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Understanding the origins of N₂O ecomposition activity in Mn(Fe)CoAlOₓ hydrotalcite derived mixed metal oxides

Jabłońska, M; Arán, MA; Beale, AM; Delahay, G; Petitto, C; Nocuń, M; Palkovits, R; (2019) Understanding the origins of N₂O ecomposition activity in Mn(Fe)CoAlOₓ hydrotalcite derived mixed metal oxides. Applied Catalysis B: Environmental , 243 pp. 66-75. 10.1016/j.apcatb.2018.10.010. Green open access

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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.

Type: Article
Title: Understanding the origins of N₂O ecomposition activity in Mn(Fe)CoAlOₓ hydrotalcite derived mixed metal oxides
Open access status: An open access version is available from UCL Discovery
DOI: 10.1016/j.apcatb.2018.10.010
Publisher version: https://doi.org/10.1016/j.apcatb.2018.10.010
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
Keywords: Hydrotalcite-like compounds, Mixed metal oxides, Cobalt, N₂O decomposition, In situ XAFS
UCL classification: UCL
UCL > Provost and Vice Provost Offices
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10061840
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