RUI: Photochemical and Kinetic Studies of Iron-Only Hydrogenase Model Compounds

RUI：纯铁氢化酶模型化合物的光化学和动力学研究

• 批准号: 1057808
• 负责人: Carmen Works
• 金额: $ 12.98万
• 依托单位: Sonoma State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2011
• 资助国家: 美国
• 起止时间: 2011-09-01 至 2015-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1057808&HistoricalAwards=false
• 关键词: RUI; Photochemical; Kinetic; Studies; Iron

In this project funded by the Chemical Catalysis Program of the Chemistry Division, Carmen Works of Sonoma State University will study the mechanism of catalyzed reversible oxidation of molecular hydrogen in model compounds of iron-only hydrogenases. The approach is to first synthesize dimeric iron complex models of the enzyme active site, and then to use these molecules to test the hypothesis that light labilizes CO in these complexes to produce a model for the uninhibited form of the enzyme active site and that the coordination site of CO is occupied by a solvent molecule. The series of experiments to be performed include: CO dependent kinetics of the reactions of the photoproduct, kinetic solvent effects, temperature studies to determine activation parameters, spectroscopic analysis to monitor reactions of the photoproduct with molecular hydrogen, and quantum yield determinations. The broader impacts involve training undergraduate students in research methods, incorporating relevant materials into lecture and laboratory courses, and broadly disseminating the research results via publications and presentations at conferences. This work will deepen our understanding of biological enzymes that utilize and generate hydrogen. Potential longer term impacts of the work could involve developing efficient methods to generate hydrogen as a clean fuel source and to use hydrogen in fuel cells.

索诺玛州立大学的Carmen Works将在化学系化学催化项目资助下，研究纯铁氢化酶模型化合物中分子氢催化可逆氧化的机理。方法是首先合成酶活性位点的二聚体铁配合物模型，然后利用这些分子来验证光稳定这些配合物中的CO的假设，从而产生酶活性位点的不受抑制形式的模型，并且CO的配位位点被溶剂分子占据。要进行的一系列实验包括：光产物反应的CO依赖动力学、溶剂动力学效应、确定活化参数的温度研究、监测光产物与氢分子反应的光谱分析和量子产率测定。更广泛的影响包括培训本科生的研究方法，将相关材料纳入讲座和实验课程，并通过出版物和会议报告广泛传播研究成果。这项工作将加深我们对利用和产生氢的生物酶的理解。这项工作的潜在长期影响可能包括开发有效的方法来产生氢作为清洁燃料来源，并在燃料电池中使用氢。