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基于 L-脯氨酸的深共晶溶剂(DESs)用于柴油的深度催化氧化脱硫(ODS)。

L-proline-based deep eutectic solvents (DESs) for deep catalytic oxidative desulfurization (ODS) of diesel.

机构信息

Green chemistry centre, College of Chemistry and Chemical Engineering, Yantai University, Yantai, 264005, China.

Institute of chemistry for Functionalized Materials, College of Chemistry and Chemical Engineering, Liaoning Normal University, Dalian, 116029, China.

出版信息

J Hazard Mater. 2017 Oct 5;339:216-222. doi: 10.1016/j.jhazmat.2017.06.050. Epub 2017 Jun 21.

Abstract

A series of L-proline-based DESs was prepared through an atom economic reaction between L-proline (L-Pro) and four different kinds of organic acids. The DESs were characterized by Fourier transform infrared spectroscopy (FT-IR), H nuclear magnetic resonance (HNMR), cyclic voltammogram (CV) and the Hammett method. The synthesized DESs were used for the oxidative desulfurization and the L-Pro/p-toluenesultonic acid (L-Pro/p-TsOH) system shows the highest catalytic activity that the removal of dibenzothiophene (DBT) reached 99% at 60°C in 2h, which may involve the dual activation of the L-Pro/p-TsOH. The acidity of four different L-proline-based DESs was measured and the results show that it could not simply conclude that the correlation between the acidity of DESs and desulfurization capability was positive or negative. The electrochemical measurements evidences and recycling experiment indicate a good stability performance of L-Pro/p-TsOH in desulfurization. This work will provide a novel and potential method for the deep oxidation desulfurization.

摘要

通过脯氨酸(L-Pro)与四种不同有机酸之间的原子经济性反应,制备了一系列基于脯氨酸的 DESs。通过傅里叶变换红外光谱(FT-IR)、氢核磁共振(HNMR)、循环伏安法(CV)和哈米特方法对 DESs 进行了表征。将合成的 DESs 用于氧化脱硫,L-Pro/对甲苯磺酸(L-Pro/p-TsOH)体系表现出最高的催化活性,在 60°C 下 2h 内二苯并噻吩(DBT)的去除率达到 99%,这可能涉及到 L-Pro/p-TsOH 的双重活化。测量了四种不同的基于脯氨酸的 DESs 的酸度,结果表明,不能简单地得出 DESs 的酸度与脱硫能力之间存在正相关或负相关的结论。电化学测量证据和回收实验表明,L-Pro/p-TsOH 在脱硫过程中具有良好的稳定性。这项工作为深度氧化脱硫提供了一种新颖而有潜力的方法。

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