Energy & Fuels · 1999 · 16 citations · 38 references
Natural SciencesChemical EngineeringMaterials ScienceCatalysisReaction EngineeringSurface ScienceCatalyst CharacterizationCatalytic MaterialsCatalytic Reaction EngineeringCatalytic Reaction KineticsSupported CatalystsSurface CatalysisCarbon CatalystsCatalyst MechanismsCatalyst Performance EvaluationCatalytic ActivityCatalytic Reaction MechanismsMetal Oxide CatalystsOxidationSurface Area
Catalytic conversion of N 2 O to N 2 over Cu- and Co-impregnated activated carbon catalysts (Cu/AC and Co/AC) was investigated. Catalytic activity measurements were carried out in a fixed-bed flow reactor at atmospheric pressure. The catalysts were characterized by N 2 adsorption, X-ray diffraction (XRD) and thermogravimetric analysis (TGA). This study aimed to provide insights into the following aspects: the metal dispersion, changes in pore structure, influence of catalyst loading on reaction, and reaction mechanism. Increasing loading of Co or Cu led to decreasing dispersion, but 20 wt % loading was an upper limit for optimal activities in both cases, with too high loading causing sintering of metal. Co exhibited a relatively better dispersion than Cu. Impregnation of metal led to a large decrease in surface area and pore volume, especially for 30 wt % of loading. 20 wt % of loading has proved to be the optimum for both Cu and Co, which shows the highest activity. Both N 2 O−Co/AC and −Cu/AC reactions are based upon a redox mechanism, but the former is limited by the oxygen transfer from catalysts to carbon, while N 2 O chemisorption on the surface of Cu catalyst controls the latter. The removal of oxygen from cobalt promotes the activity of Co/AC, but it is beneficial for Cu/AC to keep plenty of oxygen to maintain the intermediate oxidation of copper−Cu 1+ . The different nature of the two catalysts and their catalytic reaction mechanisms are closely related to their different electronegativities.
38