Methanol-Alkene Reactions in Zeotype Acid Catalysts: Insights from a Descriptor-Based Approach and Microkinetic Modeling

被引：80

作者：

Brogaard, Rasmus Y. ^{[1
,2
,4
]}

Wang, Chuan-Ming ^{[1
,2
,3
]}

Studt, Felix ^{[1
,2
]}

机构：

[1] SLAC Natl Accelerator Lab, SUNCAT Ctr Interface Sci & Catalysis, Menlo Pk, CA 94025 USA

[2] Stanford Univ, Dept Chem Engn, Stanford, CA 94305 USA

[3] SINOPEC, Shanghai Res Inst Petrochem Technol, Shanghai 201208, Peoples R China

[4] Univ Oslo, Dept Chem, inGAP Ctr Res Based Innovat, N-0315 Oslo, Norway

来源：

ACS CATALYSIS | 2014年 / 4卷 / 12期

基金：

美国国家科学基金会;

关键词：

acid catalysis; porous materials; density functional theory; ammonia adsorption; scaling relations; alkene methylation; methanol-to-hydrocarbon conversion; METHYLATION REACTIONS; REACTION-MECHANISMS; DIMETHYL ETHER; N-ALKANES; AB-INITIO; ZEOLITE; REACTIVITY; CONVERSION; STRENGTH; SITES;

D O I：

10.1021/cs5014267

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：

We recently proposed the ammonia heat of adsorption as a reactivity descriptor in solid acid catalysis, using it to predict the activity of zeotype catalysts in the propene methanol reaction (J. Phys. Chem. Lett. 2014, 5, 1516-1521). Here we extend the approach to a series of alkene reactants, establishing transition state energy scaling relations for ethene and butenes. Using these relations in connection with microkinetic modeling, we predict a change in reaction pathway as a function of acid-site reactivity and alkene size. The results illustrate the potential of the descriptor-based approach to model acid-catalyzed reactions and efficiently screen for improved solid acid catalysts.

引用

页码：4504 / 4509

页数：6

共 54 条

[1] Ru-Pt core-shell nanoparticles for preferential oxidation of carbon monoxide in hydrogen [J].