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Publication Detail
Understanding the origins of N₂O ecomposition activity in Mn(Fe)CoAlOₓ hydrotalcite derived mixed metal oxides
Abstract
The catalytic decomposition of N₂O was studied over a series of calcined Mn(Fe)CoAl hydrotalcite-like compounds. The precursors were prepared by coprecipitation and characterized by XRD and TGA. The mixed metal oxides derived after calcination at 600 °C were characterized by XRD, N₂ adsorption, H₂-TPR and XPS. Moreover, in situ XAFS measurements over selected mixed metal oxides were performed. Such investigations under relevant reaction conditions are rare, while a comprehensive understanding of the involved active species may facilitate a knowledge-based catalyst optimization. The activity of the CoAlOₓ (Co/Al = 3/1, mol.%) catalyst varied depending on the loading of Mn or Fe (0.0575, 0.0821, 0.1150, 0.1725, 0.2300, mol.%). In the investigated series, Mn₀.₁₇₂₅Co₃A₁Oₓ reached the highest activity with T₅₀ of about 305 and 376 °C under N₂O/N₂ and N₂O,NO,O₂/N₂ feed, respectively. In situ X-ray absorption experiments over Mn₀.₁₇₂₅Co₃A₁Oₓ suggested that MnₓCo_{y}O₄ spinels undergo reduction to CoO and MnO upon heating up to 600 °C in He. Under N₂O/He conditions, initial reoxidation of cobalt species began at 350 °C. The lower activity obtained for Fe₀.₁₇₂₅Co₃A₁Oₓ is explained by the fact that the majority of Fe was not incorporated into the Co₃O₄ structure but instead formed less reactive iron oxide clusters.
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