甲基咪唑盐酸盐/草酸型低共熔溶剂的制备及其在模拟油中氧化脱硫中的应用

doi:10.11949/j.issn.0438-1157.20160330

摘要/Abstract

摘要：

通过简单加热并搅拌甲基咪唑盐酸盐和草酸的混合物合成了甲基咪唑盐酸盐/草酸（[HMIM]Cl/H₂C₂O₄）型酸性低共熔溶剂，以[HMIM]Cl/H₂C₂O₄为萃取剂和催化剂、H₂O₂为氧化剂催化氧化法脱除模拟油中的二苯并噻吩，考察不同的脱硫体系、反应温度、催化剂加入量、氧硫比、模拟油中含硫化合物类型对脱硫率的影响。实验表明，在反应温度为40℃、模拟油量为5 ml、[HMIM]Cl/H₂C₂O₄加入量为1.25 ml、O/S 12、反应时间为140 min的最佳反应条件下二苯并噻吩的脱除率可以达到92.2%。动力学分析表明，该氧化脱硫体系符合一级反应动力学方程。循环使用7次后催化剂的活性没有明显降低。

关键词: 甲基咪唑盐酸盐, [HMIM]Cl/H₂C₂O₄, 催化剂, 低共熔溶剂, 氧化, 反应动力学

Abstract:

Methylimidazole hydrochloride/oxalic acid ([HMIM]Cl/H₂C₂O₄) type deep eutectic solvent was synthesized by a simple heating and stirring mixture of methyl imidazole hydrochloride and oxalic acid. The removal of dibenzothiophene (DBT) in model oil was carried out by using[HMIM]Cl/H₂C₂O₄ as a catalyst and hydrogen peroxide as oxidant. The effect of different reaction parameters such as different desulfurization system, reaction temperature, catalyst amount, molar ratio of hydrogen peroxide to sulfur and the type of sulfur-containing compounds in oil on the desulfurization rate was investigated. The experimental results indicated that the removal rate of DBT can reach 92.2% under the optimum conditions of 5 ml model oil, 1.25 ml of[HMIM]Cl/H₂C₂O₄ and O/S mole ratio of 12 in 140 min and 40℃. The kinetics analysis showed that the oxidative desulfurization system was in accord with the first order reaction kinetics equation. The catalyst was reused for 7 times without significant decrease in activity.

Key words: methylimidazole hydrochloride, [HMIM]Cl/H₂C₂O₄, catalysts, deep eutectic solvent, oxidation, reaction kinetics

中图分类号:

TE624

侯良培, 赵荣祥, 李秀萍, 石薇薇. 甲基咪唑盐酸盐/草酸型低共熔溶剂的制备及其在模拟油中氧化脱硫中的应用[J]. 化工学报, 2016, 67(9): 3972-3980.

HOU Liangpei, ZHAO Rongxiang, LI Xiuping, SHI Weiwei. Preparation of methylimidazole hydrochloride/oxalic acid type deep eutectic solvent and its application in oxidative desulfurization of model oil[J]. CIESC Journal, 2016, 67(9): 3972-3980.

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