Role of Delamination in Zeolite-Catalyzed Aromatic Alkylation: UCB‑3 versus 3‑D Al-SSZ-70
Abstract
Delaminated zeolite UCB-3 exhibits 2.4-fold greater catalytic activity relative to its three-dimensional (3D) zeolite counterpart, Al-SSZ-70, and 2.0-fold greater activity (per catalyst mass) when compared with industrial catalyst MCM-22, for the alkylation of toluene with propylene at 523 K. The former increase is nearly equal to the observed relative increase in external surface area and acid sites upon delamination. However, at 423 K for the same reaction, UCB-3 exhibits a 3.5-fold greater catalytic activity relative to 3D Al-SSZ-70. The higher relative rate enhancement for the delaminated material at lower temperature can be elucidated on the basis of increased contributions from internal acid sites. Evidence of possible contributions from such acid sites is obtained by performing catalysis after silanation treatment, which demonstrates that although virtually all catalysis in MCM-22 occurs on the external surface, catalysis also occurs on internal sites for 3D Al-SSZ-70. The additional observed enhancement at low temperatures can therefore be rationalized by greater access to internal active sites as a result of sheet breakage during delamination. Such breakage leads to shorter characteristic internal diffusion paths and was visualized using TEM comparisons of UCB-3 and 3D Al-SSZ-70.
Additional Information
© 2014 American Chemical Society. Received: March 13, 2014. Revised: May 19, 2014. Publication Date (Web): June 3, 2014. We are grateful to the Management and Transfer of Hydrogen via the Catalysis Program funded by Chevron Corporation for financial support. The NMR facility at Caltech was supported by the National Science Foundation (NSF) under Grant No. 9724240 and in part by the MRSEC Program of the NSF under Award No. DMR-520565. The STEM facility and research were funded by the Laboratory Directed Research and Development program at the Pacific Northwest National Laboratory. PNNL is operated by Battelle for the U.S. Department of Energy under Contract DE-AC05-76RL01830.Attached Files
Supplemental Material - cs500285w_si_001.pdf
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Additional details
- Eprint ID
- 48638
- DOI
- 10.1021/cs500285w
- Resolver ID
- CaltechAUTHORS:20140818-083734548
- Chevron Corporation
- NSF
- DMR-9724240
- NSF
- DMR-520565
- Pacific Northwest National Laboratory (PNNL) Laboratory Directed Research and Development program
- Department of Energy (DOE)
- DE-AC05-76RL01830
- Created
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2014-08-19Created from EPrint's datestamp field
- Updated
-
2021-11-10Created from EPrint's last_modified field