Harayama S, Rekik M, Ngai K L, Ornston L N
Department of Medical Biochemistry, University of Geneva, Switzerland.
J Bacteriol. 1989 Nov;171(11):6251-8. doi: 10.1128/jb.171.11.6251-6258.1989.
The meta-cleavage pathway of catechol is a major mechanism for degradation of aromatic compounds. In this pathway, the aromatic ring of catechol is cleaved by catechol 2,3-dioxygenase and its product, 2-hydroxymuconic semialdehyde, is further metabolized by either a hydrolytic or dehydrogenative route. In the dehydrogenative route, 2-hydroxymuconic semialdehyde is oxidized to the enol form of 4-oxalocrotonate by a dehydrogenase and then further metabolized to acetaldehyde and pyruvate by the actions of 4-oxalocrotonate isomerase, 4-oxalocrotonate decarboxylase, 2-oxopent-4-enoate hydratase, and 4-hydroxy-2-oxovalerate aldolase. In this study, the isomerase, decarboxylase, and hydratase encoded in the TOL plasmid pWW0 of Pseudomonas putida mt-2 were purified and characterized. The 28-kilodalton isomerase was formed by association of extremely small identical protein subunits with an apparent molecular weight of 3,500. The decarboxylase and the hydratase were 27- and 28-kilodalton polypeptides, respectively, and were copurified by high-performance-liquid chromatography with anion-exchange, hydrophobic interaction, and gel filtration columns. The structural genes for the decarboxylase (xylI) and the hydratase (xylJ) were cloned into Escherichia coli. The elution profile in anion-exchange chromatography of the decarboxylase and the hydratase isolated from E. coli XylI+XylJ- and XylI-XylJ+ clones, respectively, were different from those isolated from XylI+ XylJ+ bacteria. This suggests that the carboxylase and the hydratase form a complex in vivo. The keto but not the enol form of 4-oxalocrotonate was a substrate for the decarboxylase. The product of decarboxylation was 2-hydroxypent-2,4-dienoate rather than its keto form, 2-oxopent-4-enoate. The hydratase acts on the former but not the latter isomer. Because 2-hydroxypent-2,4-dienoate is chemically unstable, formation of a complex between the decarboxylase and the hydratase may assure efficient transformation of this unstable intermediate in vivo.
儿茶酚的间位裂解途径是芳香族化合物降解的主要机制。在该途径中,儿茶酚的芳香环被儿茶酚2,3-双加氧酶裂解,其产物2-羟基粘康酸半醛通过水解或脱氢途径进一步代谢。在脱氢途径中,2-羟基粘康酸半醛被脱氢酶氧化为4-草酰巴豆酸的烯醇形式,然后通过4-草酰巴豆酸异构酶、4-草酰巴豆酸脱羧酶、2-氧代戊-4-烯酸水合酶和4-羟基-2-氧代戊酸醛缩酶的作用进一步代谢为乙醛和丙酮酸。在本研究中,对恶臭假单胞菌mt-2的TOL质粒pWW0中编码的异构酶、脱羧酶和水合酶进行了纯化和表征。28千道尔顿的异构酶由表观分子量为3500的极小的相同蛋白质亚基缔合形成。脱羧酶和水合酶分别是27千道尔顿和28千道尔顿的多肽,通过阴离子交换、疏水相互作用和凝胶过滤柱的高效液相色谱法共纯化。将脱羧酶(xylI)和水合酶(xylJ)的结构基因克隆到大肠杆菌中。分别从大肠杆菌XylI+XylJ-和XylI-XylJ+克隆中分离得到的脱羧酶和水合酶在阴离子交换色谱中的洗脱图谱与从XylI+XylJ+细菌中分离得到的不同。这表明羧化酶和水合酶在体内形成复合物。4-草酰巴豆酸的酮式而非烯醇式是脱羧酶的底物。脱羧产物是2-羟基戊-2,4-二烯酸而非其酮式2-氧代戊-4-烯酸。水合酶作用于前者而非后者异构体。由于2-羟基戊-2,4-二烯酸化学性质不稳定,脱羧酶和水合酶之间形成复合物可能确保该不稳定中间体在体内的有效转化。