Hrycay E G, Gustafsson J A, Ingelman-Sundberg M, Ernster L
Eur J Biochem. 1976 Jan 2;61(1):43-52. doi: 10.1111/j.1432-1033.1976.tb09995.x.
The mechanism of steroid hydroxylation in rat liver microsomes has been investigated by employing NaIO4, NaClO2, and various organic hydroperoxides as hydroxylating agents and comparing the reaction rates and steroid products formed with those of the NADPH-dependent reaction. Androstenedione, testosterone, progesterone, and 17beta-estradiol were found to act as good substrates. NaIO4 was by far the most effective hydroxylating agent followed by cumene hydroperoxide, NADPH, NaClO2, pregnenolone 17alpha-hydroperoxide, tert-butyl hydroperoxide, and linoleic acid hydroperoxide. Androstenedione was chosen as the model substrate for inducer and inhibitor studies. The steroid was converted to its respective 6beta-, 7alpha, 15-, and 16alpha-hydroxy derivatives when incubated with microsomal fractions fortified with hydroxylating agent. Evidence for cytochrome P-450 involvement in androstenedione hydroxylation included a marked inhibition by substrates and modifiers of cytochrome P-450 and by reagents which convert cytochrome P-450 to cytochrome P-420. The ratios of the steroid products varied according to the type of hydroxylating agent used and were also modified by in vivo phenobarbital pretreatment. It was suggested that multiple forms of cytochrome P-450 exhibiting different affinities for hydroxylating agent are responsible for these different ratios. Horse-radish peroxidase, catalase, and metmyoglobin could not catalyze androstenedione hydroxylation. Addition of NaIO4, NaClO2, cumene hydroperoxide and other organic hydroperoxides to microsomal suspensions resulted in the appearance of a transient spectral change in the difference spectrum characterized by a peak at about 440 nm and a trough at 420 nm. The efficiency of these oxidizing agents in promoting steroid hydroxylation in microsomes appeared to be related to their effectiveness in eliciting the spectral complex. Electron donors, substrates, and modifiers of cytochrome P-450 greatly diminished the magnitude of the spectral change. It is proposed that NaIO4, NaClO2, and organic hydroperoxides promote steroid hydroxylation by forming a transient ferryl ion (compound I) of cytochrome P-450 which may be the common intermediate hydroxylating species involved in hydroxylations catalyzed by cytochrome P-450.
通过使用高碘酸钠(NaIO4)、亚氯酸钠(NaClO2)和各种有机氢过氧化物作为羟化剂,并将反应速率和生成的甾体产物与依赖于烟酰胺腺嘌呤二核苷酸磷酸(NADPH)的反应进行比较,对大鼠肝微粒体中甾体羟化的机制进行了研究。发现雄烯二酮、睾酮、孕酮和17β-雌二醇是良好的底物。高碘酸钠是迄今为止最有效的羟化剂,其次是氢过氧化异丙苯、NADPH、亚氯酸钠、孕烯醇酮17α-氢过氧化物、叔丁基氢过氧化物和亚油酸氢过氧化物。选择雄烯二酮作为诱导剂和抑制剂研究的模型底物。当与用羟化剂强化的微粒体部分一起孵育时,该甾体被转化为其相应的6β-、7α-、15-和十六α-羟基衍生物。细胞色素P-450参与雄烯二酮羟化的证据包括细胞色素P-450的底物和调节剂以及将细胞色素P-450转化为细胞色素P-420的试剂的显著抑制作用。甾体产物的比例根据所用羟化剂的类型而变化,并且也受到体内苯巴比妥预处理的影响。有人提出,对羟化剂表现出不同亲和力的多种形式的细胞色素P-450是造成这些不同比例的原因。辣根过氧化物酶、过氧化氢酶和高铁肌红蛋白不能催化雄烯二酮的羟化。向微粒体悬浮液中添加高碘酸钠、亚氯酸钠、氢过氧化异丙苯和其他有机氢过氧化物导致差示光谱中出现瞬时光谱变化,其特征是在约440nm处有一个峰,在420nm处有一个谷。这些氧化剂促进微粒体中甾体羟化的效率似乎与其引发光谱复合物的有效性有关。细胞色素P-450的电子供体、底物和调节剂大大降低了光谱变化的幅度。有人提出,高碘酸钠、亚氯酸钠和有机氢过氧化物通过形成细胞色素P-450的瞬时铁酰离子(化合物I)来促进甾体羟化,该离子可能是细胞色素P-450催化的羟化反应中涉及的常见中间羟化物种。