From Bond Activation to Catalysis

均相催化是高精度、低浪费合成高附加值化工产品（如药品）的首选方法。许多催化剂都含有一个被“保护层”（配体）包围的金属原子；配体的变化允许调整催化剂的性能。我的研究项目旨在了解金属化学反应的步骤，并量化配体变化如何影响这些步骤。在我的小组中，我们使用计算和实验技术，这使我们能够非常详细地探索反应机制。在一个研究主题中，我们研究的配体可以作为“电子储存器”，暂时储存电子，然后在需要时释放它们，使反应发生。在另一个主题中，我们研究的配体与它们的金属紧密结合，但占据了太多的空间，以至于金属无法获得其首选的环境，从而增加了其反应性。在这两个主题中，我们在之前的工作中发现了新的键断裂和化学反应，到目前为止仍然是化学计量学的。在即将到来的资助期内，我们的目标是将其转化为真正的催化。如果成功，这将为主题1带来新的、更清洁的碳骨架选择，碳骨架是有机化合物（包括药物）的骨架。在主题2中，催化方面的成功将使人们更容易和更清洁地获得一系列有机硅化合物，这些化合物可用于有机合成和材料制备。

Homogeneous catalysis is the preferred method for high-precision, minimal-waste synthesis of high-value-added chemical products such as pharmaceuticals. Many catalysts contain a metal atom surrounded by a "protective coat", the ligand; ligand variation allows tuning of the catalyst performance. My research program is aimed at understanding steps of chemical reactions at metals, and at quantifying how ligand variation can be used to influence those steps. Within my group, we use both computational and experimental techniques, which allows us to probe reaction mechanisms in great detail. In one research theme, we study ligands that can function as "electron reservoirs", temporarily storing electrons and then releasing them when needed to make reactions happen. In another theme, we look at ligands that bind strongly to their metal but occupy so much space that the metal is prevented from attaining its preferred surrounding, thus increasing its reactivity. In both themes, we have in previous work discovered new bond breaking and making chemistry that so far is still stoichiometric. In the coming grant period we aim to convert this into true catalysis. If successful, this would lead for theme 1 to new, cleaner options for creating carbon skeletons, the backbones of organic compounds (including pharmaceuticals). In theme 2, success in catalysis would afford easier and cleaner access to a range of organosilicon compounds, which find applications in organic synthesis as well as in the preparation of materials.