State Key Laboratory of Molecular Biology, National Center for Protein Science Shanghai, Shanghai Science Research Center, CAS Center for Excellence in Molecular Cell Science, Shanghai Institute of Biochemistry and Cell Biology, Chinese Academy of Sciences, 333 Haike Road, Shanghai, 201210, China.
University of Chinese Academy of Sciences, Shanghai, 201210, China.
Nat Commun. 2017 Nov 22;8(1):1691. doi: 10.1038/s41467-017-01821-9.
The membrane-integral glycerol 3-phosphate (G3P) acyltransferase PlsY catalyses the committed and essential step in bacterial phospholipid biosynthesis by acylation of G3P, forming lysophosphatidic acid. It contains no known acyltransferase motifs, lacks eukaryotic homologs, and uses the unusual acyl-phosphate as acyl donor, as opposed to acyl-CoA or acyl-carrier protein for other acyltransferases. Previous studies have identified several PlsY inhibitors as potential antimicrobials. Here we determine the crystal structure of PlsY at 1.48 Å resolution, revealing a seven-transmembrane helix fold. Four additional substrate- and product-bound structures uncover the atomic details of its relatively inflexible active site. Structure and mutagenesis suggest a different acylation mechanism of 'substrate-assisted catalysis' that, unlike other acyltransferases, does not require a proteinaceous catalytic base to complete. The structure data and a high-throughput enzymatic assay developed in this work should prove useful for virtual and experimental screening of inhibitors against this vital bacterial enzyme.
膜整合甘油 3-磷酸(G3P)酰基转移酶 PlsY 通过酰化 G3P 催化细菌磷脂生物合成的关键和必需步骤,形成溶血磷脂酸。它不含已知的酰基转移酶基序,缺乏真核同源物,并且使用不寻常的酰基-磷酸作为酰基供体,而不是其他酰基转移酶的酰基辅酶 A 或酰基载体蛋白。先前的研究已经确定了几种 PlsY 抑制剂作为潜在的抗菌剂。在这里,我们以 1.48 Å 的分辨率确定了 PlsY 的晶体结构,揭示了一个七跨膜螺旋折叠。另外四个结合了底物和产物的结构揭示了其相对不灵活的活性位点的原子细节。结构和突变分析表明了一种不同的酰化机制,即“底物辅助催化”,与其他酰基转移酶不同,它不需要蛋白质催化碱来完成。这项工作中开发的结构数据和高通量酶测定法应该对针对这种重要细菌酶的抑制剂的虚拟和实验筛选有用。