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The reduction of carbon dioxide by enzymes adsorbed on electrodes: from mechanistic studies to bioinspired catalysts

通过电极上吸附的酶还原二氧化碳：从机理研究到仿生催化剂

基本信息

批准号：
BB/I026367/1
负责人：
Judy Hirst
金额：
$ 30.53万
依托单位：
MRC Centre Cambridge
依托单位国家：
英国
项目类别：
Research Grant
财政年份：
2012
资助国家：
英国
起止时间：
2012 至无数据
项目状态：
已结题

来源：
https://gtr.ukri.org/projects?ref=BB%2FI026367%2F1
关键词：
reduction carbon dioxide enzymes adsorbed

项目摘要

Carbon dioxide (CO2) is produced by the combustion of carbon-containing molecules, such as fossil fuels, to power industry, for transportation, and in our homes. Burning fossil fuels is not only causing the level of CO2 in the atmosphere to increase (CO2 is a greenhouse gas and a major contributor to global warming) it is also depleting valuable resources that are required for the manufacture of plastics, chemicals, fertilizers - and countless other requirements of modern society. Unfortunately, CO2 is a very stable and unreactive molecule, and the only large scale process known that can remove CO2 from the atmosphere and use it to regenerate a carbon-containing fuel is biological photosynthesis (growing plants and trees). Therefore, an industrial process that could use the energy from sunlight, or a green-electricity source, to take CO2 out of the atmosphere and turn it into a useful fuel or chemical would revolutionise modern society, by supplying both our energy and material demands. Of course, no such process currently exists. The aim of this proposal is to explore a new approach for the development of such a process. Some bacteria use enzymes called formate dehydrogenases (FDHs) to catalyse the oxidation (= burning) of formate to CO2, and extract energy from this reaction in order to survive. Chemically, formate is one of the simplest hydrocarbons - it is already used as a chemical building block (feedstock) in industry, and formate 'fuel cells' are being developed. Turning a formate dehydrogenases 'in reverse' would turn CO2 into formate, a useful product. In fact, a small number of specialised bacteria use special 'tungsten-containing' FDHs to catalyse this reverse reaction - and live off the tiny amount of energy that they extract. In a pilot study we showed that the tungsten FDH from a bacterium called Syntrophobacter fumaroxidans can act as an extremely efficient electrically-driven catalyst for the reduction of CO2 to formate. In this project we aim to find out 'how the tungsten formate dehydrogenase does it'. We will start by looking for and characterising tungsten FDHs from different organisms, to find those that are the best for our experiments. Then we will apply sophisticated biochemical, electrochemical and physical techniques to aim to find out how they work - and why they work so well. Finally, we will compare our biological catalysts with available synthetic catalysts, aiming to find out how to improve the synthetic catalysts, and to develop 'demonstration devices' that show how efficient CO2 reduction catalysts can be powered by solar radiation and used in fuel cells.

二氧化碳（CO2）是由含碳分子（如化石燃料）燃烧产生的，用于电力工业，运输和我们的家庭。燃烧化石燃料不仅会导致大气中二氧化碳含量增加（二氧化碳是一种温室气体，也是全球变暖的主要原因），还会耗尽制造塑料、化学品、化肥所需的宝贵资源-以及现代社会的无数其他需求。不幸的是，二氧化碳是一种非常稳定和不活泼的分子，唯一已知的可以从大气中去除二氧化碳并利用它来再生含碳燃料的大规模过程是生物光合作用（种植植物和树木）。因此，一种可以利用太阳能或绿色电力资源将二氧化碳从大气中提取出来并将其转化为有用的燃料或化学品的工业过程将通过满足我们的能源和物质需求来彻底改变现代社会。当然，目前不存在这样的进程。本提案的目的是探索发展这一进程的新办法。一些细菌使用称为甲酸酯酶（FDH）的酶来催化甲酸盐氧化（=燃烧）为CO2，并从该反应中提取能量以存活。在化学上，甲酸盐是最简单的碳氢化合物之一-它已经在工业中用作化学构件（原料），甲酸盐“燃料电池”正在开发中。将甲酸脱氢酶“反向”转化将二氧化碳转化为甲酸盐，这是一种有用的产物。事实上，少数专门的细菌使用特殊的“含钨”FDH来催化这种逆反应-并依靠它们提取的少量能量生存。在一项初步研究中，我们表明，来自一种名为Syntrophobacteriumoxidans的细菌的钨FDH可以作为一种非常有效的电驱动催化剂，用于将CO2还原为甲酸盐。在这个项目中，我们的目标是找出“甲酸钨脱氢酶是如何做到这一点的”。我们将从寻找和表征来自不同生物体的钨FDH开始，以找到最适合我们实验的那些。然后，我们将应用复杂的生物化学，电化学和物理技术，旨在找出它们是如何工作的-以及为什么它们工作得这么好。最后，我们将比较我们的生物催化剂与现有的合成催化剂，旨在找出如何改善合成催化剂，并开发“示范装置”，显示如何有效的CO2还原催化剂可以通过太阳辐射供电，并用于燃料电池。