Organoiron clusters for controlled redox active catalysis

自然界通常通过使用铁簇来控制重要氧化还原反应中电子的流动。这些多金属组装体比单个金属位点更容易促进电子通量，并且用于多种金属酶中，用于各种各样的过程，如固氮成氨、水裂解和基于自由基的C-C键形成。每一个进程目前都对社会产生了或可能产生深远的影响。例如，Haber过程，固氮的人工变体，占人体氮的三分之二，但这是一个令人难以置信的能源密集型过程，占全球二氧化碳年排放量的3%左右。一旦与氧氧化相关的挑战被克服，水分解将最终形成氢经济的基础。基于自由基的催化C-C键形成在“绿色”化学合成中具有巨大的潜力。在这个项目中，我们将“借用”自然界的铁簇的结构概念，但联合收割机这些与有机金属化学，以产生新的或很少探索的结构，将显示新的氧化还原性能，我们将试图利用这三类转换。

Nature often controls the flow of electrons in important redox reactions by the use of iron clusters. These multimetallic assemblies facilitate electron flux far more readily than single metal sites and are used in a wide number of metalloenzymes for processes as diverse as nitrogen fixation to ammonia, water splitting and radical based C-C bond-formation. Each of the processes either currently has or potentially could have a profound impact on society. For instance the Haber process, the artificial variant of nitrogen fixation, accounts for two-thirds of the nitrogen in your body, yet this is an incredible energy intensive process, accounting for around 3% of annual global CO2 emissions. Water splitting will ultimately form the basis of the hydrogen economy, once the challenges associates with oxygen oxidation have been surmounted. Catalytic radical-based C-C bond-formation has a huge potential to 'green' much of chemical synthesis. In this project, we will 'borrow' the structural concepts of Nature's iron clusters, but combine these with organometallic chemistry, to produce new or seldom explored constructs that will show novel redox properties which we will attempt to exploit in these three classes of transformations.