Kinetics and thermodynamics of polymethylbenzene formation over zeolites with different pore sizes for understanding the mechanisms of methanol to olefin conversion - a computational study
文献类型:期刊论文
作者 | Chen, Yan-Yan1; Wei, Zhihong1; Wang, Sen1,2; Li, Junfen1; Dong, Mei1; Qin, Zhangfeng1; Wang, Jianguo1; Jiao, Haijun1,3; Fan, Weibin1 |
刊名 | Catalysis science & technology
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出版日期 | 2016 |
卷号 | 6期号:14页码:5326-5335 |
ISSN号 | 2044-4753 |
DOI | 10.1039/c6cy00465b |
通讯作者 | Jiao, haijun(haijun.jiao@catalysis.de) ; Fan, weibin(fanwb@sxicc.ac.cn) |
英文摘要 | On the basis of density functional theory including dispersion correction (omega b97xd), the thermodynamics and kinetics of the formation of polymethylbenzene intermediates in methanol to olefin conversion over zeolites with different pore sizes have been systematically computed. the agreement between the experimental and theoretical adsorption enthalpies of the several polymethylbenzenes over h-fau reasonably validates the applied models and methods, and reveals the importance of dispersion correction in the space confinement and electrostatic stabilization of the zeolite framework. the free energies of the step-wise formation of the polymethylbenzenes show that the most favorable active hydrocarbon pool intermediates are pentamethylbenzene and hexamethylbenzene over h-bea and h-sapo-34, as well as tetra-methylbenzene over h-zsm-5 and h-zsm-22. these stable polymethylbenzenes are also precursors for the formation of geminal methylated cationic intermediates on the basis of kinetic and thermodynamic analyses. the agreement of the thermodynamic and kinetic results on the favorable intermediates validates the use of gibbs free reaction energies to estimate the primary component of the intermediates in the various zeolites. all these pore-size-dependent differences among the zeolites show their enhanced confinement effect, which is mainly influenced by the short-range electrostatic potential including stabilization and repulsion. |
WOS关键词 | TO-HYDROCARBONS REACTION ; BRONSTED ACID SITES ; AROMATIC-HYDROCARBONS ; HEPTAMETHYLBENZENIUM CATION ; THEORETICAL INSIGHTS ; SHAPE-SELECTIVITY ; CARBENIUM IONS ; MTO REACTION ; CO-REACTION ; H-BETA |
WOS研究方向 | Chemistry |
WOS类目 | Chemistry, Physical |
语种 | 英语 |
WOS记录号 | WOS:000379438000009 |
出版者 | ROYAL SOC CHEMISTRY |
URI标识 | http://www.irgrid.ac.cn/handle/1471x/2374585 |
专题 | 中国科学院大学 |
通讯作者 | Jiao, Haijun; Fan, Weibin |
作者单位 | 1.Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Shanxi, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Univ Rostock, Leibniz Inst Katalyse eV, Albert Einstein Str 29A, D-18059 Rostock, Germany |
推荐引用方式 GB/T 7714 | Chen, Yan-Yan,Wei, Zhihong,Wang, Sen,et al. Kinetics and thermodynamics of polymethylbenzene formation over zeolites with different pore sizes for understanding the mechanisms of methanol to olefin conversion - a computational study[J]. Catalysis science & technology,2016,6(14):5326-5335. |
APA | Chen, Yan-Yan.,Wei, Zhihong.,Wang, Sen.,Li, Junfen.,Dong, Mei.,...&Fan, Weibin.(2016).Kinetics and thermodynamics of polymethylbenzene formation over zeolites with different pore sizes for understanding the mechanisms of methanol to olefin conversion - a computational study.Catalysis science & technology,6(14),5326-5335. |
MLA | Chen, Yan-Yan,et al."Kinetics and thermodynamics of polymethylbenzene formation over zeolites with different pore sizes for understanding the mechanisms of methanol to olefin conversion - a computational study".Catalysis science & technology 6.14(2016):5326-5335. |
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来源:中国科学院大学
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