Romkina Anastasia Y, Kiriukhin Michael Y
Ajinomoto-Genetika Research Institute, Moscow, Russia.
PLoS One. 2017 Apr 19;12(4):e0176056. doi: 10.1371/journal.pone.0176056. eCollection 2017.
The isocitrate dehydrogenase (MfIDH) with unique double coenzyme specificity from Methylobacillus flagellatus was purified and characterized, and its gene was cloned and overexpressed in E. coli as a fused protein. This enzyme is homodimeric,-with a subunit molecular mass of 45 kDa and a specific activity of 182 U mg -1 with NAD+ and 63 U mg -1 with NADP+. The MfIDH activity was dependent on divalent cations and Mn2+ enhanced the activity the most effectively. MfIDH exhibited a cofactor-dependent pH-activity profile. The optimum pH values were 8.5 (NAD+) and 6.0 (NADP+).The Km values for NAD+ and NADP+ were 113 μM and 184 μM respectively, while the Km values for DL-isocitrate were 9.0 μM (NAD+), 8.0 μM (NADP+). The MfIDH specificity (kcat/Km) was only 5-times higher for NAD+ than for NADP+. The purified MfIDH displayed maximal activity at 60°C. Heat-inactivation studies showed that the MfIDH was remarkably thermostable, retaining full activity at 50°C and losting ca. 50% of its activity after one hour of incubation at 75°C. The enzyme was insensitive to the presence of intermediate metabolites, with the exception of 2 mM ATP, which caused 50% inhibition of NADP+-linked activity. The indispensability of the N6 amino group of NAD(P)+ in its binding to MfIDH was demonstrated. MfIDH showed high sequence similarity with bacterial NAD(P)+-dependent type I isocitrate dehydrogenases (IDHs) rather than with eukaryotic NAD+-dependent IDHs. The unique double coenzyme specificity of MfIDH potentially resulted from the Lys340, Ile341 and Ala347 residues in the coenzyme-binding site of the enzyme. The discovery of a type I IDH with double coenzyme specificity elucidates the evolution of this subfamily IDHs and may provide fundamental information for engineering enzymes with desired properties.
对来自鞭毛甲基杆菌的具有独特双辅酶特异性的异柠檬酸脱氢酶(MfIDH)进行了纯化和表征,并克隆了其基因,在大肠杆菌中作为融合蛋白进行了过量表达。该酶为同型二聚体,亚基分子量为45 kDa,对NAD⁺的比活性为182 U mg⁻¹,对NADP⁺的比活性为63 U mg⁻¹。MfIDH活性依赖于二价阳离子,其中Mn²⁺对活性的增强最为有效。MfIDH呈现出依赖于辅因子的pH-活性曲线。最佳pH值分别为8.5(NAD⁺)和6.0(NADP⁺)。NAD⁺和NADP⁺的Km值分别为113 μM和184 μM,而DL-异柠檬酸的Km值分别为9.0 μM(NAD⁺)、8.0 μM(NADP⁺)。MfIDH对NAD⁺的特异性(kcat/Km)仅比对NADP⁺高5倍。纯化后的MfIDH在60°C时表现出最大活性。热失活研究表明,MfIDH具有显著的热稳定性,在50°C时保留全部活性,在75°C孵育1小时后约丧失50%的活性。该酶对中间代谢产物不敏感,但2 mM ATP除外,它会导致NADP⁺相关活性受到50%的抑制。证明了NAD(P)⁺的N6氨基在其与MfIDH结合中的不可或缺性。MfIDH与细菌NAD(P)⁺依赖性I型异柠檬酸脱氢酶(IDHs)具有高度序列相似性,而与真核生物NAD⁺依赖性IDHs的相似性较低。MfIDH独特的双辅酶特异性可能源于该酶辅酶结合位点中的Lys340、Ile341和Ala347残基。具有双辅酶特异性的I型IDH的发现阐明了该亚家族IDHs的进化,并可能为工程改造具有所需特性的酶提供基础信息。