Experimental study of the deactivation of Ni/AlMCM-41 catalyst in the direct conversion of ethene to propene
[Display omitted] •A detailed study of the deactivation and attempts of regeneration of Ni/AlMCM-41 was performed in the ETP-reaction.•Ni/AlMCM-41 could be regenerated by an oxygen treatment at temperatures lower than 350°C.•Severe deactivation of Ni/AlMCM-41 was observed at conditions where propene...
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Veröffentlicht in: | Applied catalysis. A, General General, 2017-03, Vol.533, p.121-131 |
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Format: | Artikel |
Sprache: | eng |
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•A detailed study of the deactivation and attempts of regeneration of Ni/AlMCM-41 was performed in the ETP-reaction.•Ni/AlMCM-41 could be regenerated by an oxygen treatment at temperatures lower than 350°C.•Severe deactivation of Ni/AlMCM-41 was observed at conditions where propene was the major reaction product.•Deactivation of Ni/AlMCM-41 is explained by a conjunct polymerization process as precursor of the reaction products.
In this work, an experimental study of the deactivation and regarding a possible regeneration procedure in the ETP-reaction using Ni/AlMCM-41 (Si/Al=60) was carried out. ETP experiments at different temperatures and long time on-stream were carried out. Characterization of the catalyst after experiments was performed using powder-XRD, N2-physisorption, NH3-TPD, TPO and TEM. At 250 and 350°C the catalyst did not suffer significant deactivation after 107h on-stream. Nevertheless, the yield of propene was low. A severe deactivation of the catalyst was observed at 450°C where propene was the main reaction product. Regeneration of the catalyst after 30h on-stream at temperatures lower than 350°C could be performed using a mixture of 5 vol.% oxygen in N2. The regeneration of the catalyst was not possible after 30h on-stream at 450°C. Filamentous carbon and Ni reduction are considered responsible of the deactivation of the catalyst at 450°C. The analysis of the obtained results suggests that a conjunct polymerization process takes place and is the precursor of the reaction products and the carbon species. However, a detailed study of the mechanism of the ETP-reaction should be done for a better understanding of the deactivation of Ni/AlMCM-41. |
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ISSN: | 0926-860X 1873-3875 |
DOI: | 10.1016/j.apcata.2016.12.022 |