Organoiron clusters for controlled redox active catalysis

在重要的氧化还原反应中，自然界经常利用铁团簇来控制电子的流动。这些多金属组件比单金属位点更容易促进电子通量，并广泛用于多种金属酶的过程，如固氮到氨，水分裂和基于自由基的C-C键形成。每一个过程都对社会产生了或潜在的深远影响。例如，哈伯法，一种人造的固氮方法，占你体内氮的三分之二，但这是一个令人难以置信的能源密集型过程，占全球每年二氧化碳排放量的3%左右。一旦克服了与氧氧化相关的挑战，水分解将最终成为氢经济的基础。基于自由基的催化C-C键形成具有巨大的“绿色”化学合成潜力。在这个项目中，我们将“借用”自然界铁簇的结构概念，但将其与有机金属化学相结合，产生新的或很少被探索的结构，这些结构将显示出新的氧化还原特性，我们将尝试在这三类转化中加以利用。

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.