Theoretical Insights into the Effect of the Framework on the Initiation Mechanism of the MTO Process

被引：47
作者：
Plessow, Philipp N. [1 ]
Studt, Felix [1 ,2 ]
机构：
[1] Karlsruhe Inst Technol, Inst Catalysis Res & Technol, Hermann von Helmholtz Pl 1, D-76344 Eggenstein Leopoldshafen, Germany
[2] Karlsruhe Inst Technol, Inst Chem Technol & Polymer Chem, D-76131 Karlsruhe, Germany
来源：
CATALYSIS LETTERS | 2018年 / 148卷 / 04期
关键词：
DFT; Theory; Processes and reactions; METHANOL-TO-OLEFIN; CARBON-CARBON BOND; SURFACE METHOXY GROUPS; DIMETHYL ETHER; HYDROCARBON FORMATION; METHYL ACETATE; ACID STRENGTH; SELECTIVE CARBONYLATION; CHEMICAL ACCURACY; HYDROGEN-TRANSFER;
D O I：
10.1007/s10562-018-2330-7
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：
In this contribution, we investigate the initiation mechanism of the methanol-to-olefins process for the different zeotype materials, H-SSZ-13, H-ZSM-5, H-BEA and H-SAPO-34 using density functional theory. While the energetics differ between these materials, variations are systematic so that the relative ordering of the barriers remains the same. We hence predict that the initiation mechanism follows an identical path in all materials with similar rate-limiting steps. We show that the observed trends that have been found for the reaction barriers can be explained by differences in acidity and van-der-Waals interactions of the materials. [GRAPHICS] .
引用
收藏
页码：1246 / 1253
页数：8
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