Laboratory of Pharmacology and Neuroscience, Department of Oncology, Biology and Genetics, University of Genova, Viale Benedetto XV, 2, 16132 Genoa, Italy.
Neurotox Res. 2011 May;19(4):556-74. doi: 10.1007/s12640-010-9189-8. Epub 2010 Apr 20.
Quinacrine is one of the few molecules tested to treat patients affected by prion diseases, although the clinical outcome is largely unsatisfactory. To identify novel derivatives with higher neuroprotective activity, we evaluated the effects of a small library of acridine derivatives. The 6-chloro-2-methoxyacridine derivatives bearing on position 9 a quinolizidin-1-ylamino (Q1, Q2) or a quinolizidin-1-ylalkylamino residue (Q3, Q4, Q6, Q7), the thio-bioisoster of Q3 (Q5), the 9-(N-lupinylthiopropyl)amino derivative (Q8) and simple acridines (Q9 and Q10) were considered. We compared the effects of quinacrine and these novel analogues in the inhibition of the cytotoxic activity and protease K (PK) resistance of the human prion protein fragment 90-231 (hPrP90-231). We demonstrate that quinacrine caused a significant reduction of hPrP90-231 toxicity due to its binding to the fragment and the prevention of its conversion in a toxic isoform. All acridine derivatives analyzed showed high affinity binding for hPrP90-231, but only Q3 and Q10, caused a significant reduction of hPrP90-231 cytotoxicity, with higher efficacy than quinacrine. We attempted to correlate the cytoprotective effects of the new compounds with some biochemical parameters (binding affinity to hPrP90-231, intrinsic fluorescence quenching, hydrophobic amino acid exposure), but a direct relationship occurred only with the reduction of PK resistance, likely due to the prevention of the acquisition of the β-sheet-rich toxic conformation. These data represent interesting leads for further modifications of the basic side chain and the substituent pattern of the acridine nucleus to develop novel compounds with improved antiprion activity to be tested in in vivo experimental setting.
吖啶是少数几种经测试可用于治疗朊病毒病患者的分子之一,尽管临床疗效大多不尽人意。为了寻找具有更高神经保护活性的新型衍生物,我们评估了一小部分吖啶衍生物文库的作用。我们研究了 9-位带有喹啉基氨基(Q1、Q2)或喹啉基烷基氨基(Q3、Q4、Q6、Q7)取代基的 6-氯-2-甲氧基吖啶衍生物、Q3 的硫代生物等排体(Q5)、9-(N-羽扇豆基硫代丙基)氨基衍生物(Q8)和简单吖啶(Q9 和 Q10)。我们比较了吖啶和这些新型类似物对人朊病毒蛋白片段 90-231(hPrP90-231)细胞毒性和蛋白酶 K(PK)抗性的抑制作用。我们证明吖啶通过与片段结合并防止其转化为毒性构象,从而显著降低 hPrP90-231 的毒性。分析的所有吖啶衍生物均显示与 hPrP90-231 具有高亲和力结合,但只有 Q3 和 Q10 可显著降低 hPrP90-231 的细胞毒性,其疗效优于吖啶。我们试图将新化合物的细胞保护作用与某些生化参数(与 hPrP90-231 的结合亲和力、固有荧光猝灭、疏水性氨基酸暴露)相关联,但仅与 PK 抗性的降低直接相关,这可能是由于阻止了β-折叠丰富的毒性构象的获得。这些数据为进一步修饰吖啶核的基本侧链和取代基模式提供了有趣的线索,以开发具有改善的抗朊病毒活性的新型化合物,然后在体内实验环境中进行测试。