Microstructures of the Sulfonic Acid-Functionalized Ionic Liquid/Sulfuric Acid and Their Interactions: A Perspective from the Isobutane Alkylation

被引:29
作者
Zheng, Weizhong [1 ]
Huang, Chizhou [1 ]
Sun, Weizhen [1 ]
Zhao, Ling [1 ]
机构
[1] East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China
基金
中国国家自然科学基金;
关键词
MOLECULAR-DYNAMICS SIMULATIONS; SULFURIC-ACID; FORCE-FIELD; AB-INITIO; CATALYTIC PERFORMANCE; VIBRATIONAL-SPECTRA; BISULFATE ION; LIQUIDS; IMIDAZOLIUM; OLEFINS;
D O I
10.1021/acs.jpcb.7b09755
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
The all-atom force field for concentrated sulfuric acid (98.30 wt %) was developed in this work based on ab initio calculations. The structural and dynamical properties of sulfuric acid and the mixing behaviors of sulfuric acid with ionic liquids (ILs), i.e., SFIL (1-methyl-3-(propyl-3-sulfonate) imidazolium bisulfate ([PSMim][HSO4])) and non-SFIL (1-methyl-3-propyl imidazolium bisulfate ([PMim] [HSO4])), were investigated using a molecular dynamics simulation. For sulfuric acid, most H3O+ ions were found beside HSO4- ions, forming a contact ion pair with the HSO4- ions, and three-dimensional hydrogen-bonding networks existed in the sulfuric acid. Analyses indicate that both ILs could be miscible with sulfuric acid with a strong exothermic character. The new strong interaction site between the sulfonic acid group of SFIL and an H2SO4 molecule through a strong hydrogen-bonding interaction was observed, which was beneficial to the catalytic activity and stability of the sulfuric acid. This observation is in good agreement with the experimental results that indicate SFILs could enhance the reusability of sulfuric acid for the isobutane alkylation about 4-fold compared to that of non-SFILs. Hopefully this work will provide insights into the screening and designing of new isobutane alkylation catalysts based on sulfuric acid and SFILs.
引用
收藏
页码:1460 / 1470
页数:11
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