Separation of fuel additives based on mechanism analysis and thermodynamic phase behavior

doi:10.1016/j.cjche.2023.05.015

摘要/Abstract

摘要： tert-butanol and ethyl acetate, as fuel additives and oxygenated fuels, can improve fuels quality and reduce exhaust emissions. Therefore, the recovery of these compounds from azeotropic systems is of great significance. Ionic liquids (ILs) are promising green solvents for separating azeotropic systems. In this study, an efficient extraction strategy based on 1-butyl-3-methylimidazolium acetate ([Bmim][AC]) is proposed. The mechanism by which ILs enable the separation of binary alcohol-ester azeotropes was revealed by evaluating the lowest conformational energy through combining an independent gradient model based on the Hirshfeld partition (IGMH) and frontier molecular orbitals, to preliminarily screen the extractants. The range of extractants was further reduced by a vapor–liquid phase equilibrium (VLE) experiment, and a modeling method for separating the alcohol–ester system and recovering the solvent using [Bmim][AC] and 1-ethyl-3-methyl-3-imidazolium acetate ([Emim][AC]) is established. Under the optimal operating conditions, the use of [Bmim][AC] can reduce the total annual cost (TAC) per year by 17.78%, and the emissions of CO₂, SO₂, and NO can be reduced by 10.86%. In this study, a comprehensive method for screening extractants is proposed, and the simulation process is optimized in combination with the economic and environmental impact. The results have important guiding significance for realizing efficient, energy-saving, and green azeotropic separation systems in industry.

关键词: Ionic liquids, Extraction separation, Quantum chemistry calculation, Azeotrope, Molecular simulation

Abstract: tert-butanol and ethyl acetate, as fuel additives and oxygenated fuels, can improve fuels quality and reduce exhaust emissions. Therefore, the recovery of these compounds from azeotropic systems is of great significance. Ionic liquids (ILs) are promising green solvents for separating azeotropic systems. In this study, an efficient extraction strategy based on 1-butyl-3-methylimidazolium acetate ([Bmim][AC]) is proposed. The mechanism by which ILs enable the separation of binary alcohol-ester azeotropes was revealed by evaluating the lowest conformational energy through combining an independent gradient model based on the Hirshfeld partition (IGMH) and frontier molecular orbitals, to preliminarily screen the extractants. The range of extractants was further reduced by a vapor–liquid phase equilibrium (VLE) experiment, and a modeling method for separating the alcohol–ester system and recovering the solvent using [Bmim][AC] and 1-ethyl-3-methyl-3-imidazolium acetate ([Emim][AC]) is established. Under the optimal operating conditions, the use of [Bmim][AC] can reduce the total annual cost (TAC) per year by 17.78%, and the emissions of CO₂, SO₂, and NO can be reduced by 10.86%. In this study, a comprehensive method for screening extractants is proposed, and the simulation process is optimized in combination with the economic and environmental impact. The results have important guiding significance for realizing efficient, energy-saving, and green azeotropic separation systems in industry.

Key words: Ionic liquids, Extraction separation, Quantum chemistry calculation, Azeotrope, Molecular simulation

Mengjin Zhou, Yanli Zhang, Ke Xue, Haixia Li, Zhaoyou Zhu, Peizhe Cui, Yinglong Wang, Jingwei Yang. Separation of fuel additives based on mechanism analysis and thermodynamic phase behavior[J]. 中国化学工程学报, 2023, 64(12): 168-176.

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