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: 6646050
• 负责人: ERIC C BROWN
• 金额: $ 3.97万
• 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
• 项目状态: 未结题
• 来源: https://reporter.nih.gov/project-details/6646050
• 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）：一氧化二氮还原酶（N2OR）是一种同型二聚体蛋白质，每个亚基含有一个二铜位点（“CUA”）和一个四铜位点（“CuZ”）。它负责将 N20 催化双电子还原为 N2，是参与 ATP 合成的重要呼吸酶。 N2OR 的 CuZ 位点被认为是该酶的催化位点，但对于催化所需的还原或氧化态的机制知之甚少。 CuZ簇包含与四个铜原子结合的扭曲四面体β4-硫化物，并且是自然界中观察到的N-硫化物四核铜簇的唯一例子。本研究计划的目标是合成设计新型模型化合物，模拟 N2OR 中 CuZ 位点的结构排列、光谱特性和反应性。将模型化合物和天然酶之间进行比较，以更好地了解与酶相关的某些特性，例如不寻常的光谱特性、氧化还原行为和反应性。类似于不同形式的 N2OR 的混合价合成模型的生成也将被检查。