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将手性、刚性和极性砜基引入羧酸的β位,发现具有口服活性和安全性的 GPR40 激动剂。

Discovery of orally effective and safe GPR40 agonists by incorporating a chiral, rigid and polar sulfoxide into β-position to the carboxylic acid.

机构信息

College of Pharmaceutical Sciences, Soochow University, 199 Renai Road, Suzhou, 215123, China; Department of Chemistry, Shanghai University, 99 Shangda Road, Shanghai, 200444, China; State Key Laboratory of Drug Research, National Center for Drug Screening, Shanghai Institute of Materia Medica, Chinese Academy of Sciences, Shanghai, 201203, China.

State Key Laboratory of Drug Research, National Center for Drug Screening, Shanghai Institute of Materia Medica, Chinese Academy of Sciences, Shanghai, 201203, China.

出版信息

Eur J Med Chem. 2023 May 5;251:115267. doi: 10.1016/j.ejmech.2023.115267. Epub 2023 Mar 11.

Abstract

GPR40 is primarily expressed in pancreatic islet β-cells, and its activation by endogenous ligands of medium to long-chain free fatty acids or synthetic agonists is clinically proved to improve glycemic control by stimulating glucose-dependent insulin secretion. However, most of the reported agonists are highly lipophilic, which might cause lipotoxicity and the off-target effects in CNS. Particularly, the withdrawal of TAK-875 from clinical trials phase III due to liver toxicity concern threw doubt over the long-term safety of targeting GPR40. Improving the efficacy and the selectivity, thus enlarging the therapeutic window would provide an alternative to develop safe GPR40-targeted therapeutics. Herein, by employing an innovative "three-in-one" pharmacophore drug design strategy, the optimal structural features for GPR40 agonist was integrated into one functional group of sulfoxide, which was incorporated into the β-position of the propanoic acid core pharmacophore. As a result, the conformational constraint, polarity as well as chirality endowed by the sulfoxide significantly enhanced the efficacy, selectivity and ADMET properties of the novel (S)- 2-(phenylsulfinyl)acetic acid-based GPR40 agonists. The lead compounds (S)-4a and (S)-4s exhibited robust plasma glucose-lowering effects and insulinotropic action during an oral glucose tolerance test in C57/BL6 mice, excellent pharmacokinetic profile and little hepatobiliary transporter inhibition, marginal cell toxicities against human primary hepatocyte at 100 μM.

摘要

GPR40 主要表达于胰岛β细胞,其内源性中长链游离脂肪酸配体或合成激动剂的激活已被临床证明可通过刺激葡萄糖依赖性胰岛素分泌来改善血糖控制。然而,大多数报道的激动剂具有较高的亲脂性,可能导致脂毒性和中枢神经系统的脱靶效应。特别是,由于对 TAK-875 的肝毒性的担忧,TAK-875 从 III 期临床试验中撤出,这对 GPR40 的长期安全性提出了质疑。提高疗效和选择性,从而扩大治疗窗口,将为开发安全的 GPR40 靶向治疗提供替代方案。在此,通过采用创新的“三位一体”药效团药物设计策略,将 GPR40 激动剂的最佳结构特征整合到亚砜的一个功能基团中,该亚砜被引入丙酸酸核心药效团的β位。结果,亚砜赋予的构象约束、极性和手性显著提高了新型(S)-2-(苯基亚磺酰基)乙酸基 GPR40 激动剂的疗效、选择性和 ADMET 性质。先导化合物(S)-4a 和(S)-4s 在 C57/BL6 小鼠口服葡萄糖耐量试验中表现出强大的降低血糖作用和胰岛素促分泌作用,具有良好的药代动力学特性和对肝胆转运体的抑制作用很小,在 100 μM 时对人原代肝细胞的细胞毒性较小。

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