功能化酸性低共熔剂催化氧化柴油深度脱硫的研究

Deep desulfurization of diesel is an urgent research topic in the world. Catalytic oxidative desulfurization in the ionic liquids is one of the most promising desulfurization process. However, ionic liquids technologies for large scale application still shows some limitations in terms of poor biodegradability and expensiveness. The functional acidic deep eutectic solvents are green, environmentally friendly and inexpensive. They do not only share extraction performance of traditional low ionic liquids, but also exhibit high a catalytic oxidative desulfurization activity. In this project, a series of functional acidic deep eutectic solvents will be prepared for oxidative desulfurization of diesel. The organic acids and their derivatives are used as hydrogen bond donor, the quaternary amines or quaternary phosphorus compounds are used as hydrogen bond acceptors. The desulfurization process will be investigated by mordern spectroscopic characterization methods and Density Functional Theory. The influence of composition and structure of functional acidic deep eutectic solvents on the catalytic activity is studied. The reaction mechanism will be studied to provide a theoretical basis for controlled synthesis and applications. It has scientific significance for the development of desulfurization technology of diesel.

柴油的深度脱硫是全球范围内急需解决的一个重要课题。功能化离子液体催化氧化是实现柴油深度脱硫最有前景的工艺之一。然而，离子液体生物降解性较差、价格昂贵，严重制约了该脱硫工艺的发展。功能化酸性低共熔剂绿色环保，价格低廉，既具有传统离子液体的萃取性能，又具有催化氧化脱硫的能力。本项目拟采用有机酸及其衍生物为氢键供体，季铵类或季磷类化合物为氢键受体，合成系列功能化酸性低共熔剂，并考察其催化氧化柴油深度脱硫的性能。运用现代波谱技术等表征手段，结合密度泛函理论对脱硫过程中功能化酸性低共熔剂和有机硫化物的变化进行系统分析，关联其组成、结构与催化性能，为其可控合成和应用提供理论依据。揭示功能化酸性低共熔剂催化氧化柴油深度脱硫的反应机理。本研究工作的开展，为柴油的深度氧化脱硫开拓了新的思路，对于深入理解柴油氧化脱硫的本质，推动柴油深度脱硫工艺的发展具有科学的指导意义。

柴油的深度脱硫是世界范围内急需解决的一个重要研究课题。氧化脱硫是实现柴油深度脱硫最有前景的工艺之一。本课题开发了多种类型的离子液体及酸性低共熔溶剂催化氧化脱硫体系，特别是构建了低共熔溶剂仿生催化体系，对柴油进行深度氧化脱硫的研究，取得了较好的进展。运用现代波谱技术等表征手段对脱硫过程中有机硫化物的变化进行系统分析，揭示了低共熔溶剂仿生体系活化氧气和电子转移的反应机理。另外，我们还研究了二氧化碳的环加成反应，生物质的催化转化等反应以及分子筛的制备与催化性能，均取得较好的结果。