Role of Delamination in Zeolite-Catalyzed Aromatic Alkylation: UCB-3 versus 3-D Al-SSZ-70

被引:19
作者
Runnehaum, Ron C. [1 ]
Ouyang, Xiaoying [1 ]
Edsinga, Jeffrey A. [1 ]
Rea, Thomas [4 ]
Arslan, Ilke [2 ]
Hwang, Son-Jong [3 ]
Zones, Stacey I. [1 ,4 ]
Katz, Alexander [1 ]
机构
[1] Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA
[2] Pacific NW Natl Lab, Richland, WA 99352 USA
[3] CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA
[4] Chevron Energy Technol Co, Richmond, CA 94804 USA
来源
ACS CATALYSIS | 2014年 / 4卷 / 07期
基金
美国国家科学基金会;
关键词
delamination; exfoliation; layered zeolite precursor; SSZ-70; MCM-22; aromatic alkylation; cymene; cumene; LAYER STRUCTURE PRESERVATION; TOLUENE; MCM-22; SELECTIVITY; LOCATION; LAMELLAR; BEHAVIOR; BENZENE;
D O I
10.1021/cs500285w
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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.
引用
收藏
页码:2364 / 2368
页数:5
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