新型单原子钯催化剂的制备及在sp2 C-H活化反应中的应用

单原子催化因其催化的高效性及兼具均相和非均相催化特性而成为催化研究领域的前沿方向之一，在甲烷、二氧化碳等小分子的惰性键活化转化中表现出优越的催化性能，有望拓展应用于芳烃碳氢活化、C-杂键的构建，成为芳烃高效催化转化的新策略，而目前尚未有文献报导。本项目拟以芳烃Csp2活化为重点，围绕“单原子催化剂表界面局域原子与高效定向Csp2活化区域之间的作用规律”这一科学问题，深入开展石墨烯负载单原子钯催化剂的设计、制备与高选择性碳氢键活化及催化机理研究：1.以催化剂的精准设计与构建为关键控制点，探讨光化学制备负载均匀、载量较大和分布可控的单原子钯催化剂的方法；2.以苯基间位碳氢高选择性活化为研究对象，开展底物分子在单原子钯催化剂表面作用机制和调控规律的研究；3. 将形成的成键规律用于指导具有高生物活性的嘌呤类化合物的高效制备，为基于C-H键活化的定向合成新型嘌呤类化合物提供新型高效催化方法。

Single atom catalysis has become one of the frontiers in the field of catalytic research because of its catalytic performance and both homogeneous and heterogeneous catalytic properties. The inert bond activation conversion of small molecules, such as methane and carbon dioxide, shows excellent catalytic performance. It is expected to be applied to the construction of C-heterogeneity bonds of aromatics activated by hydrocarbon, and become a new strategy for the efficient catalytic conversion of aromatics. However, there has not been any relevant report. This project is intended to focus on the activation of Csp2 at the aromatic site. The design of graphene supported monoatomic palladium catalyst was carried out, focusing on the scientific problem of "the interaction between the local atoms at the surface of the monatomic catalyst and the high efficiency oriented Csp2 activation region". Study on preparation and highly selective hydrocarbon bond activation and catalytic mechanism. 1. Taking the precise design and construction of catalyst as the key control point, the method of preparing monoatomic palladium catalyst with uniform loading, large load and controllable distribution was discussed. 2. The mechanism and regulation of substrate molecules acting on the surface of monoatomic palladium catalyst were studied. 3. The bond formation rule is used to guide the efficient preparation of purine compounds with high biological activity, and to provide a new efficient catalytic strategy for the directional synthesis of new purine compounds based on C-H bond activation.