Cu containing octahedral molecular sieves and octahedral layered materials

被引:45
作者
Shen, YF
Suib, SL
OYoung, CL
机构
[1] UNIV CONNECTICUT,DEPT CHEM,STORRS,CT 06269
[2] UNIV CONNECTICUT,DEPT CHEM ENGN,STORRS,CT 06269
[3] UNIV CONNECTICUT,INST MAT SCI,STORRS,CT 06269
[4] TEXACO USA INC,RES CTR,BEACON,NY 12508
关键词
D O I
10.1006/jcat.1996.0168
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
Manganese oxide octahedral molecular sieves (OMS) with Cu2+ in the tunnel(Cu-OMS-1) and octahedral layer (OL) manganese oxides with CU2+ in the interlayer of buserite-like materials (Cu-OL-1) were prepared and characterized by X-ray diffraction, scanning electron microscopy/energy dispersive X-ray analysis, temperature programmed reduction, thiosulfate titrations, and volumetric adsorption of carbon monoxide (GO). The materials were tested as CO oxidation catalysts, Results show that autoclave treatment of Cu-OL-1 suspensions induces complete removal of chlorine as well as a change of the Cu/Mn ratio and average manganese oxidation state, Such changes depend on the initial MnO4-/Mn2+ ratio. At a ratio of 0.34-0.40, autoclave treatment increases the manganese oxidation state and the Cu/Mn ratio. At a ratio of 0.44, however, treatment decreases manganese oxidation state and the Cu/Mn ratio. A possible mechanism is proposed for the hydrothermal transformation of Cu-OL-1 to Cu-OMS-1, CO oxidation data show that Cu-OMS-1 has a CO conversion of 89-99% at 60-100 degrees C, while Cu-OL-1 has almost no activity in the same temperature region. This dramatic difference is due to the fact that Cu-OMS-1 has more surface oxygen and a larger CO adsorption capacity, as compared to Cu-OL-1. Different structural properties may also contribute to the difference in catalytic activity, since the todorokite tunnel structure of OMS-1 is correlated with CO conversion. Blockage of the tunnels by water and tunnel collapse cause a significant decrease in CO oxidation, Kinetic studies of CO oxidation show that water vapor in the feed stream induces a small and reversible inhibition and that a positive reaction order is found with respect to CO partial pressure under these experimental conditions. (C) 1996 Academic Press, Inc.
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收藏
页码:115 / 122
页数:8
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