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Title: 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.

Authors:
; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1171888
Report Number(s):
PNNL-SA-105047
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
ACS Catalysis, 4(7):2364-2368
Additional Journal Information:
Journal Name: ACS Catalysis, 4(7):2364-2368
Country of Publication:
United States
Language:
English
Subject:
delamination; exfoliation; layered zeolite precursor; SSZ-70; MCM-22; aromatic alkylation; cymene; cumene

Citation Formats

Runnebaum, Ron C., Ouyang, Xiaoying, Edsinga, Jeffrey A., Rea, Thomas, Arslan, Ilke, Hwang, Son-Jong, Zones, Stacey I., and Katz, Alexander. Role of Delamination in Zeolite-Catalyzed Aromatic Alkylation: UCB-3 versus 3-D Al-SSZ-70. United States: N. p., 2014. Web. doi:10.1021/cs500285w.
Runnebaum, Ron C., Ouyang, Xiaoying, Edsinga, Jeffrey A., Rea, Thomas, Arslan, Ilke, Hwang, Son-Jong, Zones, Stacey I., & Katz, Alexander. Role of Delamination in Zeolite-Catalyzed Aromatic Alkylation: UCB-3 versus 3-D Al-SSZ-70. United States. doi:10.1021/cs500285w.
Runnebaum, Ron C., Ouyang, Xiaoying, Edsinga, Jeffrey A., Rea, Thomas, Arslan, Ilke, Hwang, Son-Jong, Zones, Stacey I., and Katz, Alexander. Thu . "Role of Delamination in Zeolite-Catalyzed Aromatic Alkylation: UCB-3 versus 3-D Al-SSZ-70". United States. doi:10.1021/cs500285w.
@article{osti_1171888,
title = {Role of Delamination in Zeolite-Catalyzed Aromatic Alkylation: UCB-3 versus 3-D Al-SSZ-70},
author = {Runnebaum, Ron C. and Ouyang, Xiaoying and Edsinga, Jeffrey A. and Rea, Thomas and Arslan, Ilke and Hwang, Son-Jong and Zones, Stacey I. and Katz, Alexander},
abstractNote = {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.},
doi = {10.1021/cs500285w},
journal = {ACS Catalysis, 4(7):2364-2368},
number = ,
volume = ,
place = {United States},
year = {2014},
month = {7}
}