National Medicines Institute, Warsaw, Poland.
Eur J Med Chem. 2012 Mar;49:200-10. doi: 10.1016/j.ejmech.2012.01.012. Epub 2012 Jan 15.
It is well known that 6-nitroquipazine exhibits about 150-fold higher affinity for the serotonin transporter (SERT) than quipazine and recently we showed quipazine buspirone analogues with high to moderate SERT affinity. Now we have designed and synthesized several 6-nitroquipazine buspirone derivatives. Unexpectedly, their SERT binding affinities were moderate, and much lower than that of the previously studied quipazine buspirone analogues. To explain these findings, docking studies of both groups of compounds into two different homology models of human SERT was performed using a flexible target-ligand docking approach (4D docking). The crystal structures of leucine transporter from Aquifex aeolicus in complex with leucine and with tryptophan were used as templates for the SERT models in closed and outward-facing conformations, respectively. We found that the latter conformation represents the most reliable model for binding of buspirone analogues. Docking into that model showed that the nitrated compounds acquire a rod like shape in the binding pocket with polar groups (nitro- and imido-) at the ends of the rod. 6-Nitro substituents gave steric clashes with amino acids located at the extracellular loop 4, which may explain their lower affinity than corresponding quipazine buspirone analogues. The results from the present study may suggest chemical design strategies to improve the SERT modulators.
众所周知,6-硝基喹哌嗪对 5-羟色胺转运体(SERT)的亲和力比喹哌嗪高约 150 倍,最近我们还展示了具有高到中等 SERT 亲和力的喹哌嗪丁螺环酮类似物。现在,我们设计并合成了几种 6-硝基喹哌嗪丁螺环酮衍生物。出乎意料的是,它们对 SERT 的结合亲和力适中,远低于之前研究的喹哌嗪丁螺环酮类似物。为了解释这些发现,我们使用灵活的靶标-配体对接方法(4D 对接)对这两组化合物分别对接进入两种不同的人 SERT 同源模型中进行了对接研究。来自水生栖热菌的亮氨酸转运蛋白与亮氨酸和色氨酸复合物的晶体结构分别被用作 SERT 模型在封闭和向外开放构象的模板。我们发现,后一种构象代表了丁螺环酮类似物结合的最可靠模型。对接入该模型表明,硝化化合物在结合口袋中获得棒状形状,棒的两端具有极性基团(硝基和亚氨基)。6-硝基取代基与位于细胞外环 4 上的氨基酸发生空间位阻冲突,这可能解释了它们与相应的喹哌嗪丁螺环酮类似物相比亲和力较低的原因。本研究的结果可能为改善 SERT 调节剂提供了化学设计策略。