Department of Chemistry, University of California, Davis, CA 95616, USA.
Acta Crystallogr F Struct Biol Commun. 2020 Nov 1;76(Pt 11):557-567. doi: 10.1107/S2053230X20013680. Epub 2020 Oct 29.
Bacterial nonhydrolyzing UDP-N-acetylglucosamine 2-epimerases catalyze the reversible interconversion of UDP-N-acetylglucosamine (UDP-GlcNAc) and UDP-N-acetylmannosamine (UDP-ManNAc). UDP-ManNAc is an important intermediate in the biosynthesis of certain cell-surface polysaccharides, including those in some pathogenic bacteria, such as Neisseria meningitidis and Streptococcus pneumoniae. Many of these epimerases are allosterically regulated by UDP-GlcNAc, which binds adjacent to the active site and is required to initiate UDP-ManNAc epimerization. Here, two crystal structures of UDP-N-acetylglucosamine 2-epimerase from Neisseria meningitidis serogroup A (NmSacA) are presented. One crystal structure is of the substrate-free enzyme, while the other structure contains UDP-GlcNAc substrate bound to the active site. Both structures form dimers as seen in similar epimerases, and substrate binding to the active site induces a large conformational change in which two Rossmann-like domains clamp down on the substrate. Unlike other epimerases, NmSacA does not require UDP-GlcNAc to instigate the epimerization of UDP-ManNAc, although UDP-GlcNAc was found to enhance the rate of epimerization. In spite of the conservation of residues involved in binding the allosteric UDP-GlcNAc observed in similar UDP-GlcNAc 2-epimerases, the structures presented here do not contain UDP-GlcNAc bound in the allosteric site. These structural results provide additional insight into the mechanism and regulation of this critical enzyme and improve the structural understanding of the ability of NmSacA to epimerize modified substrates.
细菌非水解型 UDP-N-乙酰葡萄糖胺 2-差向异构酶催化 UDP-N-乙酰葡萄糖胺 (UDP-GlcNAc) 和 UDP-N-乙酰甘露糖胺 (UDP-ManNAc) 的可逆转化。UDP-ManNAc 是某些细胞表面多糖生物合成的重要中间体,包括某些致病菌中的多糖,如脑膜炎奈瑟菌和肺炎链球菌。许多这些差向异构酶受 UDP-GlcNAc 的别构调节,UDP-GlcNAc 结合在活性位点的相邻位置,是启动 UDP-ManNAc 差向异构化所必需的。本文介绍了来自脑膜炎奈瑟菌 A 群(NmSacA)的 UDP-N-乙酰葡萄糖胺 2-差向异构酶的两个晶体结构。一个晶体结构是无底物的酶,另一个结构包含结合在活性位点的 UDP-GlcNAc 底物。这两种结构都形成二聚体,类似于其他差向异构酶,底物结合到活性位点会引起很大的构象变化,其中两个类似 Rossmann 的结构域夹住底物。与其他差向异构酶不同,尽管发现 UDP-GlcNAc 可以提高差向异构化的速率,但 NmSacA 不需要 UDP-GlcNAc 来启动 UDP-ManNAc 的差向异构化。尽管在类似的 UDP-GlcNAc 2-差向异构酶中观察到参与结合别构 UDP-GlcNAc 的残基保守,但这里呈现的结构不包含结合在别构位点的 UDP-GlcNAc。这些结构结果为该关键酶的机制和调节提供了更多的见解,并提高了对 NmSacA 差向异构化修饰底物能力的结构理解。