Discovery Science and Technology, RTI International, 3040 Cornwallis Rd., Research Triangle Park, NC 27709-2194, USA.
Discovery Science and Technology, RTI International, 3040 Cornwallis Rd., Research Triangle Park, NC 27709-2194, USA.
Bioorg Med Chem. 2019 Aug 15;27(16):3632-3649. doi: 10.1016/j.bmc.2019.07.002. Epub 2019 Jul 4.
Antagonists of type 1 cannabinoid receptors (CB1) may be useful in treating diabetes, hepatic disorders, and fibrosis. Otenabant (1) is a potent and selective CB1 inverse agonist that was under investigation as an anti-obesity agent, but its development was halted once adverse effects associated with another marketed inverse agonist rimonabant (2) became known. Non-tissue selective antagonists of CB1 that have high levels of brain penetration produce adverse effects in a small subset of patients including anxiety, depression and suicidal ideation. Currently, efforts are underway to produce compounds that have limited brain penetration. In this report, novel analogs of 1 are explored to develop and test strategies for peripheralization. The piperidine of 1 is studied as a linker, which is functionalized with alkyl, heteroalkyl, aryl and heteroaryl groups using a connector in the form of an amine, amide, sulfonamide, sulfamide, carbamate, oxime, amidine, or guanidine. We also report more polar replacements for the 4-chlorophenyl group in the 9-position of the purine core, which improve calculated physical properties of the molecules. These studies resulted in compounds such as 75 that are potent inverse agonists of hCB1 with exceptional selectivity for hCB1 over hCB2. SAR studies revealed ways to adjust physical properties to limit brain exposure.
1 型大麻素受体(CB1)拮抗剂可能有助于治疗糖尿病、肝疾病和纤维化。奥坦布烷(1)是一种强效且选择性的 CB1 反向激动剂,曾作为抗肥胖药物进行研究,但由于另一种已上市的反向激动剂利莫那班(2)的不良反应被发现,其研发被停止。对 CB1 具有高脑穿透性的非组织选择性拮抗剂会在一小部分患者中引起不良反应,包括焦虑、抑郁和自杀意念。目前,正在努力开发脑穿透性有限的化合物。在本报告中,探索了 1 的新型类似物,以开发和测试外周化策略。将 1 的哌啶用作连接体,使用胺、酰胺、磺酰胺、磺酰胺、氨基甲酸酯、肟、脒或胍的形式的连接器将其官能化,用烷基、杂烷基、芳基和杂芳基进行修饰。我们还报告了嘌呤核 9 位的 4-氯苯基的更极性替代品,这改善了分子的计算物理性质。这些研究产生了 75 等化合物,它们是 hCB1 的强效反向激动剂,对 hCB1 具有出色的选择性,对 hCB2 没有活性。SAR 研究揭示了调整物理性质以限制脑暴露的方法。