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Discovery of Pyrrolidine-Containing GPR40 Agonists: Stereochemistry Effects a Change in Binding Mode.

Elizabeth Anne JuricaXimao WuKristin N WilliamsAndres S HernandezDavid S NirschlRichard A RampullaArvind MathurMin ZhouGary CaoChunshan XieBiji JacobHong CaiTao WangBrian J MurphyHeng LiuCarrie XuLori K KunselmanMichael B HicksQin SunDora M SchnurDoree F SitkoffElizabeth A DierksAtsu ApedoDouglas B MooreKimberly A FosterMary Ellen CvijicReshma PanemangaloreNeil A FlynnBrad D MaxwellYang HongYuan TianJason J WilkesBradley A ZinkerJean M WhaleyJoel C BarrishJeffrey A RoblWilliam R EwingBruce A Ellsworth
Published in: Journal of medicinal chemistry (2017)
A novel series of pyrrolidine-containing GPR40 agonists is described as a potential treatment for type 2 diabetes. The initial pyrrolidine hit was modified by moving the position of the carboxylic acid, a key pharmacophore for GPR40. Addition of a 4-cis-CF3 to the pyrrolidine improves the human GPR40 binding Ki and agonist efficacy. After further optimization, the discovery of a minor enantiomeric impurity with agonist activity led to the finding that enantiomers (R,R)-68 and (S,S)-68 have differential effects on the radioligand used for the binding assay, with (R,R)-68 potentiating the radioligand and (S,S)-68 displacing the radioligand. Compound (R,R)-68 activates both Gq-coupled intracellular Ca2+ flux and Gs-coupled cAMP accumulation. This signaling bias results in a dual mechanism of action for compound (R,R)-68, demonstrating glucose-dependent insulin and GLP-1 secretion in vitro. In vivo, compound (R,R)-68 significantly lowers plasma glucose levels in mice during an oral glucose challenge, encouraging further development of the series.
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