BIOMIMETIC CATALYSIS THROUGH MOLECULAR RECOGNITION

本工作将开发几种新的仿生催化体系。 统一的主题是分子识别，使用强大的，通用的 这是我们开发的一类手性受体。 这些主机是 它们结合和定向有机分子的能力无与伦比。 我们现在 我们希望将这些结构开发成有用的催化剂，我们将继续研究 两种不同的策略。 首先，我们将利用固有的约束能力 电子结合过渡态， 加速有机反应。 我们已经看到了非常令人鼓舞的 这一领域的初步结果表明， 生物催化剂的作用。 其次，我们将修改主机， 结合反应性过渡金属作为本征部分， 受体，从而在结合位点产生会聚功能。 我们已经瞄准了几种反应类型，我们将寻求催化 速率增强，特别是立体化学控制。 我们的目标是 开发真正的催化系统，可以接受广泛的底物 并实施实质性的立体化学控制。 任何一个成功 我们的目标系统将构成生物有机的重大进步， 和合成有机化学。

The present work will develop several new biomimetic, catalytic systems. The unifying theme is molecular recognition, using a powerful, general class of chiral receptors that we have developed. These hosts are unsurpassed in their ability to bind and orient organic molecules. We now wish to develop these structures into useful catalysts, and we will pursue two different strategies. First, we will use the inherent binding ability of our hosts to electronically bind transition states, and thereby accelerate organic reactions. We have already seen very encouraging preliminary results in this area that suggest new insights into the nature of biological catalysis may be gained. Second, we will modify our hosts to incorporate reactive transition metals as an intrinsic part of the receptor, thereby creating convergent functionality at the binding site. We have targeted several reaction types, and we will be pursuing catalytic rate enhancements and, especially, stereochemical control. Our goal is to develop truly catalytic systems that can accept a broad range of substrates and that enforce substantial stereochemical control. Success in any one of our target systems would constitute a significant advance for bioorganic and synthetic organic chemistry.