钯催化下甲苯类酰化试剂参与的邻位和间位C-H酰基化反应

C-H键酰基化反应可简易高效制备具有生物或药理活性的二芳（杂环）酮类化合物。但目前反应新底物的开发十分有限，仅限于少量具有邻位导向基团的C-H键活化底物制备邻位取代芳酮的研究，无法提供结构多样化的二芳（杂环）酮物质。大量新型高效C-H键活化底物尤其是具有间位导向基团的C-H键活化底物相关酰基化反应研究亟需开发。申请人前期研究中发现甲苯类物质可作为酰化试剂绿色高效地参与C-H键酰基化反应，但应用范围和反应机理均有待深入探索。在项目组已有工作基础上，拟系统化开展钯催化下新型C-H键活化底物与甲苯类酰化试剂的C-H键酰基化反应研究，重点研究具有间位导向基团底物参与的间位C-H键酰基化反应，深入探索反应机理及产物转化为生物活性物质的途径。本项目通过系统化研究，将实现间位C-H键酰基化反应，并扩展邻位C-H键酰基化反应的应用范围，寻找反应普适性规律及机理，为芳（杂）酮类化合物提供高效和绿色的合成方法

Benzophenone derivatives or hetero-aromatic ketones are important structural motifs in natural products and pharmaceutical useful products. Direct C-H bond acylations promoted by palladium have been successful as a valuable tool for their modular and facile synthesis. However, the research limited to the ortho-C-H bond acylations and couldn’t provide benzophenone derivatives or hetero-aromatic ketones with diversified structure. Many substrates widely used in C-H bonds activation have not been involved in the C-H bond acylations yet, especially those with remote meta-C-H directing groups. Our previous works proved that toluene derivatives could be used in the C-H bond acylation as a green and efficient acylation agent, but the scope and the mechanism have not been explored clearly yet..Based on our previous work and the limitation in C-H bond acylations, this project we design will be the research of palladium catalyzed C-H bond acylations with new C-H activated substrates, focusing on the meta-C-H bond acylations using substrates with meta-C-H directing groups. We also will explore the mechanism and the transformed way of final product to natural or pharmaceutical useful products. We hope this project will succeed in meta-C-H bond acylations, broadening the application of C-H bond acylations, giving an explanation of the mechanism, providing an "atom efficiency" and "green" way for the synthesis of benzophenone derivatives or hetero-aromatic ketones.