Production of hydrogen by partial oxidation of methanol over Cu/ZnO catalysts prepared by microemulsion technique

被引:125
作者
Agrell, J [1 ]
Hasselbo, K
Jansson, K
Järås, SG
Boutonnet, M
机构
[1] Royal Inst Technol, KTH, Dept Chem Engn & Technol, SE-10044 Stockholm, Sweden
[2] Stockholm Univ, Arrhenius Lab, SE-10691 Stockholm, Sweden
关键词
fuel cell vehicles; hydrogen production; methanol oxidation (partial); Cu/ZnO catalysts; microemulsion technique;
D O I
10.1016/S0926-860X(00)00876-0
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
Production of hydrogen by partial oxidation of methanol, using air as oxidant. has been studied over a series of Cu/ZnO catalysts prepared by microemulsion technique. The catalytic activity was compared to that of a reference catalyst prepared by conventional co-precipitation. The BET surface areas of the microemulsion catalysts (30-70 wt.% Cu) ranged from 22 to 36 m(2)/g and were considerably lower than that of the reference (60 m(2)/g). Nevertheless, the microemulsion catalysts were more active in the partial oxidation reaction and exhibited high hydrogen and carbon dioxide selectivities. At a molar O-2/CH3OH ratio of 0.1, hydrogen production was initiated at about 185 degreesC over the microemulsion catalysts. Over the reference, hydrogen production began at 215 degreesC under the same conditions. The catalytic activity was Found to be strongly dependent on the partial pressure of oxygen, which also plays an important role in determining the product distribution. By increasing the O-2/CH3OH ratio, the methanol conversion and carbon dioxide selectivity increase. while production of water occurs at the expense of hydrogen. By TEM and TPR, it was observed that Cu is less well-dispersed in the microemulsion catalysts than in the reference. The higher catalytic activity is not expected considering the lower number of exposed Cu sites, i.e, the turnover frequencies are substantially higher over the microemulsion catalysts. It is possible that, a strong interaction between a small part of CuO and the ZnO lattice is responsible for the higher turnover frequencies of the microemulsion catalysts, or that particular crystallographic Cu planes or surface imperfections are the active sites of the reaction. (C) 2001 Elsevier Science B.V. All rights reserved.
引用
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页码:239 / 250
页数:12
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