over M1 than oxidation at the CH2 group and decarbonylation to acetaldehyde. In contrast, the latter process is preferred over silica-supported vanadium oxide resulting in lower selectivity to unsaturated oxygenates.
引用
收藏
页码：3446 / 3455
页数：10
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