Influence of Topology and Bronsted Acid Site Presence on Methanol Diffusion in Zeolites Beta and MFI

被引:17
作者
Botchway, Cecil H. [1 ,2 ]
Tia, Richard [1 ]
Adei, Evans [1 ]
O'Malley, Alexander J. [3 ]
Dzade, Nelson Y. [2 ]
Hernandez-Tamargo, Carlos [2 ,4 ]
de Leeuw, Nora H. [2 ,5 ]
机构
[1] Kwame Nkrumah Univ Sci & Technol, Dept Chem, Kumasi 1916, Ghana
[2] Cardiff Univ, Sch Chem, Main Bldg, Cardiff CF10 3AT, Wales
[3] Univ Bath, Dept Chem, Bath BA2 7AY, Avon, England
[4] Indian Inst Technol Madras, Dept Chem, Natl Ctr Catalysis Res, Chennai 600036, Tamil Nadu, India
[5] Univ Leeds, Sch Chem, Leeds LT2 9JT, W Yorkshire, England
基金
英国自然环境研究理事会; 英国工程与自然科学研究理事会;
关键词
methanol diffusion; zeolites; molecular dynamics; MTH reactions; ELASTIC NEUTRON-SCATTERING; DIMETHYL ETHER; MOLECULAR-DYNAMICS; SHAPE SELECTIVITY; COKE FORMATION; HYDROCARBONS; CONVERSION; ADSORPTION; ZSM-5; CATALYSTS;
D O I
10.3390/catal10111342
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
Detailed insight into molecular diffusion in zeolite frameworks is crucial for the analysis of the factors governing their catalytic performance in methanol-to-hydrocarbons (MTH) reactions. In this work, we present a molecular dynamics study of the diffusion of methanol in all-silica and acidic zeolite MFI and Beta frameworks over the range of temperatures 373-473 K. Owing to the difference in pore dimensions, methanol diffusion is more hindered in H-MFI, with diffusion coefficients that do not exceed 10x10-10 m2s-1. In comparison, H-Beta shows diffusivities that are one to two orders of magnitude larger. Consequently, the activation energy of translational diffusion can reach 16 kJ center dot mol(-1) in H-MFI, depending on the molecular loading, against a value for H-Beta that remains between 6 and 8 kJ center dot mol(-1). The analysis of the radial distribution functions and the residence time at the Bronsted acid sites shows a greater probability for methylation of the framework in the MFI structure compared to zeolite Beta, with the latter displaying a higher prevalence for methanol clustering. These results contribute to the understanding of the differences in catalytic performance of zeolites with varying micropore dimensions in MTH reactions.
引用
收藏
页码:1 / 18
页数:18
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