Mechanistic Investigation of CO activation by Nitrogenase

开发可持续的碳燃料来源，同时应对碳燃料燃烧产生的碳废物（CO和CO2）的积累，是相互竞争的全球挑战。有了这个奖项，化学系的生命过程化学项目资助了来自加州大学欧文分校的Markus Ribbe教授和Yilin Hu教授，研究固氮酶如何减少CO和CO2形成更大的碳氢化合物的详细化学机制。通过这项研究获得的知识为新型催化剂的设计提供了信息，这些催化剂可将碳废物回收为可用燃料，从而同时应对能源和环境相关问题。该项目为研究生研究人员以及研究生和本科生提供广泛的实验和计算技术的多学科教育和培训。通过在所有教育级别提供研究机会，并通过将微生物生物技术纳入课堂教学，将研究和教育结合起来。各种外展活动和计划的开发，包括科学星期六在加州大学欧文分校，从事中学生，包括那些来自代表性不足的少数民族社区，了解全球能源和环境问题，以及潜在的生物技术解决方案，这些problem.The无法产生不同的底物或中间绑定状态一直是固氮酶的机械调查的主要障碍。该提议利用一种新的方法将CO或CO衍生的中间体的结合与随后的周转解偶联，从而提供了一种独特的工具，用于通过控制电子/质子向CO或CO衍生的物质的传递来沿着CO还原的反应途径生成连续的快照。化学、生物化学和光谱学方法的战略组合将被用来分析这些定义的快照，希望（1）获得对CO转化为CH 4的C1途径的洞察;（2）定义第二个CO的结合和偶联的C1构象;以及（3）该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准。

Developing sustainable sources of carbon fuels while confronting the accumulation of carbon wastes (CO and CO2) from the combustion of carbon fuels are competing global challenges. With this award, the Chemistry of Life Processes Program in the Chemistry Division is funding Professor Markus Ribbe and Professor Yilin Hu from the University of California, Irvine, to investigate the detailed chemical mechanism for how the nitrogenase enzyme reduces CO and CO2 to form larger hydrocarbon compounds. The knowledge acquired through this research informs the design of novel catalysts that recycle carbon wastes into usable fuels, thereby simultaneously combating energy- and environment-related problems. This project provides multidisciplinary education and training across a broad range of experimental and computational techniques to postgraduate researchers, and graduate and undergraduate students. Research and education are integrated through research opportunities across all education levels and through incorporation of microbial biotechnology into classroom teaching. Various outreach events and programs are developed, including Science Saturdays at UC Irvine, to engage middle school students, including those from underrepresented minority communities, to learn about global energy and environmental problems, and potential biotechnological solutions to these problems.The inability to generate distinct substrate- or intermediate-bound states has remained a major roadblock for mechanistic investigations of nitrogenase. This proposal utilizes a novel approach to uncouple the binding of CO or CO-derived intermediates from the subsequent turnover, thereby providing a unique tool for the generation of successive snapshots along the reaction pathway of CO reduction via controlled delivery of electron(s)/proton(s) to CO or CO-derived species. A strategic combination of chemical, biochemical and spectroscopic approaches will then be used to analyze these defined snapshots in hopes of (1) obtaining insights into the C1 pathway that converts CO to CH4; (2) defining the C1 conformation for the binding and coupling of the second CO; and (3) identifying the mechanism of carbon chain extension.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.