Catalytic Amination Reactions Utilizing Bimetallic Cooperativity

利用双金属协同作用的催化胺化反应

• 批准号: 8110064
• 负责人: Neal P Mankad
• 金额: $ 4.84万
• 依托单位: UNIVERSITY OF CALIFORNIA BERKELEY
• 依托单位国家: 美国
• 财政年份: 2010
• 资助国家: 美国
• 起止时间: 2010-03-03 至 2013-03-02
• 项目状态: 已结题
• 来源: https://reporter.nih.gov/project-details/8110064
• 关键词: Address; Alkenes; Amination; Amines; Amino Acids; Area; Attention; Biochemistry; Biological Factors; Biology; Catalysis; Chemicals; Chemistry; Communities; Complement; Complex; Development; Environment; Exhibits; Health; Human; Hydrogen Bonding; Literature; Mediating; Methodology; Methods; Molecular; Molecular Bank; Nitrogen; Organic Chemistry; Organic Synthesis; Pharmacologic Substance; Pharmacology; Reaction; Reagent; Research; Research Personnel; Science; Scientist; Transition Elements; Work; catalyst; cost; diene; meetings; novel; public health relevance; tool; wasting

DESCRIPTION (provided by applicant): Scientific research relevant to human health in areas such as biology, biochemistry, pharmacology, natural product synthesis, and environmental chemistry requires a growing and increasingly complex library of molecular tools in order to proceed. Synthetic organic chemistry must evolve to meet this need for useful molecules, and its ability to contribute to the scientific community is founded on the continued development of efficient and applicable synthetic methods. One of the great remaining challenges in synthetic methodology development is to uncover simple and general methods to introduce heteroatoms such as nitrogen into organic molecules. Within this broad context, this proposal focuses on new methods for installing C-N bonds into organic molecules in simple and efficient ways. Though many researchers have worked and are working in this area, this proposal utilizes novel and creative strategies to address the problem, making the methods proposed herein unique for several reasons. First, many of the current state-of-the-art methods for C-N bond formation require harsh oxidizing conditions and generate copious chemical waste. Portions of this proposal put forth methods that require only a catalyst and no additional reagents to convert substrates to products, with liberation of gaseous dihydrogen (H2) as the only byproduct. This strategy obviates the need for harsh reaction conditions, optimizes atom economy, and keeps chemical waste to a minimum. Secondly, the synthetic methods in this proposal hold the promise to exhibit modes of chemical selectivity distinct from existing methods by virtue of utilizing unconventional reaction mechanisms. This emerging dichotomy will cause the proposed methods to complement the larger body of synthetic literature and therefore contribute to the set of tools available to synthetic organic chemists for the synthesis of complicated molecules. These collective factors make the proposed research applicable and important to areas of scientific research devoted to human health. PUBLIC HEALTH RELEVANCE: The development of new synthetic methods in organic chemistry is crucial 1) to allow scientists in several fields of human health to access the molecules necessary for their research, 2) to streamline the efficiency (and, therefore, cost) of making pharmaceutical compounds, and 3) to find methods that allow the synthesis of these complicated molecules while minimizing the chemical waste that pollutes the environment. The research in this proposal addresses all of these topics, and therefore is tremendously relevant to human health in tangible and applicable ways.

描述（由申请人提供）：与人类健康有关的科学研究在生物学，生物化学，药理学，自然产品合成和环境化学等领域，需要一个分子工具的增长且越来越复杂的分子工具库才能进行。合成有机化学必须发展以满足对有用分子的需求，并且其为科学界做出贡献的能力是基于持续发展有效且适用的合成方法的。合成方法论发展中剩下的一项巨大挑战之一是发现简单而通用的方法将杂原子（例如氮）引入有机分子中。在这种广泛的背景下，该提案着重于以简单有效的方式将C-N键安装到有机分子中的新方法。尽管许多研究人员已经在这一领域工作并正在工作，但该提案利用新颖和创造性的策略来解决该问题，从而使本文所提出的独特方法出于多种原因。首先，许多当前的C-N键形成方法都需要恶劣的氧化条件并产生大量的化学废物。该提案的一部分提出的方法仅需要催化剂，也不需要其他试剂即可将底物转换为产品，而气态二氢（H2）则是唯一的副产品。该策略消除了对严酷的反应条件的需求，优化了原子经济，并将化学废物保持在最低水平。其次，该提案中的合成方法有望通过利用非常规反应机制表现出与现有方法不同的化学选择性模式。这种新兴的二分法将导致提出的方法补充较大的合成文献体，因此有助于合成有机化学家可用的一组工具，以合成复杂的分子。这些集体因素使所提出的研究适用于专门针对人类健康的科学研究领域。 公共卫生相关性：有机化学中新的合成方法的发展至关重要1）允许在人类健康的多个领域中的科学家访问其研究所需的分子，2）简化制造药物化合物的效率（以及成本），以及3），可以找到这些复杂的化学量化的化学量来弥补这些复杂的化学量的方法。该提案中的研究涉及所有这些主题，因此以有形和适用的方式与人类健康非常相关。