Modeling the Catalytic Site of Nitrous Oxide Reductase

模拟一氧化二氮还原酶的催化位点

• 批准号: 6749533
• 负责人: ERIC C BROWN
• 金额: $ 4.3万
• 依托单位: UNIVERSITY OF MINNESOTA
• 依托单位国家: 美国
• 财政年份: 2003
• 资助国家: 美国
• 起止时间: 2003-07-01 至 2005-06-30
• 项目状态: 已结题
• 来源: https://reporter.nih.gov/project-details/6749533
• 关键词: Raman spectrometry; X ray crystallography; active sites; binding sites; catalyst; chemical kinetics; copper; electrochemistry; electron spin resonance spectroscopy; enzyme model; mass spectrometry; metalloenzyme; nitrate reductases; nitrous oxide; nuclear magnetic resonance spectroscopy; oxidation reduction reaction; postdoctoral investigator; synthetic enzyme; ultraviolet spectrometry

DESCRIPTION (provided by applicant): Nitrous oxide reductase (N2OR) is a homodimeric protein containing one dicopper site ("CUA") and one tetracopper site ("CuZ") per subunit. It is responsible for the catalytic two-electron reduction of N20 to N2 and is an important respiratory enzyme involved in ATP synthesis. The CuZ site of N2OR is proposed to be the catalytic site of the enzyme, yet little is known about the mechanism of reduction or oxidation states required for catalysis. The CuZ cluster contains a distorted tetrahedral ?4-sulfide bound to four copper atoms and is the only example of a N-sulfide tetranuclear copper cluster observed in nature. The goal of this research proposal is the synthetic design of novel model compounds, which mimic the structural arrangement, spectroscopic properties, and reactivity of the CuZ site in N2OR. Comparisons between the model compounds and the natural enzyme will be made to better understand certain properties, such as the unusual spectroscopic properties, redox behavior and reactivity, associated with the enzyme. The generation of mixed valence synthetic models that resemble the different forms of N2OR will be examined as well.

描述（由申请人提供）：一二氮还原酶（N2OR）是一个含有一个二氧化碳位点（“ CUA”）和一个四型tetracopper位点（“ CUZ”）的同型二聚体蛋白。它负责催化N20至N2的催化两电子还原，并且是参与ATP合成的重要呼吸酶。认为N2OR的CUZ位点是酶的催化位点，但对催化所需的还原或氧化状态的机理知之甚少。 CUZ簇包含一个与四个铜原子结合的四面体的四面体？4-硫化物，这是在本质上观察到的N硫化物四核铜簇的唯一例子。该研究建议的目的是新型模型化合物的合成设计，它们模仿了N2OR中CUZ位点的结构排列，光谱特性和反应性。将进行模型化合物与天然酶之间的比较，以更好地理解某些特性，例如与酶相关的异常光谱特性，氧化还原行为和反应性。也将研究类似于不同形式的N2OR的混合价合成模型的产生。