纳米孔道限域离子液体催化羟醛缩合过程研究

The aldol condensation of formaldehyde and propaldehyde is the critical step in the process of methyl methacrylate production from C2 and syngas. Traditional catalyst for aldol condensation has much disadvantage such as inefficiency, strongly corrosive and difficult to recycle. The ionic liquid catalyst with high efficiency needs to solve the stability and the loss in the using. High efficiency catalyst for the aldol condensation of formaldehyde and propaldehyde and the reaction mechanism research is urgent need for the development of this clean process for aldol condensation. In this project, limited nanospace ionic liquids will be designed and prepared through changing the anion type, group and the structure of cation, in order to attain the rule of the properties and the boundary dimension. The limited nanospace ionic liquids will be revised to get high efficiency catalyst for the aldol condensation of formaldehyde and propaldehyde. Combining in-suit detection method with molecular simulation, the synergistic effect and the reaction mechanism in the aldol condensation will be studied. This will give theoretical support for the critical technique to cleanly produce methylacrolein and methyl methacrylate. Also this is good for the modification of aldol-condensation catalyst and the extensive application of aldol condensation reaction in theory.

甲醛与丙醛羟醛缩合制备甲基丙烯醛是煤基合成气-C2路线清洁生产甲基丙烯酸甲酯的关键步骤。传统催化剂存在效率低、腐蚀性强及无法重复使用等问题，新型绿色离子液体高效催化剂仍存在流失和稳定性问题。设计开发高效催化剂和反应过程机理研究是推动甲基丙烯酸甲酯技术进步及羟醛缩合绿色反应过程推广应用的关键和迫切需求。本研究将通过“瓶中造船”方式制备稳定的限域离子液体催化材料，合成不同种类的限域离子液体催化剂，获得限域离子液体性能调变规律和边界尺寸，并进行以甲醛与丙醛的羟醛缩合反应为实例的催化过程研究，探索限域离子液体催化材料的构效关系；结合原位在线检测手段辅助以分子模拟，系统地研究纳米限域离子液体催化剂催化羟醛缩合反应过程的催化过程机制和可能的协同效应关系，为羟醛缩合反应高效离子液体催化剂的改进和应用推广提供新的途径，同时为通过羟醛缩合高效、绿色合成甲基丙烯醛及甲基丙烯酸甲酯清洁技术开发提供理论指导。

甲醛与丙醛羟醛缩合制备甲基丙烯醛是煤基合成气-C2路线清洁生产甲基丙烯酸甲酯的关键步骤。传统催化剂存在效率低、腐蚀性强及无法重复使用等问题，新型绿色离子液体高效催化剂仍存在流失和稳定性问题。设计开发高效催化剂和反应过程机理研究是推动甲基丙烯酸甲酯技术进步及羟醛缩合绿色反应过程推广应用的关键和迫切需求。本研究通过负载与构筑等制备稳定的限域离子液体催化材料，合成不同种类的限域离子液体催化剂，获得了限域离子液体链长调变规律和边界尺寸，并进行以甲醛与丙醛的羟醛缩合反应为实例的催化过程研究，探索限域离子液体催化材料的构效关系；结合原位在线检测手段辅助以分子模拟，研究了纳米离子液体催化剂催化羟醛缩合反应过程的催化过程机制，为羟醛缩合反应高效离子液体催化剂的改进和应用推广提供新的途径，同时为通过羟醛缩合高效、绿色合成甲基丙烯醛及甲基丙烯酸甲酯清洁技术开发提供理论指导。