New Silacyclic Platforms for Complex Target Synthesis

描述（由申请人提供）：主要强调创新，该计划的主要目标是利用现成的硅环平台开发高效，完全立体控制和实用的合成策略来复杂的生物活性目标。硅环戊烷和硅环己烷通过对映选择性去对称组装，为许多具有生物医学意义的天然产物中发现的一系列合成有价值的构建块提供了新的条目。此外，适当功能化的硅环支架将导致具有广泛合成用途的新型不对称催化剂。在拟议的四年资助期内，我们将集中于以下具体目标：(a)利用功能化五元和六元硅烷开发新的立体选择性转化；(b)高收敛合成制霉菌素A1的设计；(c)开发了一种完全立体控制合成新西施巴因a的方法；(d)发展通往PF1018的快速路线；(e)合理设计手性硅基路易斯酸催化剂。在广泛的初步结果的支持下，这项全面的研究计划旨在通过创新和有效地使用新型硅环模板来推进现代有机合成的最新技术。

DESCRIPTION (provided by applicant): With the main emphasis on innovation, the primary objective of this program is to develop highly efficient, fully stereocontrolled, and practical synthetic strategies to complex bioactive targets utilizing readily available silacyclic platforms. Assembled via enantioselective desymmetrization, silacyclopentanes and silacyclohexanes provide new entries into a range of synthetically valuable building blocks found in many natural products of biomedical significance. In addition, appropriately functionalized silacyclic scaffolds will lead to new classes of asymmetric catalysts of broad synthetic utility. Within the proposed four-year grant period, we will concentrate on the following specific objectives: (a) development of new stereoselective transformations utilizing functionalized five- and six-membered silanes; (b) design of a highly convergent synthesis of nystatin A1; (c) development of a fully stereocontrolled synthesis of neodysiherbaine A; (d) development of expeditious route to PF1018; (e) rational design of chiral silicon-based Lewis acid catalysts. Supported by extensive preliminary results, this comprehensive research program is aimed at advancing the state-of-the-art of modern organic synthesis through innovative and efficient use of novel silacycles templates.