Vithani Neha, Bais Vaibhav, Prakash Balaji
Department of Biological Sciences and Bioengineering, Indian Institute of Technology, Kanpur 208 016, India.
Acta Crystallogr F Struct Biol Commun. 2014 Jun;70(Pt 6):703-8. doi: 10.1107/S2053230X14008279. Epub 2014 May 10.
N-Acetylglucosamine-1-phosphate uridyltransferase (GlmU), a bifunctional enzyme exclusive to prokaryotes, belongs to the family of sugar nucleotidyltransferases (SNTs). The enzyme binds GlcNAc-1-P and UTP, and catalyzes a uridyltransfer reaction to synthesize UDP-GlcNAc, an important precursor for cell-wall biosynthesis. As many SNTs are known to utilize a broad range of substrates, substrate specificity in GlmU was probed using biochemical and structural studies. The enzymatic assays reported here demonstrate that GlmU is specific for its natural substrates UTP and GlcNAc-1-P. The crystal structure of GlmU bound to ATP and GlcNAc-1-P provides molecular details for the inability of the enzyme to utilize ATP for the nucleotidyltransfer reaction. ATP binding results in an inactive pre-catalytic enzyme-substrate complex, where it adopts an unusual conformation such that the reaction cannot be catalyzed; here, ATP is shown to be bound together with three Mg2+ ions. Overall, this structure represents the binding of an inhibitory molecule at the active site and can potentially be used to develop new inhibitors of the enzyme. Further, similar to DNA/RNA polymerases, GlmU was recently recognized to utilize two metal ions, MgA2+ and MgB2+, to catalyze the uridyltransfer reaction. Interestingly, displacement of MgB2+ from its usual catalytically competent position, as noted in the crystal structure of RNA polymerase in an inactive state, was considered to be a key factor inhibiting the reaction. Surprisingly, in the current structure of GlmU MgB2+ is similarly displaced; this raises the possibility that an analogous inhibitory mechanism may be operative in GlmU.
N-乙酰葡糖胺-1-磷酸尿苷转移酶(GlmU)是一种原核生物特有的双功能酶,属于糖核苷酸转移酶(SNTs)家族。该酶结合GlcNAc-1-P和UTP,并催化尿苷转移反应以合成UDP-GlcNAc,这是细胞壁生物合成的重要前体。由于已知许多SNTs可利用多种底物,因此通过生化和结构研究探究了GlmU中的底物特异性。本文报道的酶活性测定表明,GlmU对其天然底物UTP和GlcNAc-1-P具有特异性。与ATP和GlcNAc-1-P结合的GlmU晶体结构为该酶无法利用ATP进行核苷酸转移反应提供了分子细节。ATP结合导致形成无活性的催化前酶-底物复合物,其中它采用异常构象,使得反应无法被催化;在此,ATP显示与三个Mg2+离子结合在一起。总体而言,该结构代表了抑制性分子在活性位点的结合,并有可能用于开发该酶的新型抑制剂。此外,与DNA/RNA聚合酶类似,GlmU最近被认为利用两种金属离子MgA2+和MgB2+来催化尿苷转移反应。有趣的是,如在处于无活性状态的RNA聚合酶晶体结构中所观察到的,MgB2+从其通常的催化活性位置被取代被认为是抑制反应的关键因素。令人惊讶的是,在当前GlmU的结构中,MgB2+同样被取代;这增加了类似的抑制机制可能在GlmU中起作用的可能性。