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CAREER: CO2 activation by nitrogenase Fe proteins

职业：固氮酶 Fe 蛋白活化 CO2

基本信息

批准号：
1651398
负责人：
Yilin Hu
金额：
$ 70万
依托单位：
University of California-Irvine
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2017
资助国家：
美国
起止时间：
2017-07-01 至 2023-06-30
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1651398&HistoricalAwards=false
关键词：
CAREER CO2 activation nitrogenase Fe

项目摘要

With this award, the Chemistry of Life Processes Program in the Chemistry Division is funding Dr. Yilin Hu from the University of California, Irvine, to investigate carbon dioxide activation by the iron protein of nitrogenase, the enzyme responsible for nitrogen fixation in microorganisms. Conversion of the greenhouse gas carbon dioxide into valuable chemicals represents an effective strategy to simultaneously combat the problems of increased carbon dioxide emission into the atmosphere and the decreased supply of fossil fuels. However, activation or splitting of carbon dioxide normally requires high temperature and pressure conditions, which puts a tremendous burden on our energy supply and environmental wellness. This pursuit focuses on just how the reaction takes place by a simple iron-sulfur enzyme, which will provide a crucial framework for future adaptations of this novel type of reaction for recycling the greenhouse gas carbon dioxide into useful products. As such, it has broad scientific impacts on our society by addressing two of the most important challenges we face nowadays: fossil fuel depletion and climate change. In addition, incorporation of this research into training of current students and outreach to prospective students raises public interest and awareness of the importance of this line of research and, therefore, has broader impacts on the education of future generations.This project investigates the mechanism of in vitro carbon dioxide activation by the iron protein of nitrogenase and the engineering of an Azotobacter vinelandii strain with improved efficiency of in vivo carbon dioxide reduction upon expression of the iron protein. Guided by theoretical calculations, the proposed research employs a combination of genetic, biochemical, spectroscopic and structural approaches to tackle the unique reaction of carbon dioxide reduction by the all-ferrous iron protein and address several fundamental questions related to the mechanism of this reaction. Further, a combination of screening and expression strategies are used to identify iron proteins or homologs with higher efficiencies of carbon dioxide reduction and improve the specificity of electron transfer to the iron protein during the process of carbon dioxide reduction. The outcome of these studies provides important insights into how iron-sulfur based catalysts work to effect carbon dioxide activation and reduction under ambient conditions and what principles can be derived from studies of A. vinelandii for future development of cost-efficient, whole-cell-based strategies for carbon dioxide conversion.

有了这个奖项，化学部的生命过程化学项目资助了加州大学欧文分校的Yilin Hu博士，研究固氮酶的铁蛋白对二氧化碳的活化作用，固氮酶是微生物中负责固氮的酶。将温室气体二氧化碳转化为有价值的化学品是一种有效的战略，可以同时解决向大气中排放的二氧化碳增加和化石燃料供应减少的问题。然而，二氧化碳的活化或分解通常需要高温和高压条件，这给我们的能源供应和环境健康带来了巨大的负担。这项研究的重点是简单的铁硫酶如何发生反应，这将为未来适应这种新型反应，将温室气体二氧化碳回收为有用的产品提供重要的框架。因此，它通过解决我们当今面临的两个最重要的挑战对我们的社会产生了广泛的科学影响：化石燃料耗尽和气候变化。此外，将这项研究纳入对现有学生的培训和对未来学生的宣传，提高了公众对这一研究领域重要性的兴趣和认识，因此，本项目研究固氮酶铁蛋白体外激活二氧化碳的机制，并对棕色固氮菌进行基因工程改造，铁蛋白表达后体内二氧化碳减少。在理论计算的指导下，拟议的研究采用遗传，生物化学，光谱和结构方法相结合的方法来解决全亚铁铁蛋白还原二氧化碳的独特反应，并解决与该反应机制相关的几个基本问题。此外，使用筛选和表达策略的组合来鉴定具有更高二氧化碳还原效率的铁蛋白或同源物，并提高在二氧化碳还原过程中电子转移到铁蛋白的特异性。这些研究的结果提供了重要的见解，如何铁硫基催化剂的工作，以影响二氧化碳的活化和还原在环境条件下，什么原则可以从A. vinelandii为未来开发具有成本效益的，基于全细胞的二氧化碳转化策略。

项目成果

期刊论文数量（17）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Mackinawite‐Supported Reduction of C 1 Substrates into Prebiotically Relevant Precursors

Mackinawite — 支持将 C 1 底物还原为益生元相关前体

DOI：
10.1002/syst.202200010
发表时间：
2022
期刊：
ChemSystemsChem
影响因子：
0
作者：
Grosch, Mario;Stiebritz, Martin T.;Bolney, Robert;Winkler, Mario;Jückstock, Eric;Busch, Hannah;Peters, Sophia;Siegle, Alexander F.;van Slageren, Joris;Ribbe, Markus
通讯作者：
Ribbe, Markus

Structural and Mechanistic Insights into CO 2 Activation by Nitrogenase Iron Protein

固氮酶铁蛋白激活 CO 2 的结构和机制见解

DOI：
10.1002/chem.201903387
发表时间：
2019
期刊：
Chemistry – A European Journal
影响因子：
0
作者：
Rettberg, Lee A.;Stiebritz, Martin T.;Kang, Wonchull;Lee, Chi Chung;Ribbe, Markus W.;Hu, Yilin
通讯作者：
Hu, Yilin

Special Issue on Nitrogenases and Homologous Systems

固氮酶和同源系统特刊