Drug Discovery and Biomedical Sciences, College of Pharmacy, University of South Carolina, 715 Sumter Street, Columbia, South Carolina 29208, United States.
ACS Chem Biol. 2023 Jul 21;18(7):1642-1652. doi: 10.1021/acschembio.3c00269. Epub 2023 Jul 11.
Polo-like kinase 1 (PLK1) is an essential protein kinase with multiple roles in mitotic progression. PLK1 consists of a kinase domain (KD) and a phosphopeptide-binding polobox domain (PBD), which is responsible for substrate recognition and subcellular localization. The regulation of PLK1 involves an autoinhibitory conformation in which KD and PBD interact. Our previous work identified PBD-binding molecules termed abbapolins that inhibit the cellular phosphorylation of a PLK1 substrate and induce the loss of intracellular PLK1. Here, we describe a comparison of the abbapolin activity with that of KD inhibitors to gain insight into conformational features of PLK1. As measured by a cellular thermal shift assay, abbapolins produce ligand-induced thermal stabilization of PLK1. In contrast, KD inhibitors decreased the soluble PLK1, suggesting that catalytic-site binding causes a less thermally stable PLK1 conformation. Binding measurements with full-length PLK1 and a KD inhibitor also demonstrated a conformational change. Interestingly, the cellular consequences of KD versus PBD engagement contrast as KD binding causes the accumulation of intracellular PLK1, whereas PBD binding produces a striking loss of nuclear PLK1. These data are consistent with the relief of autoinhibited PLK1 by KD binders; an explanation for these observations is presented using structures for the catalytic domain and full-length PLK1 predicted by AlphaFold. Collectively, the results highlight an underappreciated aspect of targeting PLK1, namely, conformational perturbations induced by KD versus PBD binding. In addition to their significance for PBD-binding ligands, these observations have implications for the development of ATP-competitive PLK1 inhibitors because catalytic inhibitors may conversely promote PLK1 noncatalytic functions, which may explain their lack of clinical efficacy to date.
丝氨酸/苏氨酸蛋白激酶 PLK1 是一种在有丝分裂进展中具有多种作用的必需蛋白激酶。PLK1 由激酶结构域(KD)和磷酸肽结合的 polobox 结构域(PBD)组成,负责底物识别和亚细胞定位。PLK1 的调节涉及 KD 和 PBD 相互作用的自动抑制构象。我们之前的工作鉴定了 PBD 结合分子 abbapolins,它们抑制 PLK1 底物的细胞磷酸化,并诱导细胞内 PLK1 的丢失。在这里,我们比较了 abbapolin 的活性与 KD 抑制剂的活性,以深入了解 PLK1 的构象特征。如细胞热转移测定法所测,abbapolins 使 PLK1 的配体诱导热稳定性增加。相比之下,KD 抑制剂降低了可溶性 PLK1,表明催化位点结合导致 PLK1 构象的热稳定性降低。与全长 PLK1 和 KD 抑制剂的结合测量也表明了构象变化。有趣的是,KD 与 PBD 结合的细胞后果形成对比,因为 KD 结合导致细胞内 PLK1 的积累,而 PBD 结合则导致核内 PLK1 的明显丢失。这些数据与 KD 结合物对自动抑制的 PLK1 的释放一致;使用 AlphaFold 预测的催化结构域和全长 PLK1 的结构提出了对这些观察结果的解释。总的来说,这些结果突出了靶向 PLK1 的一个被低估的方面,即 KD 与 PBD 结合引起的构象扰动。除了对 PBD 结合配体的重要性外,这些观察结果对 ATP 竞争性 PLK1 抑制剂的开发也具有意义,因为催化抑制剂可能相反地促进 PLK1 的非催化功能,这可以解释迄今为止它们缺乏临床疗效的原因。