Iron-only hydrogenases: a functional artificial H-cluster

仅铁氢化酶：功能性人工 H 簇

• 批准号: BB/E023290/1
• 负责人: Christopher Pickett
• 金额: $ 39.06万
• 依托单位: University of East Anglia
• 依托单位国家: 英国
• 项目类别: Research Grant
• 财政年份: 2007
• 资助国家: 英国
• 起止时间: 2007 至 无数据
• 项目状态: 已结题
• 来源: https://gtr.ukri.org/projects?ref=BB%2FE023290%2F1
• 关键词: Iron; only; hydrogenases; functional; artificial

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.

在电极上将质子转化为氢气及其反向从氢气中获取电力是对氢经济至关重要的反应。铂金是目前通过电解从水中获取氢气作为燃料以及通过在燃料电池中氧化氢气来发电的最佳催化剂。它是一种昂贵的金属，从长远来看，对于不断扩大的氢经济的需求来说，它可能是不可持续的。与供应安全有关的问题也被提出。自然界使用氢化酶来催化细菌和藻类中氢的产生或使用，进行相同的反应。其中一种酶的核心机制是铁和硫原子（丰富的元素）簇，称为 H 簇。我们正在解决这样一个问题：“我们能否根据自然蓝图制造新材料来替代燃料电池中的铂？”到目前为止，我们和其他人已经证明可以合成与酶催化中心非常相似的结构。然而，这些已被证明是很差的催化剂，部分原因是人造结构有一个“额外”的一氧化碳分子连接到其中一个铁原子上，这“阻止”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。这既有助于我们加深对生物催化工作原理的理解，又可以提供具有技术相关性的先导材料。

项目成果

Anode modification to improve the performance of a microbial fuel cell volatile fatty acid biosensor

• DOI: 10.1016/j.snb.2014.04.062
• 发表时间: 2014-10-01
• 期刊: SENSORS AND ACTUATORS B-CHEMICAL
• 影响因子: 8.4
• 作者: Kaur, Amandeep;Ibrahim, Saad;Premier, Giuliano C.
• 通讯作者: Premier, Giuliano C.

Electronic Control of the Protonation Rates of Fe-Fe Bonds

• DOI: 10.1021/ja506693m
• 发表时间: 2014-09-17
• 期刊: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
• 影响因子: 15
• 作者: Jablonskyte, Ausra;Webster, Lee R.;Pickett, Christopher J.
• 通讯作者: Pickett, Christopher J.

[FeFe] hydrogenase: protonation of {2Fe3S} systems and formation of super-reduced hydride states.

• DOI: 10.1002/anie.201406210
• 发表时间: 2014-09-15
• 期刊: ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
• 影响因子: 16.6
• 作者: Jablonskyte, Ausra;Wright, Joseph A.;Fairhurst, Shirley A.;Webster, Lee R.;Pickett, Christopher J.
• 通讯作者: Pickett, Christopher J.