Deactivation of a commercial catalyst in the epoxidation of ethylene to ethylene oxide-basis for accelerated testing

被引:24
作者
Boskovic, G [1 ]
Wolf, D [1 ]
Bruckner, A [1 ]
Baerns, M [1 ]
机构
[1] ACA, Inst Appl Chem Berlin Adlershof, D-12489 Berlin, Germany
关键词
catalyst deactivation; accelerated deactivation test; deactivation compensation; Ag-based catalyst; ethylene epoxidation; deactivation mechanism; sintering;
D O I
10.1016/j.jcat.2004.02.030
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
An accelerated deactivation procedure for a commercial Ag-based catalyst for ethylene epoxidation was developed in a gradientless Bertyrecycle reactor by increasing temperature and oxygen concentration which, however, were kept constant in the whole reactor for a single experiment. Thus, deactivation kinetics could be studied explicitly. The initial rates of both C2H4O and CO2 formation and of ethylene consumption increase with reaction temperature and oxygen concentration. At 260 degreesC increasing O-2 concentration favors the rate of ethylene oxide over that of CO2 formation. Above 260 degreesC the opposite is true. Catalyst activity decays faster at both higher reaction temperature and oxygen concentration. A correlation exists between the increase of the size of Ag particles and the catalyst activity decay, pointing to sintering as the main deactivation mechanism for this catalyst. Thus, by increasing these variables the catalyst deactivation process is accelerated. (C) 2004 Elsevier Inc. All rights reserved.
引用
收藏
页码:187 / 196
页数:10
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