嗜热栖热菌细胞色素ba3与氰化物的反应：Fe(II)a3-CN.Cu(II)B-CN复合物的光谱表征表明四个14N原子与CuB配位。
Reaction of cyanide with cytochrome ba3 from Thermus thermophilus: spectroscopic characterization of the Fe(II)a3-CN.Cu(II)B-CN complex suggests four 14N atoms are coordinated to CuB.
作者信息
Surerus K K, Oertling W A, Fan C, Gurbiel R J, Einarsdóttir O, Antholine W E, Dyer R B, Hoffman B M, Woodruff W H, Fee J A
机构信息
Isotope and Structural Chemistry Group, University of California.
出版信息
Proc Natl Acad Sci U S A. 1992 Apr 15;89(8):3195-9. doi: 10.1073/pnas.89.8.3195.
Abstract
Cytochrome ba3 from Thermus thermophilus reacts slowly with excess HCN at pH 7.4 to create a form of the enzyme in which CuA, cytochrome b, and CuB remain oxidized, while cytochrome a3 is reduced by one electron, presumably with the formation of cyanogen. We have examined this form of the enzyme by UV-visible, resonance Raman, EPR, and electron nuclear double resonance spectroscopies in conjunction with permutations of 13C- and 15N-labeled cyanide. The results support a model in which one CN- binds through the carbon atom to ferrous a3, supporting a low-spin (S = 0) configuration on the Fe; bridging by this cyanide to the CuB is weak or absent. Four 14N atoms, presumably donated by histidine residues of the protein, provide a strong equatorial ligand field about CuB; a second CN- is coordinated through the carbon atom to CuB in an axial position.
摘要
嗜热栖热菌的细胞色素ba3在pH 7.4时与过量HCN反应缓慢，生成一种酶形式，其中CuA、细胞色素b和CuB保持氧化态，而细胞色素a3被一个电子还原，推测同时形成了氰。我们通过紫外可见光谱、共振拉曼光谱、电子顺磁共振光谱和电子核双共振光谱，并结合13C和15N标记氰化物的排列，对这种酶形式进行了研究。结果支持了一种模型，即一个CN-通过碳原子与亚铁a3结合，使Fe上形成低自旋（S = 0）构型；这种氰化物与CuB的桥连作用较弱或不存在。四个14N原子，推测由蛋白质的组氨酸残基提供，在CuB周围形成了一个强的赤道配体场；第二个CN-通过碳原子在轴向位置与CuB配位。
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本文引用的文献
1
Iron-carbon bond lengths in carbonmonoxy and cyanomet complexes of the monomeric hemoglobin III from Chironomus thummi thummi: a critical comparison between resonance Raman and x-ray diffraction studies.嗜尸摇蚊单体血红蛋白III的一氧化碳和氰化物配合物中的铁-碳键长：共振拉曼光谱与X射线衍射研究的关键比较
Proc Natl Acad Sci U S A. 1984 Aug;81(16):5106-10. doi: 10.1073/pnas.81.16.5106.
2
3
Mössbauer study of a bacterial cytochrome oxidase: cytochrome c1aa3 from Thermus thermophilus.嗜热栖热菌细菌细胞色素氧化酶的穆斯堡尔研究：细胞色素c1aa3
J Biol Chem. 1982 Nov 10;257(21):12489-92.
4
A study of the electron paramagnetic resonance properties of single monoclinic crystals of bovine superoxide dismutase.牛超氧化物歧化酶单斜晶体的电子顺磁共振特性研究。
J Biol Chem. 1982 Jan 10;257(1):336-44.
5
A study of the magnetic properties of haem a3 in cytochrome c oxidase by using magnetic-circular-dichroism spectroscopy.利用磁圆二色光谱研究细胞色素c氧化酶中血红素a3的磁性特性。
Biochem J. 1981 Mar 1;193(3):687-97. doi: 10.1042/bj1930687.
6
7
Cu (II)-carbon bonding in cyanide complexes of copper enzymes. 13C splitting of the Cu(II) electron spin resonance.铜酶氰化物配合物中的铜（II）-碳键。铜（II）电子自旋共振的13C分裂。
J Biol Chem. 1973 Oct 10;248(19):6626-9.
8
Studies of the metal sites of copper proteins. Symmetry of copper in bovine superoxide dismutase and its functional significance.
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9
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10
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