The performance of iron-containing catalysts prepared at low temperature for carbon monoxide hydrogenation

Abstract

The performance for carbon monoxide hydrogenation of amorphous- and crystalline-unsupported iron oxides following low temperature pretreatment in nitrogen, carbon monoxide and hydrogen has been examined. The phase compositions of the catalysts before and after catalytic evaluation have been determined by⁵⁷Fe Mössbauer spectroscopy.

Pretreatment of amorphous non-potassium doped precipitates gave the formation of metallic iron catalysts which were catalytically active at low temperatures and which were shown by Mössbauer spectroscopy to be converted during evaluation to iron carbide and the iron oxide Fe₃O₄. Catalysts which were not pretreated were reduced during catalytic evaluation to Fe₃O₄.

Pretreated potassium-doped catalysts composed of either iron carbide or a mixture of iron carbide and metallic iron gave hydrocarbon product distributions which showed a higher Schulz-Flory alpha value and a lower selectivity towards methane when the catalyst reached steady state as a result of an increase in carbon monoxide adsorption and/or a decrease in hydrogen adsorption. The used catalysts were shown by Mössbauer spectroscopy to contain iron carbide together with various proportions of metallic iron and the iron oxide Fe₃O₄.

The activities of the pretreated amorphous and crystalline catalysts were comparable and may be related to the disintegration of the crystalline catalysts during pretreatment in carbon monoxide which induces the formation of particles with surface areas similar to those observed in the amorphous catalysts.