Arylation of weakly acidic sp3 hybridized C-H's

在此输入文本，它是应用程序的新摘要信息。本节必须是否 超过30行的文本。 绝大多数药物和具有生物活性的天然产品都含有碳- 碳键因此，这些和相关小分子的合成依赖于 碳-碳键形成反应。因此，创新的方法， 有效的C-C键形成将容易地扩大小分子的多样性 并加速药物的发现。本报告的总体目标 应用是发展新的和实用的方法sp3-C-H键 官能化/与非常弱酸性的C-H的C-C偶联（pKa为32至超过40）。 为实现这一目标，采取了两种基于机制的战略。第一 涉及芳烃通过配位向过渡而向温和的去质子化方向活化 金属催化剂，并且包括对映选择性变体。在产品中， 这些反应是三芳基甲烷和二芳基甲胺。第二种方法是 基于去质子交叉偶联方法（DCCP），其中sp3-C-H与 pKa高达35的化合物在催化条件下去质子化并与芳基偶联 卤化物。为了进行这类具有挑战性的反应，已经开发了新的催化剂。 具有前所未有的反应性。通过对催化剂作用机理的研究， 新的指导原则被揭示出来， 更大的化学社区。该催化剂将应用于未活化的DCCP 二芳基甲烷、烯丙基苯、N，N-二烷基苄基胺、亚砜、磺酰胺和 砜以产生新的芳基化产物。拟定的方法开发，以及 机械的洞察力，将提供一个实用的工具，使新的和 容易应用于药物合成的有效的结合结构。的 在本申请中形成C-C键的两种方法是创新的，因为它们 与已知的化学性质明显不同。

Enter the text here that is the new abstract information for your application. This section must be no longer than 30 lines of text. The vast majority of medications and biologically active natural products contain carbon- carbon bonds. The synthesis of these, and related small molecules, is therefore reliant on carbon-carbon bond-forming reactions. It follows that innovative approaches to efficient C-C bond formations will broaden the diversity of small molecules easily accessible and accelerate the discovery of drugs. The overall objective of this application is to develop novel and practical methods for sp3-C-H bond functionalizations/C-C couplings with very weakly acidic C-H's (pKa's 32 to over 40). Two mechanistic-based strategies are pursued to achieve this objective. The first involves activation of arenes toward mild deprotonation by coordination to transition metal catalysts, and encompasses enantioselective variants. Among the products of these reactions are tiarylmethanes and diarylmethylamines. The second approach is based on deprotonative cross-coupling procedures (DCCP's) wherein sp3-C-H's with pKa's as high as 35 are deprotonated under catalytic conditions and coupled with aryl halides. To perform this challenging class of reactions, new catalysts have been identified with unprecedented reactivity. By study of the mechanism of these catalysts, fundamentally new guiding principles have been revealed that are of interest to the greater chemistry community. This catalysts will be applied to DCCP's of unactivated diarylmethanes, allylbenzenes, N,N-dialkylbenzylamines, sulfoxides, sulfonamides, and sulfones to generate novel arylated products. The proposed method development, and mechanistic insight, will provide a collection of practical tools that enable new and efficient bond constructions that are easily applied to the synthesis of medications. The two approaches to C-C bond-formation in this application are innovative because they represent a clear departure from known chemistry.