Synthetic Modeling of Copper Protein Active Sites

铜蛋白活性位点的综合建模

基本信息

  • 批准号:
    7258964
  • 负责人:
  • 金额:
    $ 29.56万
  • 依托单位:
  • 依托单位国家:
    美国
  • 项目类别:
  • 财政年份:
    1992
  • 资助国家:
    美国
  • 起止时间:
    1992-08-01 至 2008-07-31
  • 项目状态:
    已结题

项目摘要

DESCRIPTION (provided by applicant): Proteins that contain copper ions in their active sites represent a large and functionally significant class of metallobiomolecules that play important roles in a wide range of life processes. The functional diversity of copper proteins is matched by variability in active site geometric, electronic structural, and spectroscopic features. A molecular level understanding of structure/function relationships is desirable, but despite extensive research efforts many issues remain unresolved regarding the detailed mechanisms of action and underlying chemistry of copper protein active sites. The aim of the proposed research is to obtain essential chemical insights into copper protein structure and function and to develop novel and fundamentally significant copper chemistry through the synthetic modeling approach, wherein low molecular weight complexes designed to replicate metalloprotein active site properties are characterized and their reactivity studied. The specific aims of the proposed research are to: 1. Understand the interrelationships of the variable structures and redox behaviors of type 1 copper electron transfer sites found in numerous metalloproteins. Perturbations of copper-thiolate complex properties and electron transfer kinetics of ruthenium and/or rhenium/copper-thiolate assemblies will be examined. 2. Obtain fundamental insight into dioxygen activation by monocopper sites in biologically important proteins such as dopamine beta-monooxygenase and galactose oxidase through studies of the O2 reactivity of copper complexes of hindered bidentate N-donor ligands, phenolate chelates, and ligands with attached remote oxidants like those operative in catalysis by copper enzymes. 3. Investigate dioxgyen activation by the tricopper active sites of the ubiquitous and biologically significant multicopper oxidases by using a novel stepwise synthetic strategy involving the reaction of 1:1 Cu/O2 species with dicopper complexes. 4. Understand the underlying chemistry of the novel (mu-sulfido)tetracopper active site of nitrous oxide reductase, an important participant in the global nitrogen cycle. Parallel studies will be performed of various mono- and disulfido-bridged dicopper complexes and of specifically designed tetracopper clusters.
描述(申请人提供):在活性部位含有铜离子的蛋白质代表了一大类具有重要功能的金属生物分子,它们在广泛的生命过程中扮演着重要的角色。铜蛋白的功能多样性与活性中心几何、电子结构和光谱特征的多样性相匹配。对结构/功能关系的分子水平的了解是可取的,但尽管进行了广泛的研究,但关于铜蛋白活性位点的详细作用机制和潜在化学仍有许多问题尚未解决。这项研究的目的是通过合成模拟的方法,获得对铜蛋白质结构和功能的基本化学见解,并发展新的和根本上有意义的铜化学,其中设计用于复制金属蛋白活性中心性质的低分子络合物被表征,并研究它们的反应性。这项研究的具体目的是:1.了解在众多金属蛋白中发现的第一类铜电子转移位点的可变结构与氧化还原行为之间的相互关系。将考察铜-硫酸盐络合物性质的扰动和Ru和/或Re/铜-硫酸盐组件的电子转移动力学。2.通过研究受阻的双齿N-供体配体的铜配合物、酚类螯合物以及与远端氧化剂连接的配体(如铜酶催化的那些配体)的氧反应活性,获得对生物重要蛋白质如多巴胺-β-单加氧酶和半乳糖氧化酶等生物重要蛋白质中单铜位置激活氧的基本认识。3.采用1:1铜/氧物种与二铜络合物反应的新的分步合成策略,研究了普遍存在的、具有生物意义的多铜氧化酶的三拷贝活性中心对二氧杂环己烯的激活作用。4.了解全球氮循环中的重要参与者--一氧化二氮还原酶新的(Mu-硫代)四铜活性部位的基本化学。将对各种一硫和二硫桥联的双铜络合物以及专门设计的四铜簇合物进行平行研究。

项目成果

期刊论文数量(0)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)

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WILLIAM B Tolman其他文献

WILLIAM B Tolman的其他文献

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{{ truncateString('WILLIAM B Tolman', 18)}}的其他基金

2011-2013 Metals in Biology GRC and Bioinorganic GRS
2011-2013 生物GRC和生物无机GRS中的金属
  • 批准号:
    8197758
  • 财政年份:
    2010
  • 资助金额:
    $ 29.56万
  • 项目类别:
2011-2013 Metals in Biology GRC and Bioinorganic GRS
2011-2013 生物GRC和生物无机GRS中的金属
  • 批准号:
    8045631
  • 财政年份:
    2010
  • 资助金额:
    $ 29.56万
  • 项目类别:
2011-2013 Metals in Biology GRC and Bioinorganic GRS
2011-2013 生物GRC和生物无机GRS中的金属
  • 批准号:
    8394937
  • 财政年份:
    2010
  • 资助金额:
    $ 29.56万
  • 项目类别:
Synthetic Modeling of Copper Protein Active Sites
铜蛋白活性位点的综合建模
  • 批准号:
    7924288
  • 财政年份:
    2009
  • 资助金额:
    $ 29.56万
  • 项目类别:
SYNTHETIC MODELING OF COPPER PROTEIN ACTIVE SITES
铜蛋白活性位点的综合建模
  • 批准号:
    6192240
  • 财政年份:
    1992
  • 资助金额:
    $ 29.56万
  • 项目类别:
SYNTHETIC MODELING OF COPPER PROTEIN ACTIVE SITES
铜蛋白活性位点的综合建模
  • 批准号:
    6018887
  • 财政年份:
    1992
  • 资助金额:
    $ 29.56万
  • 项目类别:
Synthetic Modeling of Copper Protein Active Sites
铜蛋白活性位点的综合建模
  • 批准号:
    7108007
  • 财政年份:
    1992
  • 资助金额:
    $ 29.56万
  • 项目类别:
Synthetic Modeling of Copper Protein Active Sites
铜蛋白活性位点的综合建模
  • 批准号:
    10217146
  • 财政年份:
    1992
  • 资助金额:
    $ 29.56万
  • 项目类别:
Synthetic Modeling of Copper Protein Active Sites
铜蛋白活性位点的综合建模
  • 批准号:
    9320793
  • 财政年份:
    1992
  • 资助金额:
    $ 29.56万
  • 项目类别:
SYNTHETIC MODELING OF COPPER PROTEIN ACTIVE SITES
铜蛋白活性位点的综合建模
  • 批准号:
    6642860
  • 财政年份:
    1992
  • 资助金额:
    $ 29.56万
  • 项目类别:

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