Graduate School of Pharmaceutical Sciences, Osaka University, 1-6 Yamada-oka Suita, Osaka, 565-0871, Japan.
Department of Chemistry, Faculty of Sciences, University of Kinshasa, Kinshasa, Democratic Republic of the Congo.
J Nat Med. 2020 Sep;74(4):702-709. doi: 10.1007/s11418-020-01422-9. Epub 2020 Jun 11.
Africa Trypanosomiasis remains a serious health problem, but the approved drugs for this disease are so few that novel trypanocidal compounds are demanded. In search for trypanocidal principles from medicinal plants, we found MeOH extracts of Meliae Cortex with potent activity through the screening from about 300 kinds of methanolic extract. By bioassay-guided fractionation from this extract through the liquid-liquid partition and subsequent chromatographic technique using silica gel and ODS, finally we disclosed toosendanin (1) and its relatives as active principles. These active congeners showed not only potent trypanocidal activity but also little cytotoxicity to display the excellent selective index. Taking the isolated amount as well as trypanocidal activity into consideration, 1 was disclosed to be the responsible active principle in Meliae Cortex. Additionally, the derivatives of 1 were chemically prepared from 1 and bioactivity of them were also evaluated. Through the comparison with their trypanocidal activity among the isolated relatives and the synthesized derivatives of 1, the epoxide moiety was revealed to be essential for their potent trypanocidal activity. Furthermore, 3-O-acetyl group and 7-hydroxyl group were presumed to be important functional groups and introduction of methylpropionyl group into hemiacetal hydroxy moiety was clarified to enhance their typanocidal activity.
非洲锥虫病仍然是一个严重的健康问题,但对此病的批准药物却很少,因此需要新型的杀锥虫化合物。在从药用植物中寻找杀锥虫原则的过程中,我们通过对大约 300 种甲醇提取物的筛选,发现了具有很强活性的桃金娘科树皮的甲醇提取物。通过从该提取物中进行基于生物测定的分级分离,通过液-液分配和随后使用硅胶和 ODS 的色谱技术,最终我们揭示了川楝素(1)及其类似物作为活性成分。这些活性同系物不仅表现出很强的杀锥虫活性,而且对细胞毒性很小,显示出极好的选择性指数。考虑到分离量和杀锥虫活性,1 被揭示为桃金娘科树皮中的有效活性成分。此外,还从 1 化学制备了 1 的衍生物,并评估了它们的生物活性。通过与分离的同系物和 1 的合成衍生物的杀锥虫活性进行比较,揭示了环氧化物部分对于它们的强杀锥虫活性是必不可少的。此外,3-O-乙酰基和 7-羟基被认为是重要的功能基团,将甲基丙酰基引入半缩醛羟基被阐明可以增强它们的杀锥虫活性。