Transition metal complexes for hydroxylation of unactivated hydrocarbons

我的小组从事金属离子化学的研究，对氧化过程特别感兴趣。工业非常需要能量上可行且对环境友好的反应，将石油和天然气的成分碳氢化合物转化为有用的化学品。然而，在温和的条件下，碳氢化合物的直接氧化转化仍然非常难以实现。大自然通过使用在环境友好条件下运作的含金属酶，优化了许多这样的反应；因此，它是这种化学的一个伟大的灵感来源。因此，我的小组的研究目标是双重的：(1)了解酶效率的起源，(2)制备可以进行类似反应的催化剂。我们最初的方法是用小的含金属分子（称为金属配合物）来模拟酶活性位点，并研究它们的反应性行为。模型和酶的比较将告诉我们实现强反应性所需的因素。接下来，我们将在金属配合物中实现这些因子的高效催化。在短期内，这项研究将更好地理解大自然使用的工具箱，以及如何改善衬底与与金属离子结合的氧原子之间的相互作用。从长远来看，我们的发现将指导碳氢化合物氧化转化的设计，从而最大限度地减少步骤和废物副产品的数量。

My group pursues research in the chemistry of metal ions and is specifically interested in oxidation processes. Industry has a great need for energetically viable and environmentally friendly reactions that convert hydrocarbons, the constituents of oil and natural gas, into useful chemicals. Yet, the direct oxidative transformation of hydrocarbons remains tremendously difficult to achieve in mild conditions. Nature has optimized many such reactions through the use of metal-containing enzymes which operate in environmentally friendly conditions; it is therefore a great source of inspiration for this chemistry. The research goals of my group are thus two-fold: (1) understand the origin of the efficiency of the enzymes, and (2) prepare catalysts that can perform similar reactions. Our initial approach is to model the enzymatic active sites with small metal-containing molecules (called metal complexes) and study their reactivity behaviour. Comparison of the models and the enzymes will inform us on the factors necessary to achieve a strong reactivity. Next, we will implement these factors in metal complexes to perform efficient catalysis. In the short term, this research will provide a better understanding of the toolkit used by nature and how to improve the interaction between a substrate and an oxygen atom bonded to a metal ion. In the long term, our discoveries will guide the design of oxidative hydrocarbon transformations that minimize the number of steps and waste by-products.