Zhang Meng-Qi, Zhang Xiao-Le, Li Yan, Fan Wen-Jia, Wang Yong-Hua, Hao Ming, Zhang Shu-Wei, Ai Chun-Zhi
Department of Materials Science and Chemical Engineering, Dalian University of Technology, Dalian, Liaoning 116024, China; E-Mails:
Int J Mol Sci. 2011;12(9):5999-6023. doi: 10.3390/ijms12095999. Epub 2011 Sep 16.
MGluR2 is G protein-coupled receptor that is targeted for diseases like anxiety, depression, Parkinson's disease and schizophrenia. Herein, we report the three-dimensional quantitative structure-activity relationship (3D-QSAR) studies of a series of 1,3-dihydrobenzo[ b][1,4]diazepin-2-one derivatives as mGluR2 antagonists. Two series of models using two different activities of the antagonists against rat mGluR2, which has been shown to be very similar to the human mGluR2, (activity I: inhibition of [(3)H]-LY354740; activity II: mGluR2 (1S,3R)-ACPD inhibition of forskolin stimulated cAMP.) were derived from datasets composed of 137 and 69 molecules respectively. For activity I study, the best predictive model obtained from CoMFA analysis yielded a Q(2) of 0.513, R(2) (ncv) of 0.868, R(2) (pred) = 0.876, while the CoMSIA model yielded a Q(2) of 0.450, R(2) (ncv) = 0.899, R(2) (pred) = 0.735. For activity II study, CoMFA model yielded statistics of Q(2) = 0.5, R(2) (ncv) = 0.715, R(2) (pred) = 0.723. These results prove the high predictability of the models. Furthermore, a combined analysis between the CoMFA, CoMSIA contour maps shows that: (1) Bulky substituents in R(7), R(3) and position A benefit activity I of the antagonists, but decrease it when projected in R(8) and position B; (2) Hydrophilic groups at position A and B increase both antagonistic activity I and II; (3) Electrostatic field plays an essential rule in the variance of activity II. In search for more potent mGluR2 antagonists, two pharmacophore models were developed separately for the two activities. The first model reveals six pharmacophoric features, namely an aromatic center, two hydrophobic centers, an H-donor atom, an H-acceptor atom and an H-donor site. The second model shares all features of the first one and has an additional acceptor site, a positive N and an aromatic center. These models can be used as guidance for the development of new mGluR2 antagonists of high activity and selectivity. This work is the first report on 3D-QSAR modeling of these mGluR2 antagonists. All the conclusions may lead to a better understanding of the mechanism of antagonism and be helpful in the design of new potent mGluR2 antagonists.
代谢型谷氨酸受体2(mGluR2)是一种G蛋白偶联受体,与焦虑症、抑郁症、帕金森病和精神分裂症等疾病有关。在此,我们报告了一系列1,3 - 二氢苯并[b][1,4]二氮杂卓 - 2 - 酮衍生物作为mGluR2拮抗剂的三维定量构效关系(3D - QSAR)研究。使用拮抗剂针对大鼠mGluR2的两种不同活性构建了两个系列的模型,已证明大鼠mGluR2与人mGluR2非常相似,(活性I:抑制[³H] - LY354740;活性II:mGluR2对(1S,3R) - ACPD刺激的福斯高林诱导的环磷酸腺苷(cAMP)的抑制作用。)分别从由137个和69个分子组成的数据集中得出。对于活性I研究,从比较分子场分析(CoMFA)获得的最佳预测模型的交叉验证系数(Q²)为0.513,非交叉验证系数(R²(ncv))为0.868,预测系数(R²(pred)) = 0.876,而比较分子相似性指数分析(CoMSIA)模型的Q²为0.450,R²(ncv) = 0.899,R²(pred) = 0.735。对于活性II研究,CoMFA模型的统计数据为Q² = 0.5,R²(ncv) = 0.715,R²(pred) = 0.723。这些结果证明了模型的高预测性。此外,CoMFA和CoMSIA等高线图之间的联合分析表明:(1)R(7)、R(3)和A位的大体积取代基有利于拮抗剂的活性I,但当投影到R(8)和B位时活性降低;(2)A位和B位的亲水性基团增加了拮抗活性I和II;(3)静电场在活性II的变化中起重要作用。为了寻找更有效的mGluR2拮抗剂,针对这两种活性分别开发了两个药效团模型。第一个模型揭示了六个药效团特征,即一个芳香中心、两个疏水中心、一个氢供体原子、一个氢受体原子和一个氢供体位点。第二个模型具有第一个模型的所有特征,并具有一个额外的受体位点、一个带正电的氮原子和一个芳香中心。这些模型可作为开发高活性和高选择性新型mGluR2拮抗剂的指导。这项工作是关于这些mGluR2拮抗剂的3D - QSAR建模的首次报告。所有这些结论可能有助于更好地理解拮抗作用机制,并有助于设计新型强效mGluR2拮抗剂。