A theoretical investigation of the methylation of alkenes with methanol over acidic zeolites

被引：74

作者：

Svelle, S

Arstad, B

Kolboe, S

Swang, O

机构：

[1] Univ Oslo, Dept Chem, N-0315 Oslo, Norway

[2] SINTEF Appl Chem, Dept Hydrocarbon Proc Chem, N-0134 Oslo, Norway

来源：

JOURNAL OF PHYSICAL CHEMISTRY B | 2003年 / 107卷 / 35期

关键词：

D O I：

10.1021/jp022201q

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：

A quantum chemical investigation of the methylation of alkenes by methanol over acidic zeolite catalysts has been performed. A cluster model consisting of four tetrahedrally coordinated atoms (T-atoms) has been used to represent the zeolite. The activation barrier for methylation is dependent on the size and substitution pattern of the alkene reactant. The results can be rationalized by considering the relative energies of the carbocations that describe the reaction path. Implications for methanol-to-hydrocarbon chemistry are discussed. The effect of zeolite acidity on the activation barrier has also been probed. The barrier decreases when the catalyst acidity is increased.

引用

页码：9281 / 9289

页数：9

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