A New Approach To Selective Noble Metal Catalysts

选择性贵金属催化剂的新方法

• 批准号: 8320349
• 负责人: MICHEL R GAGNE
• 金额: $ 29.59万
• 依托单位: UNIV OF NORTH CAROLINA CHAPEL HILL
• 依托单位国家: 美国
• 财政年份: 2000
• 资助国家: 美国
• 起止时间: 2000-02-01 至 2014-08-31
• 项目状态: 已结题
• 来源: https://reporter.nih.gov/project-details/8320349
• 关键词: Alcohols; Alkenes; Alkynes; Anabolism; Carbon; Catalysis; Cations; Chemicals; Cleaved cell; Complex; Consumption; Coupling; Cyclization; DNA Sequence Rearrangement; Development; Diterpenes; Ensure; Enzymes; Generations; Goals; Gold; In Situ; Individual; Intercept; Ions; Ketones; Lead; Metals; Methods; One-Step dentin bonding system; Outcome; Reaction; Research; Rest; Rewards; Route; Scheme; Silver; Skeleton; Steroids; Sterol Biosynthesis Pathway; Sterols; Structure; Terpenes; Transition Elements; analog; catalyst; coping; cross reactivity; design; diene; improved; interest; novel strategies; oxidation; preference; propadiene; public health relevance; success; usability

DESCRIPTION (provided by applicant): The design and execution of reliable complexity enhancing chemical transformations continues to be a goal at the forefront of synthesis. Since transition metal catalysts increase efficiency and enable new routes to complex molecules, their utility will continue to grow. This proposal outlines a research plan for developing a broad class of metal catalyzed reactions that utilize electrophilic metal catalysts (Pt, Au) to initiate, propagate, and terminate cation-olefin reactions (CORs), the principal C-C bond (and ring) forming reaction in terpene biosynthesis. The first Specific Aim focuses on the development of asymmetric catalysts for the dehydrogenative cation-olefin cyclization reaction, with a special emphasis on alkene terminated examples. The second Specific Aim takes this concept one step further by oxidatively intercepting the intermediate Pt-C3 organometallic to generate C3-oxygenated products, which are common bio-active compounds. The third specific aim investigates the mechanism of common Gold(I) catalyzed reactions to support new approaches to asymmetric catalysis and cyclization/cross-coupling. PUBLIC HEALTH RELEVANCE: This project will develop new approaches to the synthesis of complex carbocyclic structures. The emphasis is on discovering synthetic catalysts that mimic the outcome of terpene cyclase enzymes in biosynthesis. Success will provide access to natural bioactive compounds and non-natural analogs thereof.

描述（由申请人提供）：设计和执行可靠的复杂性增强化学转化仍然是合成的最前沿目标。由于过渡金属催化剂提高了效率，并使复杂分子的新途径成为可能，因此它们的实用性将继续增长。该提案概述了开发利用亲电金属催化剂（Pt、Au）来引发、传播和终止阳离子-烯烃反应（COR）的大类金属催化反应的研究计划，所述阳离子-烯烃反应是萜烯生物合成中的主要C-C键（和环）形成反应。第一个具体目标集中在不对称催化剂的发展，为双价阳离子烯烃环化反应，特别强调烯烃封端的例子。第二个具体目标通过氧化截取中间体Pt-C3有机金属以生成C3-氧化产物（其是常见的生物活性化合物）将这一概念更进一步。第三个具体目标是研究常见的金（I）催化反应的机理，以支持不对称催化和环化/交叉偶联的新方法。 公共卫生相关性：该项目将开发合成复杂碳环结构的新方法。重点是发现合成催化剂，模仿萜烯环化酶的生物合成的结果。成功将提供获得天然生物活性化合物及其非天然类似物的途径。