Development and Study of Enzyme Functional Mimics

金属催化新工艺的发展对立体选择性有机具有重要意义 这也有助于我们对金属有机化学基础知识的理解。什么时候有用的新闻 催化过程能够在低催化剂负载量下进行，在室温下进行，并直接在 商业上可获得的材料，它们可以作为整体合成工作的关键，也可以作为 生产基本有机积木的有效途径。具有这些设计的催化反应 标准是拟议研究的主题。中描述的，是一项针对 介绍了一系列新的有用的催化转化，这些转化是 立体生成的碳-硼键。中心转化是催化的烯烃二硼反应。 其提供了一种合成的多功能邻位双硼中间体。除了开发这一过程外， 我们的目标是开发二硼加合物的合成用途，以使丰富的手性官能化阵列 化合物可以不对称的方式从不饱和底物中获得。 具体目标是： (1)研制了模块化的P-N配体支架，并利用它们建立了不对称诱导模型 并扩大反应范围。 (2)开发基于涉及C-B转化的级联序列的复杂性生成反应 债券到C-X债券。 (3)开发由前手性联烯二硼引发的合成方法。 (4)发展对映体选择性氢化反应有效的手性配体结构。 乙烯基硼酸盐。

Development of novel metal-catalyzed processes has significant implications for stereoselective organic synthesis and also for our understanding of fundamental organometallic chemistry. When useful new catalytic processes are able to proceed at low catalyst loading, at room temperature and directly on commercially available materials, they can serve as a linchpin for total synthesis efforts and also as an efficient route to the production of basic organic building blocks. Catalytic reactions with these design criteria are the subject of the proposed research. Described within, is a program directed towards introducing a broad range of new and useful catalytic transformations which are the creation of stereogenic carbon-boron bonds. The centerpiece transformation is a catalytic alkene diboration reaction which provides a synthetically versatile vicinal diboron intermediate. In addition to developing this process, we aim to develop the synthetic utility of the diboron adducts such that a rich array of chiral functionalized compounds may be accessed from unsaturated substrates in an asymmetric fashion. Specific Aims are: (1) Develop modular P-N ligand scaffolds and employ them to develop a model for asymmetric induction and to improve reaction scope. (2) Develop complexity-generating reactions based on cascade sequences that involve conversion of C-B bonds to C-X bonds. (3) Develop synthetic methods that are initiated by diboration of prochiral allenes . (4) Develop chiral ligand structures that are effective for the catalytic enantioselective hydrogenation of vinylboronates .