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）：在生物学、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。合成有机化学必须发展以满足对有用分子的这种需求，其为科学界做出贡献的能力建立在有效和适用的合成方法的持续发展之上。在合成方法学发展中，最大的挑战之一是发现将杂原子如氮引入有机分子中的简单和通用的方法。在这一广泛的背景下，该提案侧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。虽然许多研究人员已经和正在这一领域工作，但该提案利用新颖和创造性的策略来解决这个问题，由于几个原因，本文提出的方法是独一无二的。首先，许多目前最先进的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。该提案的部分提出了仅需要催化剂而不需要额外的试剂来将底物转化为产物的方法，其中释放气态二氢（H2）作为唯一的副产物。这种策略避免了苛刻的反应条件，优化了原子经济性，并将化学废物降至最低。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。这种新出现的二分法将使所提出的方法补充更大的合成文献，因此有助于合成有机化学家合成复杂分子的工具集。这些集体因素使拟议的研究适用于致力于人类健康的科学研究领域，并具有重要意义。 公共卫生相关性：有机化学中新合成方法的开发至关重要：1）允许人类健康多个领域的科学家获得研究所需的分子，2）简化制造药物化合物的效率（以及因此的成本），以及3）找到允许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。本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密切相关。