Winner Millicent, Meier Jason, Zierow Swen, Rendon Beatriz E, Crichlow Gregg V, Riggs Randall, Bucala Richard, Leng Lin, Smith Ned, Lolis Elias, Trent John O, Mitchell Robert A
Molecular Targets Program, University of Louisville, KY, USA.
Cancer Res. 2008 Sep 15;68(18):7253-7. doi: 10.1158/0008-5472.CAN-07-6227.
Although chemokine and growth factor receptors are attractive and popular targets for cancer therapeutic intervention, structure-based targeting of the ligands themselves is generally not considered practical. New evidence indicates that a notable exception to this is macrophage migration inhibitory factor (MIF). MIF, an autocrine- and paracrine-acting cytokine/growth factor, plays a pivotal role in both the initiation and maintenance of neoplastic diseases. MIF possesses a nonphysiologic enzymatic activity that is evolutionarily well-conserved. Although small molecule antagonists of MIFs enzymatic active site have been reported to inhibit biological activities of MIF, universally high IC(50)s have limited their clinical appeal. Using a computational virtual screening strategy, we have identified a unique small molecule inhibitor that serves as a suicide substrate for MIF, resulting in the covalent modification of the catalytically active NH(2)-terminal proline. Our studies further reveal that this compound, 4-iodo-6-phenylpyrimidine (4-IPP), is approximately 5x to 10x times more potent in blocking MIF-dependent catalysis and lung adenocarcinoma cell migration and anchorage-independent growth than the prototypical MIF inhibitor, ISO-1. Finally, using an in silico combinatorial optimization strategy, we have identified four unique congeners of 4-IPP that exhibit MIF inhibitory activity at concentrations 10x to 20x lower than that of parental 4-IPP.
尽管趋化因子和生长因子受体是癌症治疗干预中引人关注且热门的靶点,但基于结构对配体本身进行靶向治疗通常被认为不切实际。新证据表明,巨噬细胞迁移抑制因子(MIF)是一个显著的例外。MIF是一种自分泌和旁分泌作用的细胞因子/生长因子,在肿瘤疾病的起始和维持过程中都起着关键作用。MIF具有一种在进化过程中高度保守的非生理性酶活性。尽管据报道MIF酶活性位点的小分子拮抗剂可抑制MIF的生物学活性,但普遍较高的半数抑制浓度(IC50)限制了它们的临床应用价值。通过计算虚拟筛选策略,我们鉴定出一种独特的小分子抑制剂,它作为MIF的自杀底物,导致催化活性的NH2末端脯氨酸发生共价修饰。我们的研究进一步表明,这种化合物4-碘-6-苯基嘧啶(4-IPP)在阻断MIF依赖性催化、肺腺癌细胞迁移和非锚定依赖性生长方面,比典型的MIF抑制剂ISO-1强约5至10倍。最后,通过计算机辅助组合优化策略,我们鉴定出4-IPP的四种独特类似物,它们在比亲本4-IPP低10至20倍的浓度下表现出MIF抑制活性。