Tavares Norbert K, Zayas Carmen L, Escalante-Semerena Jorge C
Department of Microbiology , University of Georgia , Athens , Georgia 30602 , United States.
Department of Bacteriology , University of Wisconsin , Madison , Wisconsin 53706 , United States.
Biochemistry. 2018 Jul 31;57(30):4478-4495. doi: 10.1021/acs.biochem.8b00546. Epub 2018 Jul 13.
Cobamides (Cbas) are synthesized by many archaea, but some aspects of Cba biosynthesis in these microorganisms remain unclear. Here, we demonstrate that open reading frame MM2060 in the archaeum Methanosarcina mazei strain Gö1 encodes a bifunctional enzyme with l-threonine- O-3-phosphate (l-Thr-P) decarboxylase (EC 4.1.1.81) and l-Thr kinase activities (EC 2.7.1.177). In Salmonella enterica, where Cba biosynthesis has been extensively studied, the activities mentioned above are encoded by separate genes, namely, cobD and pduX, respectively. The activities associated with the MM2060 protein ( MmCobD) were validated in vitro and in vivo. In vitro, MmCobD used ATP and l-Thr as substrates and generated ADP, l-Thr-P, and ( R)-1-aminopropan-2-ol O-phosphate as products. Notably, MmCobD has a 111-amino acid C-terminal extension of unknown function, which contains a putative metal-binding motif. This C-terminal domain alone did not display activity either in vivo or in vitro. Although the C-terminal MmCobD domain was not required for l-Thr-P decarboxylase or l-Thr kinase activities in vivo, its absence negatively affected both activities. In vitro results suggested that this domain may have a regulatory or substrate-gating role. When purified under anoxic conditions, MmCobD displayed Michaelis-Menten kinetics and had a 1000-fold higher affinity for ATP and a catalytic efficiency 1300-fold higher than that of MmCobD purified under oxic conditions. To the best of our knowledge, MmCobD is the first example of a new class of l-Thr-P decarboxylases that also have l-Thr kinase activity. An archaeal protein with l-Thr kinase activity had not been identified prior to this work.
钴胺素(Cbas)由许多古生菌合成,但这些微生物中Cba生物合成的某些方面仍不清楚。在这里,我们证明古生菌马氏甲烷八叠球菌菌株Gö1中的开放阅读框MM2060编码一种具有L-苏氨酸-O-3-磷酸(L-Thr-P)脱羧酶(EC 4.1.1.81)和L-Thr激酶活性(EC 2.7.1.177)的双功能酶。在已对Cba生物合成进行广泛研究的肠炎沙门氏菌中,上述活性分别由单独的基因cobD和pduX编码。与MM2060蛋白(MmCobD)相关的活性在体外和体内均得到验证。在体外,MmCobD以ATP和L-Thr为底物,生成ADP、L-Thr-P和(R)-1-氨基丙-2-醇O-磷酸作为产物。值得注意的是,MmCobD具有一个功能未知的111个氨基酸的C末端延伸,其中包含一个假定的金属结合基序。单独的这个C末端结构域在体内或体外均未显示活性。尽管C末端MmCobD结构域在体内对于L-Thr-P脱羧酶或L-Thr激酶活性不是必需的,但其缺失对这两种活性均有负面影响。体外结果表明该结构域可能具有调节或底物门控作用。在缺氧条件下纯化时,MmCobD表现出米氏动力学,对ATP的亲和力比在有氧条件下纯化的MmCobD高1000倍,催化效率高1300倍。据我们所知,MmCobD是一类新的同时具有L-Thr激酶活性的L-Thr-P脱羧酶的首个实例。在这项工作之前尚未鉴定出具有L-Thr激酶活性的古生菌蛋白。