Baum Bernhard, Lecker Laura S M, Zoltner Martin, Jaenicke Elmar, Schnell Robert, Hunter William N, Brenk Ruth
Institut für Pharmazie und Biochemie, Johannes Gutenberg-Universität, Staudinger Weg 5, 55128 Mainz, Germany.
Division of Biological Chemistry and Drug Discovery, College of Life Sciences, University of Dundee, Dundee DD1 4EH, Scotland.
Acta Crystallogr F Struct Biol Commun. 2015 Aug;71(Pt 8):1020-6. doi: 10.1107/S2053230X15010614. Epub 2015 Jul 28.
Bacterial infections remain a serious health concern, in particular causing life-threatening infections of hospitalized and immunocompromised patients. The situation is exacerbated by the rise in antibacterial drug resistance, and new treatments are urgently sought. In this endeavour, accurate structures of molecular targets can support early-stage drug discovery. Here, crystal structures, in three distinct forms, of recombinant Pseudomonas aeruginosa β-ketoacyl-(acyl-carrier-protein) synthase II (FabF) are presented. This enzyme, which is involved in fatty-acid biosynthesis, has been validated by genetic and chemical means as an antibiotic target in Gram-positive bacteria and represents a potential target in Gram-negative bacteria. The structures of apo FabF, of a C164Q mutant in which the binding site is altered to resemble the substrate-bound state and of a complex with 3-(benzoylamino)-2-hydroxybenzoic acid are reported. This compound mimics aspects of a known natural product inhibitor, platensimycin, and surprisingly was observed binding outside the active site, interacting with a symmetry-related molecule. An unusual feature is a completely buried potassium-binding site that was identified in all three structures. Comparisons suggest that this may represent a conserved structural feature of FabF relevant to fold stability. The new structures provide templates for structure-based ligand design and, together with the protocols and reagents, may underpin a target-based drug-discovery project for urgently needed antibacterials.
细菌感染仍然是一个严重的健康问题,尤其会导致住院患者和免疫功能低下患者出现危及生命的感染。抗菌药物耐药性的上升加剧了这种情况,因此迫切需要新的治疗方法。在这一努力过程中,分子靶点的精确结构能够支持早期药物研发。本文展示了重组铜绿假单胞菌β-酮酰基-(酰基载体蛋白)合酶II(FabF)的三种不同形式的晶体结构。这种参与脂肪酸生物合成的酶已通过基因和化学方法验证为革兰氏阳性菌中的抗生素靶点,并且在革兰氏阴性菌中也代表一个潜在靶点。报道了无配体FabF、结合位点改变为类似底物结合状态的C164Q突变体以及与3-(苯甲酰氨基)-2-羟基苯甲酸复合物的结构。该化合物模拟了已知天然产物抑制剂扁平霉素的某些方面,令人惊讶的是,它被观察到结合在活性位点之外,与一个对称相关分子相互作用。一个不寻常的特征是在所有三种结构中都鉴定出了一个完全埋藏的钾结合位点。比较结果表明,这可能代表了与折叠稳定性相关的FabF保守结构特征。这些新结构为基于结构的配体设计提供了模板,并且连同实验方案和试剂一起,可能为急需的抗菌药物基于靶点的药物研发项目奠定基础。