Iron-only hydrogenases: a functional artificial H-cluster

将质子在电极上转化为氢，并将其反过来从氢中获得电力，这些反应对氢经济至关重要。铂是目前最好的催化剂，无论是通过电解从水中获得作为燃料的氢，还是通过在燃料电池中氧化氢来发电。它是一种昂贵的金属，从长远来看，相对于不断扩大的氢经济的需求，它可能是不可持续的。还提出了与供应安全有关的问题。大自然利用氢化酶在细菌和藻类中催化氢的产生或使用，进行同样的反应。其中一种酶的核心机制是一簇铁和硫原子（丰富的元素），被称为h簇。我们正在解决这样一个问题：“我们能否根据大自然的蓝图制造出新的材料来取代燃料电池中的铂？”到目前为止，我们和其他人已经证明，与酶的催化中心非常相似的结构可以被合成。然而，这些被证明是很差的催化剂，部分原因是人工结构有一个“额外的”一氧化碳分子附着在一个铁原子上，这“阻碍”了它与氢或质子的反应。该项目旨在构建一个正常运行的h集群。这将有助于我们发展对生物催化如何工作的理解，并可能提供与技术相关的主要材料。

Converting protons to hydrogen at an electrode and its reverse getting electricity from hydrogen are reactions of fundamental importance to a hydrogen economy. Platinum is currently the best catalyst for both obtaining hydrogen as a fuel from water by electrolysis and using hydrogen to produce electricity by oxidising it in fuel cells. It is an expensive metal and in the long term is likely unsustainable with respect to demand from an expanding hydrogen economy . Issues relating to security of supply have also been raised. Nature carries out the same reactions using hydrogenase enzymes to catalyse the production or use of hydrogen in bacteria and algae . The machinery at the heart of one of these enzymes is a cluster of iron and sulfur atoms (abundant elements) known as the H-cluster. We are addressing the question 'can we make new materials based on nature's blueprint to replace platinum in fuel cells?' So far we and others have shown that structures closely similar to the catalytic centre of the enzyme can be synthesised. However these have proved poor catalysts, in part because the artifical structures have an 'extra' molecule of carbon monoxide attached to one of the iron atom and this 'blocks' its reaction with hydrogen or protons. This project sets out to build a functioning H-cluster. This will both help us to develop our understanding of how the biological catalysis works and may provide lead materials of technological relevance.