Organic Photoredox Catalysts for Synthetic Method Development

项目摘要 用于合成方法开发的有机光氧化还原催化剂 加勒特·M三宅，科罗拉多州立大学，化学系 催化可以说是对社会最重要的化学贡献，因为它使 合成对改善人类生活至关重要的药物和材料。到 解决当前和未来的健康需求，开发催化剂系统， 通过新的、更有效的技术， 化学反应是必要的。然而，许多经典的催化方法 使用贵金属、危险试剂或强制条件。相比之下， 光氧化还原催化已成为一种强大的途径，以获得独特的反应 并利用光驱动化学反应。光氧化还原催化的优点 包括在温和条件下进行反应的能力，避免危险， 非选择性试剂，实现新的选择性，增加官能团 耐受性，提高反应效率，并获得前所未有的反应 中间体和歧管。在光氧化还原催化方面的许多工作都得到了很好的应用- 研究了具有氧化激发态的贵金属络合物或有机染料 作为催化剂。因此，为了解决金属污染、可持续性和 为了扩大和新颖的反应性，具有不同的光氧化还原活性的新型有机光氧化还原催化剂 必须开发生物物理和电化学性能。的长期目标 拟议的研究活动是开发有机光氧化还原催化剂体系， 能够实现新的和改进的小分子和材料的合成， 人的健康需要。本文介绍了有机光氧化还原反应的发展 具有前所未有的氧化还原电位的催化剂体系， 反应性我们将采用实验和计算相结合的方法 获得对催化剂和反应机理的基本理解。 通过机械引导的催化剂设计，我们试图设计出能够 获得必要的极端还原性或氧化性化学势， 具有挑战性的反应性。最终，这项研究将有助于人类健康， 开发具有独特反应性的催化剂， 药物和医学重要材料的合成。

Project Summary Organic Photoredox Catalysts for Synthetic Method Development Garret M. Miyake, Colorado State University, Department of Chemistry Catalysis is arguably the most important chemical contribution to society as it enables the synthesis of medicines and materials that are critical to enhancing human lives. To address current and future health needs, the development of catalyst systems that accelerate the discovery and manufacturing of medicines through new and more efficient chemical reactions are necessary. However, many classic catalytic methodologies employ precious metals, hazardous reagents, or forcing conditions. By contrast, photoredox catalysis has emerged as a powerful approach to access unique reaction pathways and drive chemical reactions using light. Advantages of photoredox catalysis include the ability to perform reactions under mild conditions, obviation of hazardous and non-selective reagents, achievement of new selectivity, increased functional group tolerance, increased reaction efficiencies, and access to unprecedented reaction intermediates and manifolds. Much of the work in photoredox catalysis has applied well- studied precious metal complexes or organic dyes that possess oxidizing excited states as the catalysts. As such, to address metal contamination, sustainability, and the need for expanded and novel reactivity, new organic photoredox catalysts with diverse photophysical and electrochemical properties must be developed. The long-term goal of the proposed research activities is to develop organic photoredox catalyst systems that enable novel and improved syntheses of small molecules and materials that address human health needs. This proposal describes the development of organic photoredox catalyst systems with unprecedented redox potentials that enable new chemical reactivity. We will employ a combination of experimental and computational approaches to gain a fundamental understanding into the catalysts and reaction mechanisms. Through mechanistically guided catalyst design, we seek to engineer systems that can access the extremely reducing or oxidizing chemical potentials necessary to enable challenging reactivity. Ultimately, this research will contribute to human health through the development of catalysts with unique reactivity to enable new and improved syntheses of medicines and medically important materials.