Enhancement of Dehydrogenation and Hydride Transfer by La3+ Cations in Zeolites during Acid Catalyzed Alkane Reactions

被引:48
|
作者
Schuessler, Florian [1 ]
Schallmoser, Stefan [1 ]
Shi, Hui [1 ]
Haller, Gary L. [1 ]
Ember, Erika [1 ]
Lercher, Johannes A. [1 ]
机构
[1] Tech Univ Munich, Dept Chem, Catalysis Res Ctr, D-85747 Garching, Germany
来源
ACS CATALYSIS | 2014年 / 4卷 / 06期
关键词
alkylation; cracking; La3+ exchange; hydride transfer; C-H bond polarization; ISOBUTANE/BUTENE ALKYLATION; DEACTIVATION; LOCATION; ACTIVATION; NMR; MIGRATION; ALUMINUM; LA-139; SITE; NAY;
D O I
10.1021/cs500200k
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
La3+ cations exchanged into ultrastable zeolite Y and zeolite X promote catalytic isomerization, cracking, and alkylation of alkanes. La3+ cations stabilize the zeolite lattices and, more importantly, polarize alkane C-H bonds to enhance the rates of all three reactions. This unique activity leads to stable cracking and isomerization of reactive alkanes, with polarizable C-H bonds with adjacent tertiary or quaternary carbon atoms below 370 K. The presence of La3+ cations also enhances the zeolite catalyzed hydride transfer rate for isobutane alkylation with 2-butene leading to high catalyst stability. Solid state MAS NMR shows that the strongest positive effects are associated with nonhydroxylated La3+ cations accessible to the reacting molecules in supercages of the zeolite. The high activity is the result of a cooperative polarization of C-H bonds of alkanes by La3+ cations and the presence of stable and strong Bronsted acid sites.
引用
收藏
页码:1743 / 1752
页数:10
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