A microkinetic model of the methanol oxidation over silver

被引:56
作者
Andreasen, A [1 ]
Lynggaard, H [1 ]
Stegelmann, C [1 ]
Stoltze, P [1 ]
机构
[1] Aalborg Univ, Dept Chem & Appl Engn Sci, DK-6700 Esbjerg, Denmark
关键词
computer simulations; models of surface kinetics; equilibrium thermodynamics and statistical mechanics; oxidation; catalysis; silver; alcohols; oxygen;
D O I
10.1016/j.susc.2003.08.007
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
A simple microkinetic model for the oxidation of methanol on silver based on surface science studies at UHV and low temperatures has been formulated. The reaction mechanism is a simple Langmuir-Hinshelwood mechanism, with one type of active oxygen and one route to formaldehyde and carbon dioxide, respectively. The model explains observed reaction orders, selectivity, apparent activation enthalpies and the choice of industrial reaction conditions. More interesting the model disproves the notion that the mechanism deduced from surface science in UHV cannot be responsible for formaldehyde synthesis at industrial steady-state conditions. The present work therefore seriously questions the prevailing models of formaldehyde synthesis in the literature. One of the reasons for this controversy is that many of the models in the literature are derived from transient experiments exhibiting dynamic effects that are not present at steady state under industrial conditions. (C) 2003 Elsevier B.V. All rights reserved.
引用
收藏
页码:5 / 23
页数:19
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