CATALYTIC PLATFORMS USING AROMATIC IONS AND OTHER CHARGED SPECIES

项目摘要。长期以来，催化一直是推动生物医学研究的一股强大力量，因为它使 以不断提高的速度、效率和多功能性构建具有生物重要性的分子。其中之一 催化领域取得进展的最强大动力是发现了新的催化剂 平台和概念。拟议的研究计划主要集中在推进催化领域。 通过开发新的催化平台、概念和方法。特别是，我们已经开发出 两种具有广泛适用性的通用催化策略，适用于多种反应类型。在第一个节目中， 我们帮助开创了电光催化领域的先河，它结合了光和电的力量 单一催化剂内的能量，以促进具有挑战性的化学反应。特别是，我们已经介绍了 三氨基环丙烯(TAC)离子作为一类新型的电光催化剂已被证明 可用于许多转换，包括C-H键功能化和烯烃衍生化。这个 目前的应用寻求利用电光催化来实现其他具有挑战性的、前所未有的 反应，尤其是那些需要非常高的氧化还原电位或涉及多个氧化还原事件的反应。在 第二个项目，我们开创了使用联氨催化羰基-烯烃歧化反应的领域。 这种基础能力使一系列具有潜在优势的合成方法成为可能。海流 应用程序寻求通过设计高反应性的下一代 催化剂极大地扩大了可使用的底物的范围。我们还打算将这种模式应用于 催化转化为有用的新化学方法，并利用这些通用的催化方法开发相关的催化平台 原则。这些和其他关于在催化中使用新想法的调查将继续发挥作用 化学合成进步的推动力。

Project Summary. Catalysis has long been a potent force for advancing biomedical research by enabling the construction of biologically important molecules with ever-increasing speed, efficiency, and versatility. One of the most potent driving forces for progress in the area of catalysis has been the discovery of new catalytic platforms and concepts. The proposed research program is broadly focused on advancing the area of catalysis through the development of novel catalytic platforms, concepts, and methods. In particular, we have developed two generic catalytic strategies with broad applicability over a wide array of reaction types. In the first program, we have helped to pioneer the area of electrophotocatalysis, which combines the power of light and electrical energy within a single catalyst to promote challenging chemical reactions. Especially, we have introduced trisaminocyclopropenium (TAC) ions as a novel class of electrophotocatalyst; these catalysts have proven to be useful for a number of transformations, including C–H bond functionalizations and olefin derivatizations. The current application seeks to leverage electrophotocatalysis to realize other challenging, unprecedented reactions, especially those requiring very high redox potentials or involving multiple redox events. In the second program, we have pioneered the area of catalytic carbonyl-olefin metathesis, using hydrazine catalysis. This foundational capability enables a wide range of potentially advantageous synthetic methods. The current application seeks to make major advances to this program by designing highly reactive, next-generation catalysts that greatly expand the scope of substrates that can be engaged. We also aim to apply this mode of catalysis to useful new chemical methods, and to develop related catalytic platforms using these general principles. These and other investigations into the use of novel ideas in catalysis will continue to serve as a stimulus for advancements in chemical synthesis.