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: 7914639
• 负责人: Neal P Mankad
• 金额: $ 4.56万
• 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/7914639
• 关键词: Address; Amination; Area; Arts; Biochemistry; Biological Factors; Biology; Chemicals; Chemistry; Communities; Complement; Complex; Development; Environment; Exhibits; Health; Human; Literature; Methodology; Methods; Molecular Bank; Nitrogen; Organic Chemistry; Pharmacologic Substance; Pharmacology; Reaction; Reagent; Research; Research Personnel; Scientist; Work; catalyst; cost; 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）：生物学、生物化学、药理学、天然产物合成和环境化学等领域与人类健康相关的科学研究需要不断增长且日益复杂的分子工具库才能进行。合成有机化学必须不断发展以满足对有用分子的需求，其为科学界做出贡献的能力建立在持续开发高效且适用的合成方法的基础上。合成方法开发中剩下的巨大挑战之一是发现简单而通用的方法，将氮等杂原子引入有机分子中。在此广泛的背景下，该提案重点关注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并正在该领域工作，但该提案利用新颖且创造性的策略来解决该问题，使得本文提出的方法因多种原因而独一无二。首先，目前许多最先进的 C-N 键形成方法需要苛刻的氧化条件并产生大量的化学废物。该提案的部分内容提出了仅需要催化剂而无需额外试剂即可将底物转化为产物的方法，并且释放气态二氢（H2）作为唯一的副产物。这种策略不需要苛刻的反应条件，优化了原子经济性，并将化学废物保持在最低限度。其次，该提案中的合成方法有望通过利用非常规反应机制来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使所提出的方法补充大量的合成文献，从而为合成有机化学家提供用于合成复杂分子的工具集。这些综合因素使得所提出的研究对于致力于人类健康的科学研究领域具有适用性和重要性。 公共健康相关性：有机化学新合成方法的开发至关重要：1) 让人类健康多个领域的科学家能够获得其研究所需的分子，2) 简化制造效率（从而降低成本）药物化合物，3）找到合成这些复杂分子的方法，同时最大限度地减少污染环境的化学废物。该提案中的研究涉及所有这些主题，因此以切实和适用的方式与人类健康密切相关。