Catalysis: Relating Structure and Reactivity

这项提案寻求开发一种普遍适用的方法来发明催化剂，该催化剂能够执行目前不可能或至少不可能使用温和和通用的方案进行的化学转化。具体地说，交叉偶联催化剂正在为广泛的应用而设计，这些应用将推动可用于促进我们社会所依赖的健康、生命和材料科学领域的新化学实体的发展。这一目标将通过加强我们对有机金属催化剂金属中心的基本物理性质(例如，电子和空间电子)的了解来实现，以便能够预测它将如何在广泛的化学转化中改变反应活性。这将涉及到结合各种不同类型的工具来解决这个问题，包括计算、速率研究、核磁共振光谱、循环伏安法和使用同步辐射的X射线吸收光谱。这种多管齐下的催化剂设计方法可以应用于交叉耦合转化家族以外的更广泛的催化过程。

This proposal seeks to develop a generally applicable process to invent catalysts capable of performing chemical transformations not currently possible, or at least not possible using mild and general protocols. Specifically, cross-coupling catalysts are being designed for widespread applications that would propel the development of new chemical entities available to advance the health-, life-, and materials-science fields upon which our society depends. This objective will be achieved by intensifying our understanding of the fundamental physical properties (e.g., electronics and sterics) at the metal centre of an organometallic catalyst so as to be able to predict how it will alter reactivity in a broad selection of chemical transformations. This will involve combining a variety of different types of tools to bear on this problem including computation, rate studies, NMR spectroscopy, cyclic voltametry, and X-ray absorption spectroscopy using synchrotron radiation. This multi-pronged approach to catalyst design can be applied to a much wider array of catalytic processes outside of the cross-coupling family of transformations.