CATALYTIC PLATFORMS USING AROMATIC IONS AND OTHER CHARGED SPECIES

项目摘要。长期以来，催化一直是推进生物医学研究的强大力量， 以不断提高的速度、效率和多功能性构建生物学上重要的分子。之一 催化领域进步的最有力的推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，我们开发了 两种通用的催化策略，具有广泛的适用性，在广泛的反应类型。在第一个节目中， 我们帮助开拓了电化学领域，它结合了光和电的力量， 在单一催化剂中产生能量，以促进具有挑战性的化学反应。特别是，我们介绍了 三氨基环丙烯（TAC）离子作为一类新型的电催化剂;这些催化剂已被证明， 可用于许多转化，包括C-H键官能化和烯烃衍生化。的 当前的申请寻求利用电解来实现其它具有挑战性的、前所未有的 反应，特别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 在第二个项目中，我们开创了使用肼催化的催化羰基-烯烃复分解领域。 这种基础能力使广泛的潜在有利的合成方法成为可能。当前 应用程序旨在通过设计高度反应性的下一代 催化剂，大大扩大了可以使用的底物的范围。我们还打算采用这种模式， 催化有用的新化学方法，并开发相关的催化平台，使用这些一般 原则这些和其他研究在催化中使用新的想法将继续作为一个 促进化学合成的发展。

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.