Varney Kristen M, Bonvin Alexandre M J J, Pazgier Marzena, Malin Jakob, Yu Wenbo, Ateh Eugene, Oashi Taiji, Lu Wuyuan, Huang Jing, Diepeveen-de Buin Marlies, Bryant Joseph, Breukink Eefjan, Mackerell Alexander D, de Leeuw Erik P H
NMR Facility, University of Maryland Baltimore School of Medicine, Baltimore, Maryland, United States of America.
PLoS Pathog. 2013;9(11):e1003732. doi: 10.1371/journal.ppat.1003732. Epub 2013 Nov 7.
We have previously reported on the functional interaction of Lipid II with human alpha-defensins, a class of antimicrobial peptides. Lipid II is an essential precursor for bacterial cell wall biosynthesis and an ideal and validated target for natural antibiotic compounds. Using a combination of structural, functional and in silico analyses, we present here the molecular basis for defensin-Lipid II binding. Based on the complex of Lipid II with Human Neutrophil peptide-1, we could identify and characterize chemically diverse low-molecular weight compounds that mimic the interactions between HNP-1 and Lipid II. Lead compound BAS00127538 was further characterized structurally and functionally; it specifically interacts with the N-acetyl muramic acid moiety and isoprenyl tail of Lipid II, targets cell wall synthesis and was protective in an in vivo model for sepsis. For the first time, we have identified and characterized low molecular weight synthetic compounds that target Lipid II with high specificity and affinity. Optimization of these compounds may allow for their development as novel, next generation therapeutic agents for the treatment of Gram-positive pathogenic infections.
我们之前曾报道过脂质II与人类α-防御素(一类抗菌肽)之间的功能相互作用。脂质II是细菌细胞壁生物合成的必需前体,也是天然抗生素化合物的理想且经过验证的靶点。通过结合结构、功能和计算机模拟分析,我们在此展示了防御素与脂质II结合的分子基础。基于脂质II与人中性粒细胞肽-1的复合物,我们能够鉴定和表征模拟HNP-1与脂质II之间相互作用的化学性质多样的低分子量化合物。先导化合物BAS00127538在结构和功能上得到了进一步表征;它特异性地与脂质II的N-乙酰胞壁酸部分和异戊二烯基尾部相互作用,靶向细胞壁合成,并在脓毒症的体内模型中具有保护作用。我们首次鉴定和表征了以高特异性和亲和力靶向脂质II的低分子量合成化合物。对这些化合物进行优化可能使其开发成为用于治疗革兰氏阳性病原菌感染的新型下一代治疗药物。