Department of Pharmacology, School of Pharmacy, Fujian Medical University (FMU), Fuzhou, PR China; Department of Pharmacy, The Second Affiliated Hospital of Fujian Medical University, Quanzhou, PR China.
Department of Pharmacology, School of Pharmacy, Fujian Medical University (FMU), Fuzhou, PR China; Fujian Key Laboratory of Natural Medicine Pharmacology, Fujian Medical University (FMU), Fuzhou, PR China.
Bioorg Med Chem. 2022 Sep 15;70:116912. doi: 10.1016/j.bmc.2022.116912. Epub 2022 Jul 8.
Poly ADP-ribose polymerase 1 (PARP1) plays an essential role in DNA repair signaling, rendering it an attractive target for cancer treatment. Despite the success of PARP1 inhibitors (PARPis), only a few patients can currently benefit from PARPis. Moreover, drug resistance to PARPis occurs during clinical treatment. Natural and acquired resistance to PARPis has forced us to seek new therapeutic approaches that target PARP1. Here, we synthesized a series of compounds by proteolysis-targeting chimera (PROTAC) technology to directly degrade the PARP1 protein. We found that CN0 (compound 3) with no polyethylene glycol (PEG) linker can degrade the PARP1 protein through the proteasome pathway. More importantly, CN0 could inhibit DNA damage repair, resulting in highly efficient accumulation of cytosolic DNA fragments due to unresolved unrepaired DNA lesions when combined with daunorubicin (DNR). Therefore, CN0 can activate the cyclic GMP-AMP synthase/stimulator of the interferon gene (cGAS/STING) pathway of innate immunity and then spread the resulting inflammatory signals, thereby reshaping the tumor microenvironment, which may eventually enhance T cell killing of tumor cells.
聚 ADP-核糖聚合酶 1(PARP1)在 DNA 修复信号转导中发挥着重要作用,使其成为癌症治疗的一个有吸引力的靶点。尽管 PARP1 抑制剂(PARPi)取得了成功,但目前只有少数患者可以从中受益。此外,在临床治疗中会出现对 PARPi 的耐药性。天然和获得性对 PARPi 的耐药性迫使我们寻求新的治疗方法,以靶向 PARP1。在这里,我们通过蛋白酶靶向嵌合体(PROTAC)技术合成了一系列化合物,以直接降解 PARP1 蛋白。我们发现,没有聚乙二醇(PEG)接头的 CN0(化合物 3)可以通过蛋白酶体途径降解 PARP1 蛋白。更重要的是,CN0 可以抑制 DNA 损伤修复,当与柔红霉素(DNR)联合使用时,由于未解决的未修复的 DNA 损伤,导致细胞质 DNA 片段的高效积累。因此,CN0 可以激活先天免疫的环鸟苷酸-腺苷酸合酶/干扰素基因刺激物(cGAS/STING)途径,然后传播由此产生的炎症信号,从而重塑肿瘤微环境,这可能最终增强 T 细胞对肿瘤细胞的杀伤作用。