Influences of the confinement effect and acid strength of zeolite on the mechanisms of Methanol-to-Olefins conversion over H-ZSM-5: A theoretical study of alkenes-based cycle
文献类型：期刊论文
| 作者 | Zhang, Wenna2,3; Chu, Yueying1; Wei, Yingxu2; Yi, Xianfeng1,3; Xu, Shutao2; Huang, Jindou2; Zhang, Mozhi2,3; Zheng, Anmin1; Deng, Feng1; Liu, Zhongmin2 |
| 刊名 | MICROPOROUS AND MESOPOROUS MATERIALS
 |
| 出版日期 | 2016-09-01 |
| 卷号 | 231页码:216-229 |
| 关键词 | Methanol-to-olefins Conversion Zeolite Catalysts Reaction Mechanism Confinement Effect Acid Strength Density Functional Theory |
| ISSN号 | 1387-1811 |
| DOI | 10.1016/j.micromeso.2016.05.029 |
| 文献子类 | Article |
| 英文摘要 | Methanol-to-Olefins (MTO) conversion over acidic zeolite catalysts has become the most important non petrochemical route for the production of light olefins. The 'dual-cycle' mechanism (i.e., alkenes-based cycle and aromatics-based cycle) over H-ZSM-5 zeolite has been generally accepted for olefins generation from methanol conversion. However, the relationship between the catalytic performance and the confinement effect/acid strength of the catalyst is still unclear. Herein, the methylation, isomerization and cracking processes involved in the alkenes-based cycle are discussed in-depth by density functional theory (DFT) calculations. The calculation results predicted that the transition states can be considerably stabilized by the van der Waals (vdW) interactions from the zeolite framework, resulting in the reduction of the activation barriers. And acid strength can also enhance the reaction activities. However, the catalytic reactivity of all elementary steps in the alkenes-based cycle can be improved at a different degree with increasing the acid strength. In addition, the ethene formation, transformation and the precursor of ethene formation need higher energy. And increasing acid strength can sharply decrease the activation barriers of ethene formation of cracking reaction, indicating that ethene formation may need strong acid strength. (C) 2016 Elsevier Inc. All rights reserved. |
| WOS关键词 | CATALYZED METHYLATION REACTIONS ; HYDROCARBON POOL MECHANISM ; CO-REACTION ; ISOMORPHOUS SUBSTITUTION ; SHAPE-SELECTIVITY ; DIMETHYL ETHER ; CARBENIUM IONS ; ZSM-5 ZEOLITE ; CRACKING ; KINETICS |
| WOS研究方向 | Chemistry ; Science & Technology - Other Topics ; Materials Science |
| 语种 | 英语 |
| WOS记录号 | WOS:000379705800024 |
| 出版者 | ELSEVIER SCIENCE BV |
| 源URL | [http://cas-ir.dicp.ac.cn/handle/321008/170420]  |
| 专题 | 大连化学物理研究所_中国科学院大连化学物理研究所 |
| 通讯作者 | Zheng, Anmin; Liu, Zhongmin |
| 作者单位 | 1.Chinese Acad Sci, Inst Phys & Math, Natl Ctr Magnet Resonance Wuhan, State Key Lab Magnet Resonance & Atom Mol Phys, Wuhan 430071, Peoples R China 2.Chinese Acad Sci, Dalian Inst Chem Phys, iChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Lab Methanol Olefins,Dalian Natl Lab Cl, Dalian 116023, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China |
| 推荐引用方式 GB/T 7714 | Zhang, Wenna,Chu, Yueying,Wei, Yingxu,et al. Influences of the confinement effect and acid strength of zeolite on the mechanisms of Methanol-to-Olefins conversion over H-ZSM-5: A theoretical study of alkenes-based cycle[J]. MICROPOROUS AND MESOPOROUS MATERIALS,2016,231:216-229. |
| APA | Zhang, Wenna.,Chu, Yueying.,Wei, Yingxu.,Yi, Xianfeng.,Xu, Shutao.,...&Liu, Zhongmin.(2016).Influences of the confinement effect and acid strength of zeolite on the mechanisms of Methanol-to-Olefins conversion over H-ZSM-5: A theoretical study of alkenes-based cycle.MICROPOROUS AND MESOPOROUS MATERIALS,231,216-229. |
| MLA | Zhang, Wenna,et al."Influences of the confinement effect and acid strength of zeolite on the mechanisms of Methanol-to-Olefins conversion over H-ZSM-5: A theoretical study of alkenes-based cycle".MICROPOROUS AND MESOPOROUS MATERIALS 231(2016):216-229. |
入库方式： OAI收割
来源：大连化学物理研究所
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