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.
Preview |
Text (Article)
Jabłońska_Manuscript MJ_MA_AB_Edit18-5-2018.pdf - Accepted Version Download (340kB) | Preview |
Preview |
Text (Figures)
Jabłońska_Figure captions MJ_AM_AB.pdf - Accepted Version Download (440kB) | Preview |
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 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 |
Archive Staff Only
 |
View Item |
