二维主体层板拓扑转变制备负载型金属催化剂介尺度表界面结构的构筑与调控

The exploration of the formation mechanism of the mesoscopic behavior and the accurate description and the directional control of the mesoscopic behavior become the edge focus in the fields of the process industry and complexity science. The work mainly focuses on the preparation of highly dispersive supported metal catalysts and the control of the mesoscopic interfaces structure by the precursor methods using layered double hydroxides (LDHs) or intercalated structure. The mesoscopic interfaces, including the interfaces between metal active site and the oxide supports, and the interfaces between metal active site and the metal promoter, are formed by controlling the topological transformation process of two dimensional LDH materials. The general rules of the formation mechanism and the accurate control of mesoscopic interfaces are to be discussed in detail to realize the high activity, high selectivity and good stability of the novel supported metal catalysts. The most important purposes of this research are to elucidate the confinement effects including lattice confinement, interface confinement and space confinement, and the synergistic effect including electron coupling and electron migration during the topological transformation process towards the mesoscopic interfaces control, which are supposed to supply the experimental and theoretical directions for controlling the mesoscopic behavior in heterogeneous catalysis.

探索多相反应过程中介尺度行为的形成机理、实现其科学定量描述与定向调控已成为过程工业发展和复杂性科学研究共同的前沿。针对石脑油催化重整、合成气制备高级醇以及生物质高效转化液体烷烃等重要资源高值化反应，采用含活性组分的层状及超分子插层结构的层状双金属氢氧化物（LDHs）前驱体法制备多级结构高分散负载型催化剂，构筑金属活性位与载体及助剂金属基元介尺度表界面结构，深入研究二维主体层板拓扑转变过程中的表界面介结构形成机理，以实现负载型金属催化剂的表界面结构的有效控制，定向调控反应实现了高活性、高选择性、高稳定性。揭示“限域效应”，晶格限域、界面限域以及空间限域等，以及“协同效应”，电子耦合、电子转移等与表界面结构的科学关联，为控制多相反应介尺度行为提供实验及理论上的指导性依据。

本项目重点针对合成气定向转化乙醇及高级醇、低碳烷烃催化脱氢制烯烃等重要石油化工反应以及5-羟甲基糠醛转化为呋喃基生物燃料等生物质转化过程，提出利用具有晶格定位作用的层状结构实现催化剂多级结构控制的研究思路量体裁衣地发展了负载型单原子分散Pt基及高分散Co、CoGa等负载型金属催化材料，深入研究了表界面介尺度结构的形成机理与反应的定向调控，取得了突破性进展。项目实现了二维主体层板拓扑转变过程中，负载型金属催化剂介尺度表界面结构的构筑与调控，重点研究了表界面金属活性相在载体上的分散结构的形成以及控制机制，研究表明，高分散结构的形成和调控依赖于二维拓扑转变过程中的晶格定位效应以及晶格诱导效应。