Department of Molecular Microbiology and Biotechnology, Tel-Aviv University, Tel-Aviv, Israel.
PLoS One. 2010 Jun 14;5(6):e11101. doi: 10.1371/journal.pone.0011101.
The rational design of amyloid oligomer inhibitors is yet an unmet drug development need. Previous studies have identified the role of tryptophan in amyloid recognition, association and inhibition. Furthermore, tryptophan was ranked as the residue with highest amyloidogenic propensity. Other studies have demonstrated that quinones, specifically anthraquinones, can serve as aggregation inhibitors probably due to the dipole interaction of the quinonic ring with aromatic recognition sites within the amyloidogenic proteins. Here, using in vitro, in vivo and in silico tools we describe the synthesis and functional characterization of a rationally designed inhibitor of the Alzheimer's disease-associated beta-amyloid. This compound, 1,4-naphthoquinon-2-yl-L-tryptophan (NQTrp), combines the recognition capacities of both quinone and tryptophan moieties and completely inhibited Abeta oligomerization and fibrillization, as well as the cytotoxic effect of Abeta oligomers towards cultured neuronal cell line. Furthermore, when fed to transgenic Alzheimer's disease Drosophila model it prolonged their life span and completely abolished their defective locomotion. Analysis of the brains of these flies showed a significant reduction in oligomeric species of Abeta while immuno-staining of the 3(rd) instar larval brains showed a significant reduction in Abeta accumulation. Computational studies, as well as NMR and CD spectroscopy provide mechanistic insight into the activity of the compound which is most likely mediated by clamping of the aromatic recognition interface in the central segment of Abeta. Our results demonstrate that interfering with the aromatic core of amyloidogenic peptides is a promising approach for inhibiting various pathogenic species associated with amyloidogenic diseases. The compound NQTrp can serve as a lead for developing a new class of disease modifying drugs for Alzheimer's disease.
淀粉样寡聚物抑制剂的合理设计是一个未满足的药物开发需求。先前的研究已经确定了色氨酸在淀粉样识别、聚集和抑制中的作用。此外,色氨酸被列为具有最高淀粉样倾向的残基。其他研究表明,醌类,特别是蒽醌类,可以作为聚集抑制剂,可能是由于醌环与淀粉样蛋白中的芳香识别位点的偶极相互作用。在这里,我们使用体外、体内和计算工具描述了一种阿尔茨海默病相关β-淀粉样蛋白的合理设计抑制剂的合成和功能表征。这种化合物,1,4-萘醌-2-基-L-色氨酸(NQTrp),结合了醌和色氨酸部分的识别能力,完全抑制了 Abeta 寡聚化和纤维化,以及 Abeta 寡聚物对培养神经元细胞系的细胞毒性作用。此外,当喂食给转基因阿尔茨海默病果蝇模型时,它延长了它们的寿命,并完全消除了它们的运动缺陷。这些果蝇大脑的分析显示 Abeta 的寡聚物种显著减少,而 3 龄幼虫大脑的免疫染色显示 Abeta 积累显著减少。计算研究以及 NMR 和 CD 光谱学为该化合物的活性提供了机制上的见解,该化合物的活性很可能是通过在 Abeta 的中心片段夹断芳香识别界面来介导的。我们的研究结果表明,干扰淀粉样肽的芳香核心是抑制与淀粉样变性疾病相关的各种致病物种的一种有前途的方法。化合物 NQTrp 可以作为开发用于治疗阿尔茨海默病的新型疾病修饰药物的先导化合物。