Department of Biochemistry and Biophysics and UNC Center for AIDS Research, ‡Center for Integrative Chemical Biology and Drug Discovery, Eshelman School of Pharmacy, §Department of Microbiology and Immunology, and ∥Cancer Genetics Program, Lineberger Comprehensive Cancer Center, University of North Carolina at Chapel Hill , Chapel Hill, North Carolina 27599, United States.
Biochemistry. 2013 Jul 23;52(29):4929-40. doi: 10.1021/bi4005232. Epub 2013 Jul 11.
The matrix/capsid processing site in the HIV-1 Gag precursor is likely the most sensitive target to inhibit HIV-1 replication. We have previously shown that modest incomplete processing at the site leads to a complete loss of virion infectivity. In the study presented here, a sensitive assay based on fluorescence polarization that can monitor cleavage at the MA/CA site in the context of the folded protein substrate is described. The substrate, an MA/CA fusion protein, was labeled with the fluorescein-based FlAsH (fluorescein arsenical hairpin) reagent that binds to a tetracysteine motif (CCGPCC) that was introduced within the N-terminal domain of CA. By limiting the size of CA and increasing the size of MA (with an N-terminal GST fusion), we were able to measure significant differences in polarization values as a function of HIV-1 protease cleavage. The sensitivity of the assay was tested in the presence of increasing amounts of an HIV-1 protease inhibitor, which resulted in a gradual decrease in the fluorescence polarization values demonstrating that the assay is sensitive in discerning changes in protease processing. The high-throughput screening assay validation in 384-well plates showed that the assay is reproducible and robust with an average Z' value of 0.79 and average coefficient of variation values of <3%. The robustness and reproducibility of the assay were further validated using the LOPAC(1280) compound library, demonstrating that the assay provides a sensitive high-throughput screening platform that can be used with large compound libraries for identifying novel maturation inhibitors targeting the MA/CA site of the HIV-1 Gag polyprotein.
HIV-1 Gag 前体中的基质/衣壳加工位点可能是抑制 HIV-1 复制的最敏感靶标。我们之前已经表明,该位点的适度不完全加工会导致病毒感染力完全丧失。在本研究中,描述了一种基于荧光偏振的灵敏测定法,该方法可以监测折叠蛋白底物中 MA/CA 位点的切割。该底物是一种 MA/CA 融合蛋白,用荧光素标记的基于 FlAsH(荧光素砷发夹)试剂进行标记,该试剂与 CA 中 N 端结构域内引入的四半胱氨酸基序(CCGPCC)结合。通过限制 CA 的大小并增加 MA 的大小(带有 N 端 GST 融合),我们能够测量作为 HIV-1 蛋白酶切割函数的偏振值的显著差异。该测定法的灵敏度通过在增加量的 HIV-1 蛋白酶抑制剂存在下进行测试,这导致荧光偏振值逐渐降低,表明该测定法灵敏地识别蛋白酶加工的变化。在 384 孔板中进行高通量筛选测定法验证显示,该测定法具有重现性和稳健性,平均 Z'值为 0.79,平均变异系数值<3%。该测定法的稳健性和重现性进一步使用 LOPAC(1280)化合物文库进行验证,表明该测定法提供了一种灵敏的高通量筛选平台,可用于具有大型化合物文库的鉴定,以鉴定针对 HIV-1 Gag 多蛋白 MA/CA 位点的新型成熟抑制剂。