Catalysis: Relating Structure and Reactivity

本提案旨在开发一种普遍适用的工艺来发明能够进行化学转化的催化剂，目前不可能，或者至少不可能使用温和和一般的协议。具体地说，交叉偶联催化剂正在被设计用于广泛应用，这将推动新的化学实体的发展，从而推动我们社会所依赖的健康、生命和材料科学领域的发展。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（例如电子学和立体学）的理解来实现，以便能够预测它将如何在广泛的化学转化中改变反应性。这将涉及结合各种不同类型的工具来处理这个问题，包括计算、速率研究、核磁共振光谱、循环伏特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更广泛的催化过程，而不是交叉耦合变换家族。

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.