Issue 10, 2013

Effect of superficial velocity on the coking behavior of a nanozeolite-based Mo/HZSM-5 catalyst in the non-oxidative CH4 dehydroaromatization at 1073 K

Abstract

The lifetime benzene and naphthalene productivity of a nanosized zeolite-based 5%Mo/HZSM-5 catalyst in the non-oxidative CH4 dehydroaromatization has been investigated at 1073 K and three different space velocities (4500, 10 000 and 30 000 mL g−1 h−1, corresponding to the superficial velocities 1.3, 3.0, and 9.0 cm s−1, respectively). The aim is to demonstrate that diffusion limitations do exist and have a strong influence on the coking behaviour and the lifetime aromatics productivity. The results showed that the catalyst deactivation rate increased with increasing CH4 superficial velocity, leading to decreased productivity. On the other hand, TPO and BET measurements of the spent samples revealed that the amount of coke accumulated in the spent samples decreased with increasing velocity, whereas their microporosity varied essentially depending upon the coke amount. Putting these observations together thus leads to a fact that less coke forms at a higher velocity but results in a more rapid deactivation and reduced productivity. As this may suggest the occurrence of non-uniform coke formation across catalyst particles, physical powdering of all spent samples and re-evaluation of the activity of all powdered samples were conducted to confirm this. It was found that the benzene formation activities of all powdered samples exhibited considerable but different degrees of recovery, and the most rapidly deactivated sample provided the greatest recovery. Thus, it is reasonably concluded that the preferential coke formation in the near-surface outer layers of catalyst particles and/or of crystal agglomerates inside the particles does occur in the nanozeolite-based catalyst at the test superficial velocities, particularly at 30 000 mL g−1 h−1. The essential cause for this occurrence is discussed in detail in the article.

Graphical abstract: Effect of superficial velocity on the coking behavior of a nanozeolite-based Mo/HZSM-5 catalyst in the non-oxidative CH4 dehydroaromatization at 1073 K

Article information

Article type
Paper
Submitted
07 May 2013
Accepted
31 Jul 2013
First published
31 Jul 2013

Catal. Sci. Technol., 2013,3, 2769-2777

Effect of superficial velocity on the coking behavior of a nanozeolite-based Mo/HZSM-5 catalyst in the non-oxidative CH4 dehydroaromatization at 1073 K

Y. Xu, Y. Song, Y. Suzuki and Z. Zhang, Catal. Sci. Technol., 2013, 3, 2769 DOI: 10.1039/C3CY00320E

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements