Department of Immunology and Infectious Diseases, Montana State University, Bozeman, MT 59717, USA.
Biochem Pharmacol. 2013 Feb 1;85(3):404-16. doi: 10.1016/j.bcp.2012.11.015. Epub 2012 Dec 3.
N-formyl peptide receptors (FPRs) are G protein-coupled receptors (GPCRs) that play critical roles in inflammatory reactions, and FPR-specific interactions can possibly be used to facilitate the resolution of pathological inflammatory reactions. Recent studies indicated that FPRs have stereo-selective preference for chiral ligands. Here, we investigated the structure-activity relationship of 24 chiral ureidopropanamides, including previously reported compounds PD168368/PD176252 and their close analogs, and used molecular modeling to define chiral recognition by FPR2. Unlike previously reported 6-methyl-2,4-disubstituted pyridazin-3(2H)-ones, whose R-forms preferentially activated FPR1/FPR2, we found that four S-enantiomers in the seven ureidopropanamide pairs tested preferentially activated intracellular Ca(2+) flux in FPR2-transfected cells, while the R-counterpart was more active in two enantiomer pairs. Thus, active enantiomers of FPR2 agonists can be in either R- or S-configurations, depending on the molecular scaffold and specific substituents at the chiral center. Using molecular modeling approaches, including field point methodology, homology modeling, and docking studies, we propose a model that can explain stereoselective activity of chiral FPR2 agonists. Importantly, our docking studies of FPR2 chiral agonists correlated well with the FPR2 pharmacophore model derived previously. We conclude that the ability of FPR2 to discriminate between the enantiomers is the consequence of the arrangement of the three asymmetric hydrophobic subpockets at the main orthosteric FPR2 binding site with specific orientation of charged regions in the subpockets.
N-甲酰肽受体(FPRs)是 G 蛋白偶联受体(GPCRs),在炎症反应中发挥关键作用,并且 FPR 特异性相互作用可能用于促进病理性炎症反应的消退。最近的研究表明,FPR 对手性配体具有立体选择性偏好。在这里,我们研究了 24 种手性脲丙酰胺的结构-活性关系,包括以前报道的化合物 PD168368/PD176252 及其近缘类似物,并使用分子建模来定义 FPR2 的手性识别。与以前报道的 6-甲基-2,4-二取代哒嗪-3(2H)-酮不同,其 R 形式优先激活 FPR1/FPR2,我们发现测试的 7 对脲丙酰胺对中的四个 S-对映体优先激活 FPR2 转染细胞中的细胞内 Ca(2+)流,而 R-对映体在两个对映体对中更活跃。因此,FPR2 激动剂的活性对映体可以是 R-或 S-构型,这取决于分子支架和手性中心的特定取代基。使用分子建模方法,包括场点方法、同源建模和对接研究,我们提出了一个可以解释手性 FPR2 激动剂立体选择性活性的模型。重要的是,我们对 FPR2 手性激动剂的对接研究与以前推导的 FPR2 药效基团模型很好地相关。我们得出结论,FPR2 区分对映体的能力是由于三个不对称疏水性亚口袋在主要的 FPR2 结合位点的排列以及亚口袋中带电荷区域的特定取向所致。