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细胞色素氧化酶中向双核中心的电子转移：催化意义及另一种中间体的证据

Electron transfer to the binuclear center in cytochrome oxidase: catalytic significance and evidence for an additional intermediate.

作者信息

Malatesta F, Sarti P, Antonini G, Vallone B, Brunori M

机构信息

Department of Experimental Medicine and Biochemical Sciences, University of Rome Tor Vergata, Italy.

出版信息

Proc Natl Acad Sci U S A. 1990 Oct;87(19):7410-3. doi: 10.1073/pnas.87.19.7410.

DOI:10.1073/pnas.87.19.7410
PMID:2170978
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC54756/
Abstract

We have followed, by transient kinetics, the reduction of cytochrome a3 in the presence of carbon monoxide under different experimental conditions. We have observed that the internal electron transfer rate accounts for the turnover number, and both display the same pH and temperature dependence [pKa = 7.4 and activation energy (Ea) = 14.7 +/- 0.1 kcal/mol]. Moreover, comparison of the time course of cytochrome c oxidation and cytochrome a3 reduction indicates that two electrons are transferred internally and with different rates to the oxygen-binding site. A kinetic model based on sequential internal electron transfer pathways, describing quantitatively the experimental data, is presented and discussed.

摘要

我们通过瞬态动力学方法，在不同实验条件下，追踪了一氧化碳存在时细胞色素a3的还原过程。我们观察到内部电子传递速率决定了周转数，并且二者都表现出相同的pH和温度依赖性[pKa = 7.4，活化能(Ea) = 14.7 +/- 0.1千卡/摩尔]。此外，细胞色素c氧化和细胞色素a3还原的时间进程比较表明，有两个电子在内部以不同速率传递到氧结合位点。本文提出并讨论了一个基于连续内部电子传递途径的动力学模型，该模型对实验数据进行了定量描述。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5753/54756/f5f17de22dac/pnas01044-0074-a.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5753/54756/f5f17de22dac/pnas01044-0074-a.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5753/54756/f5f17de22dac/pnas01044-0074-a.jpg

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本文引用的文献

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Reactions of cytochrome oxidase with oxygen and carbon monoxide.细胞色素氧化酶与氧气和一氧化碳的反应。
Biochem J. 1963 Mar;86(3):541-54. doi: 10.1042/bj0860541.
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Studies on cytochrome oxidase. III. Improved preparation and some properties.细胞色素氧化酶的研究。III. 改进的制备方法及某些特性。
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Kinetic characterization of the interaction between cytochrome oxidase and cytochrome c.细胞色素氧化酶与细胞色素c相互作用的动力学特征
细胞色素c氧化酶：结构氢离子在能量转导中的机制意义
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Electron transfer kinetics of caa3 oxidase from Bacillus stearothermophilus: a hypothesis for thermophilicity.嗜热脂肪芽孢杆菌caa3氧化酶的电子转移动力学：嗜热性假说
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Investigating the mechanism of electron transfer to the binuclear center in Cu-heme oxidases.研究电子转移至铜-血红素氧化酶双核中心的机制。
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Probing the high-affinity site of beef heart cytochrome c oxidase by cross-linking.通过交联反应探究牛心细胞色素c氧化酶的高亲和力位点
Biochem J. 1996 May 1;315 ( Pt 3)(Pt 3):909-16. doi: 10.1042/bj3150909.
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Discrete steps in dioxygen activation--the cytochrome oxidase/O2 reaction.双氧激活的离散步骤——细胞色素氧化酶/O₂反应
J Bioenerg Biomembr. 1993 Apr;25(2):71-80. doi: 10.1007/BF00762849.
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Multiwavelength analysis of the kinetics of reduction of cytochrome aa3 by cytochrome c.细胞色素c还原细胞色素aa3动力学的多波长分析
Biophys J. 1993 Sep;65(3):1307-17. doi: 10.1016/S0006-3495(93)81170-6.
9
What form of cytochrome c oxidase reacts with oxygen in vivo?哪种形式的细胞色素c氧化酶在体内与氧气发生反应？
Biochem J. 1992 Dec 15;288 ( Pt 3)(Pt 3):1070-2. doi: 10.1042/bj2881070.
10
Respiratory control in cytochrome oxidase vesicles is correlated with the rate of internal electron transfer.细胞色素氧化酶囊泡中的呼吸控制与内部电子传递速率相关。
Biochem J. 1992 May 15;284 ( Pt 1)(Pt 1):123-7. doi: 10.1042/bj2840123.
J Biol Chem. 1982 Jun 10;257(11):6194-206.
4
A plausible two-state model for cytochrome c oxidase.细胞色素c氧化酶的一种合理双态模型。
Proc Natl Acad Sci U S A. 1981 Nov;78(11):7115-8. doi: 10.1073/pnas.78.11.7115.
5
Catalytic mechanism of cytochrome oxidase.细胞色素氧化酶的催化机制。
Nature. 1970 Dec 5;228(5275):936-7. doi: 10.1038/228936a0.
6
Is the internal electron transfer the rate-limiting step in the catalytic cycle of cytochrome c oxidase?内部电子转移是细胞色素c氧化酶催化循环中的限速步骤吗？
Ann N Y Acad Sci. 1988;550:161-6. doi: 10.1111/j.1749-6632.1988.tb35332.x.
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Structure and function of cytochrome oxidase: a second look.细胞色素氧化酶的结构与功能：再审视
Adv Inorg Biochem. 1988;7:93-153.
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Long-range electron transfer in multisite metalloproteins.多位点金属蛋白中的长程电子转移
Biochemistry. 1989 Sep 19;28(19):7499-505. doi: 10.1021/bi00445a001.
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Electron transfer process in cytochrome oxidase after pulse radiolysis.脉冲辐解后细胞色素氧化酶中的电子转移过程。
J Biol Chem. 1989 May 15;264(14):7976-80.
10
Oxidation of cytochrome c by cytochrome c oxidase: spectroscopic binding studies and steady-state kinetics support a conformational transition mechanism.细胞色素c氧化酶对细胞色素c的氧化作用：光谱结合研究和稳态动力学支持一种构象转变机制。
Biochemistry. 1989 Jan 10;28(1):244-52. doi: 10.1021/bi00427a034.