Department of Medicinal Chemistry, BMC, Uppsala University, Box 574, SE-75123, Uppsala, Sweden.
Department of Cell and Molecular Biology, BMC, Uppsala University, Box 596, SE-75123, Uppsala, Sweden.
Eur J Med Chem. 2024 Nov 15;278:116790. doi: 10.1016/j.ejmech.2024.116790. Epub 2024 Aug 22.
New antibacterial compounds are urgently needed, especially for infections caused by the top-priority Gram-negative bacteria that are increasingly difficult to treat. Lipid A is a key component of the Gram-negative outer membrane and the LpxH enzyme plays an important role in its biosynthesis, making it a promising antibacterial target. Inspired by previously reported ortho-N-methyl-sulfonamidobenzamide-based LpxH inhibitors, novel benzamide substitutions were explored in this work to assess their in vitro activity. Our findings reveal that maintaining wild-type antibacterial activity necessitates removal of the N-methyl group when shifting the ortho-N-methyl-sulfonamide to the meta-position. This discovery led to the synthesis of meta-sulfonamidobenzamide analogs with potent antibacterial activity and enzyme inhibition. Moreover, we demonstrate that modifying the benzamide scaffold can alter blocking of the cardiac voltage-gated potassium ion channel hERG. Furthermore, two LpxH-bound X-ray structures show how the enzyme-ligand interactions of the meta-sulfonamidobenzamide analogs differ from those of the previously reported ortho analogs. Overall, our study has identified meta-sulfonamidobenzamide derivatives as promising LpxH inhibitors with the potential for optimization in future antibacterial hit-to-lead programs.
新的抗菌化合物迫切需要,特别是对于越来越难以治疗的顶级革兰氏阴性细菌感染。脂 A 是革兰氏阴性外膜的关键组成部分,而 LpxH 酶在其生物合成中起着重要作用,使其成为有前途的抗菌靶标。受先前报道的邻-N-甲基-磺酰胺苯甲酰胺基 LpxH 抑制剂的启发,本研究探索了新型苯甲酰胺取代基,以评估它们的体外活性。我们的研究结果表明,当将邻-N-甲基磺酰胺基转移到间位时,需要去除 N-甲基基团以保持野生型抗菌活性。这一发现导致了具有强大抗菌活性和酶抑制作用的间磺酰胺苯甲酰胺类似物的合成。此外,我们证明了修饰苯甲酰胺支架可以改变阻断心脏电压门控钾离子通道 hERG。此外,两个 LpxH 结合的 X 射线结构显示了间磺酰胺苯甲酰胺类似物的酶-配体相互作用如何与先前报道的邻位类似物不同。总的来说,我们的研究表明间磺酰胺苯甲酰胺衍生物是有前途的 LpxH 抑制剂,有可能在未来的抗菌命中致胜计划中进行优化。