Low Coordinate Fe(I) Species as Functional Mimics of Nitrogenase Enzymes.

低配位 Fe(I) 物种作为固氮酶的功能模拟物。

基本信息

  • 批准号:
    EP/H006990/1
  • 负责人:
  • 金额:
    $ 12.97万
  • 依托单位:
  • 依托单位国家:
    英国
  • 项目类别:
    Research Grant
  • 财政年份:
    2010
  • 资助国家:
    英国
  • 起止时间:
    2010 至 无数据
  • 项目状态:
    已结题

项目摘要

Nitrogen is the most abundant gas in the atmosphere. It is industrially converted on an immense scale for use in a variety of nitrogen containing materials, particularly in fertilizers that ensure there is sufficient global food production to support the ever growing population. The current industrial method, the Haber Bosch process, operates under intense gas pressure (150 to 350 atmospheres), at raised temperatures (350 to 550 C), and requires hydrogen (currently produced from hydrocarbon sources) to transform nitrogen into the useful precursor compound ammonia. This renders the process incredibly energy (and therefore cost) intensive, consuming ~2 % of the world's energy supply and ~3-5 % of the world's natural gas supply. In stark contrast nature, the synthetic chemist par excellence, performs the same conversion under drastically milder conditions (1 atmosphere pressure and mild temperatures). Mimicking nature's achievement would be a dramatic breakthrough, not only as a stand alone scientific achievement but also in potentially revolutionising the industrial production of ammonia from atmospheric nitrogen. As such a considerable effort has been expended into elucidating how the metal containing nitrogenase (nitrogen transforming) enzymes achieve this conversion. Recent findings have begun to clarify some aspects of the complex nitrogenase catalyst, particularly the identity of the resting state of this enzyme (the structure when it is not actively converting nitrogen to ammonia). These recent experimental findings combined with computational studies provide insight and inspiration for the synthetic chemist revealing the nitrogenase contains a number of highly unusual features. They also highlight how far from nature's evolved solution humankind's current systems are, perhaps explaining our current dependence on catalysts requiring very severe conditions. The research in this proposal involves the synthesis of new functional model systems that possess the vital (and unusual) features recently identified in the nitrogenase enzymes. The generation of accurate model complexes is a crucial step in elucidating enzyme mechanisms; our simplified model systems will enable the systematic study of crucial parameters that are very difficult to study directly in the very complex enzyme structure. It is imperative to understand these parameters as they are key to the facile transformation of nitrogen. Studies of this nature are particularly important for the nitrogenase enzyme as its operating mechanism is experimentally poorly defined, with only the inactive resting state physically characterised. This body of work therefore will afford a fundamental comprehension of the crucial factors required to achieve the fixation and functionalisation of atmospheric nitrogen under mild conditions. If we understand how nitrogen is converted to ammonia by metallo-enzymes then we have taken a giant leap towards being able to achieve our goal of following in nature's footsteps; and ultimately being able to take nitrogen out of the air and readily transform it, under mild conditions, into products essential to every day life.
氮是大气中最丰富的气体。它被大规模地工业化转化,用于各种含氮材料,特别是肥料,以确保全球粮食生产足以支持不断增长的人口。目前的工业方法,即哈伯-博施法,在高气压(150至350个大气压)下,在升高的温度(350至550 ℃)下操作,并且需要氢气(目前由烃源产生)将氮气转化为有用的前体化合物氨。这使得该过程非常能源密集(因此成本),消耗世界能源供应的约2%和世界天然气供应的约3- 5%。与大自然形成鲜明对比的是,卓越的合成化学家在非常温和的条件下(1个大气压和温和的温度)进行相同的转化。模仿大自然的成就将是一个巨大的突破,不仅是一项独立的科学成就,而且可能彻底改变从大气中的氮中生产氨的工业生产。因此,已经花费了相当大的努力来阐明含金属的固氮酶(氮转化)如何实现这种转化。最近的发现已经开始澄清复合固氮酶催化剂的某些方面,特别是这种酶的静止状态的身份(当它不主动将氮转化为氨时的结构)。这些最近的实验发现与计算研究相结合,为合成化学家提供了洞察力和灵感,揭示了固氮酶包含许多非常不寻常的特征。他们还强调了人类目前的系统与自然进化的解决方案有多远,也许可以解释我们目前对催化剂的依赖需要非常苛刻的条件。这项研究涉及合成新的功能模型系统,这些系统具有最近在固氮酶中发现的重要(和不寻常)特征。精确的模型复合物的生成是阐明酶机制的关键步骤;我们简化的模型系统将使系统研究非常复杂的酶结构中很难直接研究的关键参数成为可能。理解这些参数是必要的,因为它们是氮的简单转化的关键。这种性质的研究对于固氮酶特别重要,因为它的操作机制在实验上定义得很差,只有不活跃的静止状态的物理特征。因此,这项工作将提供一个基本的理解所需的关键因素,以实现在温和条件下的大气氮的固定和功能化。如果我们理解了氮是如何通过金属酶转化为氨的,那么我们就朝着能够实现跟随大自然脚步的目标迈出了一大步;最终能够从空气中提取氮,并在温和的条件下将其转化为日常生活中必不可少的产品。

项目成果

期刊论文数量(3)
专著数量(0)
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Michael Ingleson其他文献

Michael Ingleson的其他文献

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{{ truncateString('Michael Ingleson', 18)}}的其他基金

New Routes to fluorocarbons using fluoroboranes
使用氟硼烷生产碳氟化合物的新途径
  • 批准号:
    EP/X021858/1
  • 财政年份:
    2023
  • 资助金额:
    $ 12.97万
  • 项目类别:
    Research Grant
Catalysing 3 routes to C-H Borylation using Earth-abundant Metals
使用地球丰富的金属催化 C-H 硼化反应的 3 条路线
  • 批准号:
    EP/V03829X/1
  • 财政年份:
    2021
  • 资助金额:
    $ 12.97万
  • 项目类别:
    Research Grant
Cationic Carbon Lewis Acids in Frustrated Lewis Pairs as New Reduction Catalysts
受阻路易斯对中的阳离子碳路易斯酸作为新的还原催化剂
  • 批准号:
    EP/M023346/1
  • 财政年份:
    2015
  • 资助金额:
    $ 12.97万
  • 项目类别:
    Research Grant
Direct Alkene and Alkyne Borylation with Borenium Cations
用硼阳离子直接进行烯烃和炔烃硼化
  • 批准号:
    EP/J000973/1
  • 财政年份:
    2012
  • 资助金额:
    $ 12.97万
  • 项目类别:
    Research Grant

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