Olefin metathesis asymmetric metathesis and tandem catalysis

我们研究的一个主要目标是设计坚固、选择性强的催化剂，以促进碳-碳键的形成。正如2005年诺贝尔化学奖授予施罗克、格拉布斯和肖文的引文中指出的那样，烯烃复分解是目前用于这一目的的最强大的工具之一。虽然SchRock催化剂的高选择性、可调是实现所需有机化合物合成的主要优势，但它们对空气和水的高度敏感性是有问题的。格拉布斯催化剂以亲氧性较低的过渡金属Ru为基础，更易于操作，极大地扩大了有机合成中烯烃歧化反应的吸收。然而，尽管有这种强大的生命力，但它们都是短暂的。它们在调节活动性和选择性方面也受到限制。通过研究它们的失活途径，我们开发了一种寿命更长、生产效率更高的新催化剂家族。它还提供了更大的潜力来定义催化剂上的活性中心，从而实现选择性。将稳健性和选择性结合起来，将把烯烃复分解实验发展的两大主流结合起来。

A major goal of our research is the design of robust, selective catalysts that promote the formation of carbon-carbon bonds. Olefin metathesis is one of the most powerful tools now in use for this purpose, as noted in the citation awarding the 2005 Nobel Prize in Chemistry to Schrock, Grubbs, and Chauvin. While the high, tunable selectivity of the Schrock catalysts is a major asset in achieving the synthesis of desired organic compounds, their high sensitivity to air and water is problematic. The Grubbs catalysts, based on the less oxophilic transition metal ruthenium, are much more easily handled, and have greatly expanded the uptake of olefin metathesis in organic synthesis. Despite this robustness, however, they are short-lived. They are also limited in terms of the ease of tuning activity and selectivity. Studying their deactivation pathways led us to develop a new family of catalyst that is longer-lived and more productive. It also offers expanded potential to define the active site at the catalyst, and thus selectivity. Combining robustness with selectivity would unite the two main streams of experimental development in olefin metathesis.