The active role of CO2 at low temperature in oxidation processes:: the case of the oxidative dehydrogenation of propane on NiMoO4 catalysts

被引:75
作者
Dury, F [1 ]
Gaigneaux, EM [1 ]
Ruiz, P [1 ]
机构
[1] Univ Catholique Louvain, Unite Catalyse & Chim Mat Divises, B-1348 Louvain, Belgium
关键词
oxidative dehydrogenation of propane; nickel molybdate; CO2; dissociation; reactivity of CO2; dynamic control of active sites; doping gas feed;
D O I
10.1016/S0926-860X(02)00516-1
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 effects of 3 vol.% of CO2 added in the gas feed are investigated in the oxidative dehydrogenation of propane (ODP) to propene on NiMoO4 catalysts. In spite of the low reaction temperature range (400-480degreesC), it turns out that CO2 is not inert during the reaction. CO2 behaves as a strong oxidant with respect to the catalyst. CO2 helps to maintain the catalytic surface in a high oxidation state under conditions for which NiMoO4 undergoes a reduction. CO2 clearly promotes the non-selectivity of the catalyst and can inhibit deactivation. Under particular conditions it can improve propene formation. CO2 is able to oxidize propane to propene. We suggest that CO2 dissociates during the reaction to CO and an active oxygen species, which is responsible for the oxidizing effect of carbon dioxide. This work opens promising perspectives in using CO2 to tune dynamically the oxidation state of "working" oxide surfaces in their most active and selective configurations for oxidation processes. (C) 2002 Elsevier Science B.V. All rights reserved.
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页码:187 / 203
页数:17
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