Brittain T, Greenwood C
Biochem J. 1975 Jul;149(1):179-85. doi: 10.1042/bj1490179.
The reduction of 2-hydroxy-5-nitrobenzyl tryptophyl cytochrome c by the chromous ion was studied by stopped-flow techniques. At pH6.5 the reduction of 2-hydroxy-5-nitrobenzyl tryptophyl cytochrome c is complex, showing the presence of three distinct phases. Two chromium concentration-dependent phases are observed (1.1 X 10(5) M-1-S-1, phase 1; 1.25 X 10(4)M-1-S-1, phase 2) and one slow first-order process (0.25S-1, phase 3). A comparison of the static and kinetic difference spectra, along with the data from the reduction of the reoxidized reduced protein, suggests that the slow chromium concentration-independent phase is due to a slow conformational event after fast reduction of the NO2 group. The rates of the chromium concentration-dependent phases show a marked variation with pH above 7.5. The activation energies for the three processes were also measured at 33.2, 38.6 and 69.7 kJ-mol-1 for phases 1, 2 and 3 respectively. The reaction of reduced 2-hydroxy-5-nitrobenzyl tryptophyl cytochrome c with CO was foollowed by means of both stopped-flow and flash photolysis. The combination with CO at pH 6.8 as measured in stopped-flow experiments showed two phases, one CO-dependent phase (phase 2, 2.4 X 10(2)M-1-S-1) and one CO-independent phase (phase 1, 0.015S-1). Investigation of the pH-dependence of the phases showed both the rates and amounts of each phase to be pH-invariant. CO recombination, after photolytic removal, was found to be biphasic; a CO-dependent phase (phase 2, 2.4 X 10(2)M-1-S-1) and a CO-independent phase (phase 1, 1.0s-1) were observed. A tentative model which can accommodate these observations is proposed.
采用停流技术研究了亚铬离子对2-羟基-5-硝基苄基色氨酰细胞色素c的还原作用。在pH6.5时,2-羟基-5-硝基苄基色氨酰细胞色素c的还原过程较为复杂,呈现出三个不同的阶段。观察到两个铬浓度依赖性阶段(1.1×10⁵M⁻¹·s⁻¹,阶段1;1.25×10⁴M⁻¹·s⁻¹,阶段2)和一个缓慢的一级过程(0.25s⁻¹,阶段3)。静态和动力学差光谱的比较,以及再氧化还原蛋白还原数据表明,缓慢的铬浓度非依赖性阶段是由于NO₂基团快速还原后发生的缓慢构象变化所致。在pH高于7.5时,铬浓度依赖性阶段的速率随pH有显著变化。三个过程的活化能在阶段1、2和3分别测定为33.2、38.6和69.7kJ·mol⁻¹。采用停流和闪光光解技术研究了还原型2-羟基-5-硝基苄基色氨酰细胞色素c与CO的反应。在停流实验中测得的pH6.8时与CO的结合呈现两个阶段,一个CO依赖性阶段(阶段2,2.4×10²M⁻¹·s⁻¹)和一个CO非依赖性阶段(阶段1,0.015s⁻¹)。对各阶段pH依赖性的研究表明,每个阶段的速率和量均与pH无关。光解去除后CO的重新结合是双相的;观察到一个CO依赖性阶段(阶段2,2.4×10²M⁻¹·s⁻¹)和一个CO非依赖性阶段(阶段1,1.0s⁻¹)。提出了一个能够解释这些观察结果的初步模型。