Abstract
Catalytic mechanism of ethylbenzene dehydrogenation over Fe-Co/Mg(Al)O derived from hydrotalcites has been studied based on the XAFS and XPS catalyst characterization and the FTIR measurements of adsorbed species. Fe-Co/Mg(Al)O showed synergy, whereas Fe-Ni/Mg(Al)O showed no synergy, in the dehydrogenation of ethylbenzene. Ni species were stably incorporated as Ni2+ in the regular sites in periclase and spinel structure in the Fe-Ni/Mg(Al)O. Contrarily, Co species exists as a mixture of Co3+/Co2+ in the Fe-Co/Mg(Al)O and was partially isolated from the regular sites in the structures with increasing the Co content. Co addition enhanced Lewis acidity of Fe3+ active sites by forming Fe3+-O-Co 3+/2+(1/1) bond, resulting in an increase in the activity. FTIR of ethylbenzene adsorbed on the Fe-Co/Mg(Al)O clearly showed formations of C-O bond and π-adsorbed aromatic ring. This suggests that ethylbenzene was strongly adsorbed on the Fe3+ acid sites via π-bonding and the dehydrogenation was initiated by α-H+ abstraction from ethyl group on Mg2+-O2- basic sites, followed by C-O-Mg bond formation. The α-H+ abstraction by O2-(-Mg 2+) was likely followed by β-H abstraction, leading to the formations of styrene and H2. Such catalytic mechanism by the Fe 3+ acid-O2-(-Mg2+) base couple and the Fe 3+/Fe2+ reduction-oxidation cycle was further assisted by Co3+/Co2+, leading to a good catalytic activity for the dehydrogenation of ethylbenzene. © 2011 Elsevier B.V. All rights reserved.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 118-126 |
| Number of pages | 9 |
| Journal | Applied Catalysis A: General |
| Volume | 407 |
| Issue number | 1-2 |
| DOIs | |
| State | Published - Nov 2011 |
| Externally published | Yes |
Bibliographical note
KAUST Repository Item: Exported on 2020-10-01Acknowledged KAUST grant number(s): K-C1-019-12
Acknowledgements: This publication was based on work supported by Award No. K-C1-019-12 made by King Abdullah University of Science and Technology (KAUST). The support of King Fahd University of Petroleum and Minerals (KFUPM) is also highly appreciated. The XAFS measurements at the SPring-8 were carried out by the approval (proposal No. 2010B1184) of Japan Synchrotron Radiation Research Institute (JASRI). The authors also acknowledge Japan Cooperation Center, Petroleum (JCCP) for giving the opportunity of this collaborative research.
This publication acknowledges KAUST support, but has no KAUST affiliated authors.