Frontiers in Olefin Metathesis & Metathesis-Derived Nanomaterials

烯烃复分解是目前已知的最有效和最通用的方法，用于建立新的碳-碳键，从而形成新的分子框架。它的应用范围从新药的组装到可再生资源的利用，正如2005年诺贝尔化合作用奖所引用的那样。几十年来，制药和特种化学品制造业的普及是最近才出现的现实。化合作用正被用于获得新的、有效的病毒抑制剂，并将可再生植物油转化为特种化学品。 然而，尽管它具有巨大的潜力，但主要的限制仍然阻碍了它的使用，特别是在化学制造的背景下，它有可能大幅减少浪费。一个主要的挑战在于实现这些反应的催化剂的寿命很短。这导致了不经济、不可靠的过程：此外，竞争反应会产生副产品。这严重限制了化合作用在可再生植物油原料转化中的实际应用，并在制药公司的报告中被强调为一个严重的、反复出现的问题。 我们在这一重要领域的大部分工作都是为了了解和解决限制催化剂寿命和生产率的因素。我们试图了解为什么这些催化剂很脆弱，以及它们在使用条件下是如何分解的。这样的理解将有力地帮助设计下一代、寿命长的催化剂，并扩大工业吸收。我们还寻求扩大这些能力，使目前无法实现的分子结构组装成为可能。开发坚固、多功能、易于操作的催化剂将使这些用于分子设计的强大工具发挥其长期被预言的潜力。 最后，我们还在研究利用催化剂分解的大胆新可能性。我们最近发现，纳米颗粒的形成是分解的关键项目。通过学习如何阻止或促进这些反应，我们希望在分子和纳米颗粒催化的前沿创造重大机会。

Olefin metathesis is the most powerful and versatile method now known for building new carbon-carbon bonds, and hence the frameworks of new molecules. Its applications range from the assembly of new drugs to utilization of renewable resources, as cited in the Nobel Prize for metathesis in 2005. Uptake in pharmaceutical and specialty-chemicals manufacturing, anticipated for decades, is a very recent reality. Metathesis is being used to access new, potent viral inhibitors, and to transform renewable plant oils into specialty chemicals. Despite its enormous potential, however, major limitations still impede its use, particularly in the context of chemical manufacturing, where it has the potential to dramatically reduce waste. A major challenge lies in the short lifetimes of the catalysts that enable these reactions. This leads to uneconomic, unreliable processes: moreover, competing reactions lead to byproducts. This severely restricts the practical use of metathesis for transformation of renewable plant-oil feedstocks, and has been highlighted as a serious, recurring problem in reports from pharma. Much of our work in this important area is directed at understanding and addressing the factors that limit catalyst lifetimes and productivity. We seek to understand why these catalysts are vulnerable, and how they decompose under conditions of use. Such understanding would be a powerful aid to designing next-generation, long-lived catalysts, and expanding industrial uptake. We also seek to expand these capabilities, to enable the assembly of molecular structures presently unattainable. Development of robust, versatile, readily-handled catalysts would allow these powerful tools for molecular design to reach their long-heralded potential. Finally, we are also investigating bold new possibilities in which we harness catalyst decomposition. We have recently discovered that nanoparticles are formed as key projects of decomposition. By learning how to impede, or promote, these reactions, we hope to create major opportunities at the forefront of molecular and nanoparticle catalysis.