Cooper Christopher L, Stob Christian M, Jones Marjorie A, Lash Timothy D
Department of Chemistry, Illinois State University, Normal, IL 61790-4160, USA.
Bioorg Med Chem. 2005 Nov 15;13(22):6244-51. doi: 10.1016/j.bmc.2005.06.051. Epub 2005 Aug 3.
An abnormal series of porphyrin tetracarboxylic acids known as the isocoproporphyrins, are commonly excreted by patients suffering from the disease porphyria cutanea tarda (PCT). These porphyrins appear to arise by bacterial degradation of dehydroisocoproporphyrinogen that is generated by the premature metabolism of the normal pentacarboxylate intermediate (5dab) by coproporphyrinogen oxidase (copro'gen oxidase). This porphyrinogen can be further metabolized by uroporphyrinogen decarboxylase to give harderoporphyrinogen, one of the usual intermediates in heme biosynthesis. Therefore, it is possible that some of the heme formed under abnormal conditions may originate from the 'isocopro-type' porphyrinogen intermediate. In order to investigate the feasibility of alternative pathways for heme biosynthesis, the four type III pentacarboxylate isomeric porphyrinogens were incubated with purified, cloned human copro'gen oxidase at 37 degrees C with various substrate concentrations under initial velocity conditions. Of the four isomers, only 5dab was a substrate for copro'gen oxidase and this gave dehydroisocoproporphyrin. The structure of the related porphyrin tetramethyl ester was confirmed by proton NMR spectroscopy and mass spectrometry. The K(m) value for proto'gen-IX formation from copro'gen, an indicator of molecular recognition, was similar to the K(m) value for monovinyl product formation with 5dab, although copro'gen-III has an approximately twofold higher K(cat) value. Although 5dab is a slightly poorer substrate than copro'gen-III, these results support the hypothesis that an abnormal route for heme biosynthesis is possible in humans suffering from PCT or related syndromes such as hexachlorobenzene poisoning.
一种异常的卟啉四羧酸系列,即异粪卟啉,通常由患有迟发性皮肤卟啉症(PCT)的患者排出。这些卟啉似乎是由脱氢异粪卟啉原的细菌降解产生的,而脱氢异粪卟啉原是由粪卟啉原氧化酶(粪卟啉原氧化酶)对正常五羧酸盐中间体(5dab)的过早代谢产生的。这种卟啉原可以被尿卟啉原脱羧酶进一步代谢生成硬卟啉原,这是血红素生物合成中常见的中间体之一。因此,在异常条件下形成的一些血红素可能源自“异粪卟啉型”卟啉原中间体。为了研究血红素生物合成替代途径的可行性,将四种III型五羧酸盐异构体卟啉原与纯化的、克隆的人粪卟啉原氧化酶在37℃下,在初始速度条件下以各种底物浓度进行孵育。在这四种异构体中,只有5dab是粪卟啉原氧化酶的底物,它生成脱氢异粪卟啉。相关卟啉四甲酯的结构通过质子核磁共振光谱和质谱得到证实。从粪卟啉原形成原卟啉IX的K(m)值,作为分子识别的指标,与5dab形成单乙烯基产物的K(m)值相似,尽管粪卟啉原III的K(cat)值大约高两倍。虽然5dab作为底物比粪卟啉原III略差,但这些结果支持了这样一种假设,即在患有PCT或相关综合征(如六氯苯中毒)的人类中,血红素生物合成存在异常途径。