Wu Dan, Zhang Shao-Yong, Liu Ying-Qian, Wu Xiao-Bing, Zhu Gao-Xiang, Zhang Yan, Wei Wei, Liu Huan-Xiang, Chen An-Liang
Local and National Joint Engineering Laboratory of Biopesticide High-Efficient Preparation Technology, Zhejiang A&F University, Lin'an 311300, China.
School of Pharmacy, Lanzhou University, Lanzhou 730000, China.
Molecules. 2015 May 13;20(5):8634-53. doi: 10.3390/molecules20058634.
In continuation of our program aimed at the development of natural product-based pesticidal agents, three series of novel camptothecin derivatives were designed, synthesized, and evaluated for their biological activities against T. Cinnabarinus, B. brassicae, and B. xylophilus. All of the derivatives showed good-to-excellent activity against three insect species tested, with LC50 values ranging from 0.00761 to 0.35496 mmol/L. Remarkably, all of the compounds were more potent than CPT against T. Cinnabarinus, and compounds 4d and 4c displayed superior activity (LC50 0.00761 mmol/L and 0.00942 mmol/L, respectively) compared with CPT (LC50 0.19719 mmol/L) against T. Cinnabarinus. Based on the observed bioactivities, preliminary structure-activity relationship (SAR) correlations were also discussed. Furthermore, a three-dimensional quantitative structure-activity relationship (3D-QSAR) model using comparative molecular field analysis (CoMFA) was built. The model gave statistically significant results with the cross-validated q2 values of 0.580 and correlation coefficient r2 of 0.991 and of 0.993. The QSAR analysis indicated that the size of the substituents play an important in the activity of 7-modified camptothecin derivatives. These findings will pave the way for further design, structural optimization, and development of camptothecin-derived compounds as pesticidal agents.
在我们旨在开发基于天然产物的杀虫剂的项目持续推进过程中,设计、合成了三个系列的新型喜树碱衍生物,并对它们针对朱砂叶螨、甘蓝夜蛾和松材线虫的生物活性进行了评估。所有衍生物对测试的三种昆虫均表现出良好到优异的活性,LC50值范围为0.00761至0.35496 mmol/L。值得注意的是,所有化合物对朱砂叶螨的活性均比喜树碱更强,并且化合物4d和4c对朱砂叶螨的活性(LC50分别为0.00761 mmol/L和0.00942 mmol/L)优于喜树碱(LC50为0.19719 mmol/L)。基于观察到的生物活性,还讨论了初步的构效关系(SAR)相关性。此外,利用比较分子场分析(CoMFA)建立了三维定量构效关系(3D-QSAR)模型。该模型给出了具有统计学意义的结果,交叉验证q2值为0.580,相关系数r2为0.991,外部验证r2为0.993。QSAR分析表明,取代基的大小对7-修饰喜树碱衍生物的活性起着重要作用。这些发现将为进一步设计、结构优化以及开发作为杀虫剂的喜树碱衍生化合物铺平道路。