Artículo
Impact of Topology Framework of Microporous Solids on Methanol Carbonylation: An Operando DRIFTS-MS Study
Autor/es | Luque Álvarez, Ligia Amelia
Serrano Cruz, Melania González Castaño, Míriam Bobadilla Baladrón, Luis Francisco Odriozola Gordón, José Antonio |
Departamento | Universidad de Sevilla. Departamento de Química Inorgánica |
Fecha de publicación | 2023 |
Fecha de depósito | 2024-05-08 |
Publicado en |
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Resumen | Methanol carbonylation was evaluated over heterogeneous catalysts based on Cu-exchanged zeolitic materials with different topology: Cu@MOR, Cu@FER, and Cu@ZSM-5. Despite the similar Si/Al ratios, it is crucial to acknowledge ... Methanol carbonylation was evaluated over heterogeneous catalysts based on Cu-exchanged zeolitic materials with different topology: Cu@MOR, Cu@FER, and Cu@ZSM-5. Despite the similar Si/Al ratios, it is crucial to acknowledge that the acid strength is influenced by the framework topology, as supported by the NH3-TPD results. This, along with other characterization techniques allowed us to estimate the impact of pore size and pore distribution in these microporous materials on catalytic performance. The channel structure influenced catalytic parameters such as conversion and selectivity. The higher methanol conversion achieved on Cu@FER shows the importance of Brønsted acid sites and redox centres location regarding the topology of the material. Concerning the selectivity, the production of acetic acid was endorsed by the 12-MR (MOR) channels, methyl acetate's production by the 10-MR (FER) channels. Finally, the presence of 6-MR (ZSM-5) channels led to a complete selectivity towards DME production. The reaction mechanism was elucidated via operando DRIFTS-MS and results revealed a bifunctional mechanism in which methanol adsorbs and dehydrates on acidic Brønsted sites and CO is activated over Cu+ species. |
Agencias financiadoras | Ministerio de Ciencia e Innovación (MICIN). España Universidad de Sevilla |
Identificador del proyecto | PID2021-126876OB-I00
MZAMBRANO-2021-198 |
Cita | Luque Álvarez, L.A., Serrano Cruz, M., González Castaño, M., Bobadilla Baladrón, L.F. y Odriozola Gordón, J.A. (2023). Impact of Topology Framework of Microporous Solids on Methanol Carbonylation: An Operando DRIFTS-MS Study. Microporous and Mesoporous Materials, 360, 112725. https://doi.org/10.1016/j.micromeso.2023.112725. |
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