Ni as the promoter on hydrogen spillover for better hydrogenative regeneration on Pt/Y based catalysts
For (Ni-Pt)/YA catalyst, the apparent active energy is approximately equal to that of hydrogen spillover (11.9 kal/mol), which is almost 30% lower than that of Pt/YA (17.3 kal/mol). [Display omitted] •H2 activation was divided into H2 dissociation and hydrogen spillover.•Ni increased the capability...
Gespeichert in:
Veröffentlicht in: | Fuel (Guildford) 2023-03, Vol.335, p.127047, Article 127047 |
---|---|
Hauptverfasser: | , , , , |
Format: | Artikel |
Sprache: | eng |
Schlagworte: | |
Online-Zugang: | Volltext |
Tags: |
Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
|
Zusammenfassung: | For (Ni-Pt)/YA catalyst, the apparent active energy is approximately equal to that of hydrogen spillover (11.9 kal/mol), which is almost 30% lower than that of Pt/YA (17.3 kal/mol).
[Display omitted]
•H2 activation was divided into H2 dissociation and hydrogen spillover.•Ni increased the capability of H2 activation over (Ni-Pt)/YA experimentally.•Ni was selected as the promoter on hydrogen spillover theoretically.•With much less Pt, (5Ni-0.1Pt)/YA could completely be regenerated over 10 circles.
Hydrogenative regeneration of Pt/YA catalysts is vital to continuous operation of solid acid isobutane/butene alkylation. From the view of H2 activation, the mechanism of hydrogenative regeneration was investigated experimentally and theoretically. Herein with Pt/YA as reference, (Ni-Pt)/YA catalysts were prepared with almost identical cell parameter and different Ni/Pt contents by wet impregnation method following by several characterization methods, such as XPS, H2-TPR, H2-TPD, STEM-CS and Elemental mapping. Strong interactions between Ni and Pt were proven by XPS and H2-TPR. Moreover Ni can increase the capability of hydrogen spillover, which could be observed by H2-TPD, with the higher desorption temperature and more desorbed H2. DFT calculations revealed that hydrogen spillover is the rate determining step for the overall H2 activation over Pt/YA, and Ni as the hydrogen spillover promoter could couple with Pt to enhance the overall H2 activation because of almost 30% lower energy barrier for hydrogen spillover. With rather low Pt content, no obvious loss in lifetime in the 10 cycles of reaction-regeneration was observed over (5Ni-0.1Pt)/YA with rather stable product distribution. |
---|---|
ISSN: | 0016-2361 1873-7153 |
DOI: | 10.1016/j.fuel.2022.127047 |