Robinson Ralph P, Buckbinder Leonard, Haugeto Amber I, McNiff Patricia A, Millham Michele L, Reese Matthew R, Schaefer Jean F, Abramov Yuriy A, Bordner Jon, Chantigny Yves A, Kleinman Edward F, Laird Ellen R, Morgan Bradley P, Murray John C, Salter Eben D, Wessel Matthew D, Yocum Sue A
Pfizer Global Research & Development, Groton Laboratories, Eastern Point Road, Groton, Connecticut 06340, USA.
J Med Chem. 2009 Mar 26;52(6):1731-43. doi: 10.1021/jm801512v.
As exemplified by the lead compound 2, octahydrophenanthrene-2,7-diol analogues exhibit the profile of a pathway-selective or "dissociated" agonist of the glucocorticoid receptor (GR), retaining the potent activity that glucocorticoids have for transrepression (as measured by inhibition of IL-1 induced MMP-13 expression) but showing an attenuated capacity for transactivation (as measured in an MMTV luciferase reporter assay). With the guidance of a homology model of the GR ligand binding domain, structural modifications to 2 were carried out that were successful in replacing the allyl and propynyl side chains with groups likely to be more chemically stable and less likely to produce toxic metabolites. Key to success was the introduction of an additional hydroxyl group onto the tricyclic carbon framework of the series.
以先导化合物2为例,八氢菲-2,7-二醇类似物表现出糖皮质激素受体(GR)的途径选择性或“解离”激动剂的特征,保留了糖皮质激素对反式抑制的强效活性(通过抑制IL-1诱导的MMP-13表达来衡量),但显示出反式激活能力减弱(在MMTV荧光素酶报告基因测定中测量)。在GR配体结合域同源模型的指导下,对2进行了结构修饰,成功地用可能更具化学稳定性且不太可能产生有毒代谢物的基团取代了烯丙基和丙炔基侧链。成功的关键是在该系列的三环碳骨架上引入了一个额外的羟基。