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Cu containing octahedral molecular sieves and octahedral layered materials

Journal Article · · Journal of Catalysis
;  [1];  [2]
  1. Univ. of Connecticut, Storrs, CT (United States)
  2. Texaco Inc., Beacon, NY (United States)
Manganese oxide octahedral molecular sieves (OMS) with Cu{sup 2+} in the tunnel(Cu-OMS-1) and octahedral layer (OL) manganese oxides with Cu{sup 2+} 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 (CO). 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 MnO{sub 4}{sup -}/Mn{sup 2+} 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 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. 44 refs., 6 figs., 6 tabs.
OSTI ID:
476034
Journal Information:
Journal of Catalysis, Journal Name: Journal of Catalysis Journal Issue: 1 Vol. 161; ISSN 0021-9517; ISSN JCTLA5
Country of Publication:
United States
Language:
English