Discovery of new catalytic reactions through mechanistically guided screening

通过机械引导筛选发现新的催化反应

• 批准号: RGPIN-2015-05019
• 负责人: Newman, Stephen
• 金额: $ 1.82万
• 依托单位: University of Ottawa
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2019
• 资助国家: 加拿大
• 起止时间: 2019-01-01 至 2020-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=680599
• 关键词: Discovery; new; catalytic; reactions; through

Nature of the research***Research in the Newman group focuses on the application of modern technologies to the advancement of fundamental and applied chemistry. In particular, we are exploring the use of high throughput experimentation (HTE) and flow chemistry platforms for the synthesis of valuable molecules. This proposal focuses on the application of HTE to the discovery of homogeneously catalyzed reactions of readily available building blocks. Being a young research group, our goal is to take on high impact projects with the intention of establishing a unique, world-class research program. This will occur through three phases: 1) Reaction discovery, optimization, and mechanism elucidation; 2) Application to the synthesis of pharmaceuticals and biomass-derived bulk chemicals; and 3) Use of our increased understanding of catalysis for further reaction development. This research proposal describes a 5 year plan for phase 1, discovery of new chemical reactions, including a new C-C cross-coupling reaction, an atom economical olefin-aldehyde coupling, and an N2O-alkyne `click' reaction for the synthesis of diazo species.***Significance, expected outcomes, and benefits to Canadians***Synthetic chemistry has a great role to play in the most important needs for society. Our health relies on the development of lifesaving pharmaceuticals, the majority of which are small organic molecules. New synthetic methods allow medicinal chemists to produce larger, more diverse libraries, increasing the chances of finding the next life-saving therapeutics. Sustainability is another critical focus - it is important to decrease human impact on the environment and reduce dependency on non-renewable chemicals. New chemistries are needed that make use of abundant resources in an environmentally benign manner. The proposed research works towards these needs by focusing on catalytic, low-waste coupling of simple molecules to prepare complex structures that may find use in pharmaceutical and bulk chemical synthesis. The knowledge gained in these studies can also have a direct impact on Canada's large oil, bulk chemical, and biomass industries, who are facing increasing competition and demand for decreased pollution. Our group seeks direct, sustainable methods for creating value-added chemicals from readily available feedstocks, leading to new technologies to strengthen the chemical industry. Most importantly, the program provides an enriching environment for training forward-thinking scientists in organic synthesis, catalysis, and green chemistry; areas that will play a key role in the well-being of our society for many generations. Our particular focus on fundamental understanding of chemical reactions combined with the use of new technologies to streamline the discovery processes is a unique approach that will train students in the skills necessary for competitive jobs in industry and academia.**

研究性质***纽曼小组的研究重点是应用现代技术来推动基础化学和应用化学的进步。特别是，我们正在探索使用高通量实验（HTE）和流动化学平台来合成有价值的分子。该提案重点关注 HTE 在发现现成结构单元的均相催化反应中的应用。作为一个年轻的研究小组，我们的目标是开展高影响力的项目，旨在建立一个独特的、世界一流的研究项目。这将通过三个阶段进行：1）反应发现、优化和机制阐明； 2）在药物和生物质原料化学品合成中的应用； 3) 利用我们对催化作用的加深了解来进一步开发反应。该研究计划描述了第一阶段的 5 年计划，发现新的化学反应，包括新的 C-C 交叉偶联反应、原子经济的烯烃-醛偶联反应以及用于合成重氮物质的 N2O-炔“点击”反应.***对加拿大人的意义、预期成果和利益***合成化学在满足社会最重要的需求方面发挥着巨大作用。我们的健康依赖于救生药物的开发，其中大部分是有机小分子。新的合成方法使药物化学家能够产生更大、更多样化的文库，从而增加找到下一个拯救生命的疗法的机会。可持续性是另一个关键焦点 - 减少人类对环境的影响并减少对不可再生化学品的依赖非常重要。需要新的化学物质以对环境无害的方式利用丰富的资源。拟议的研究致力于满足这些需求，重点关注简单分子的催化、低废物偶联，以制备可用于药物和大宗化学合成的复杂结构。这些研究中获得的知识也可以对加拿大大型石油、大宗化学品和生物质工业产生直接影响，这些工业面临着日益激烈的竞争和减少污染的需求。我们的团队寻求直接、可持续的方法，利用现成的原料创造增值化学品，从而开发出加强化学工业的新技术。最重要的是，该项目为培训有机合成、催化和绿色化学方面具有前瞻性思维的科学家提供了丰富的环境；这些领域将对我们社会几代人的福祉发挥关键作用。我们特别注重对化学反应的基本理解，并结合使用新技术来简化发现过程，这是一种独特的方法，将培训学生在工业界和学术界竞争性工作所需的技能。 **