Barker P L, Bullens S, Bunting S, Burdick D J, Chan K S, Deisher T, Eigenbrot C, Gadek T R, Gantzos R, Lipari M T
Bioorganic Chemistry, Genentech, Inc., South San Francisco, California 94080.
J Med Chem. 1992 May 29;35(11):2040-8. doi: 10.1021/jm00089a014.
Stimulation of platelets activates GPIIbIIIa, the heterodimeric integrin receptor, to bind fibrinogen (Fg), which results in platelet aggregation. GPIIbIIIa/Fg binding inhibitors are potentially suitable for acute use during and after thrombolytic therapy as antithrombotic agents. Incorporation of the tripeptide sequence Arg-Gly-Asp (RGD), a common structural element of many integrin ligands, into cyclic peptides produced a series of peptides of the general structure BrAc-(AA1)-RGD-Cys-OH, which were prepared by solid-phase peptide synthesis. Cyclization was accomplished by reaction of the N-terminal bromoacetyl group with the cysteine sulfhydryl at pH 8 at high dilution, resulting in thioether-bridged cyclic peptides [cyclo-S-Ac-(AA1)-RGD-Cys-OH]. Use of alpha-substituted bromoacetyl groups gave rise to an analogous series of acetyl-substituted thioether-bridged cyclic peptides. Oxidation of the thioethers produced separable diastereomeric sulfoxide-bridged cyclic peptides. After thorough evaluation in a GPIIbIIIa ELISA assay and a platelet aggregation assay, G-4120 (70A; AA1 = D-Tyr; sulfoxide bridge) was selected for further investigation as an antithrombotic agent. G-4120 was equipotent in the platelet aggregation assay to kistrin, a highly potent inhibitor of fibrinogen-mediated platelet aggregation isolated from snake venom (IC50 = 0.15 microM).
血小板的激活会使异二聚体整合素受体糖蛋白IIbIIIa(GPIIbIIIa)与纤维蛋白原(Fg)结合,从而导致血小板聚集。GPIIbIIIa/Fg结合抑制剂作为抗血栓药物,在溶栓治疗期间及之后的急性使用中可能是合适的。将许多整合素配体的常见结构元件——三肽序列精氨酸-甘氨酸-天冬氨酸(Arg-Gly-Asp,RGD)引入环肽中,产生了一系列具有一般结构BrAc-(AA1)-RGD-Cys-OH的肽,这些肽通过固相肽合成制备。环化是通过N端溴乙酰基在pH 8的高稀释度下与半胱氨酸巯基反应完成的,生成硫醚桥连的环肽[环-S-乙酰基-(AA1)-RGD-Cys-OH]。使用α-取代的溴乙酰基产生了类似的一系列乙酰基取代的硫醚桥连环肽。硫醚的氧化产生了可分离的非对映体亚砜桥连环肽。在糖蛋白IIbIIIa酶联免疫吸附测定(ELISA)和血小板聚集测定中经过全面评估后,选择G-4120(70A;AA1 = D-酪氨酸;亚砜桥)作为抗血栓药物进行进一步研究。在血小板聚集测定中,G-4120与蛇毒中分离出的纤维蛋白原介导的血小板聚集的高效抑制剂抑肽酶效力相当(IC50 = 0.15 microM)。