Business Unit Oncology, Nerviano Medical Sciences, Nerviano, Italy.
Nat Chem Biol. 2013 Sep;9(9):548-56. doi: 10.1038/nchembio.1313. Epub 2013 Jul 28.
VCP (also known as p97 or Cdc48p in yeast) is an AAA(+) ATPase regulating endoplasmic reticulum-associated degradation. After high-throughput screening, we developed compounds that inhibit VCP via different mechanisms, including covalent modification of an active site cysteine and a new allosteric mechanism. Using photoaffinity labeling, structural analysis and mutagenesis, we mapped the binding site of allosteric inhibitors to a region spanning the D1 and D2 domains of adjacent protomers encompassing elements important for nucleotide-state sensing and ATP hydrolysis. These compounds induced an increased affinity for nucleotides. Interference with nucleotide turnover in individual subunits and distortion of interprotomer communication cooperated to impair VCP enzymatic activity. Chemical expansion of this allosteric class identified NMS-873, the most potent and specific VCP inhibitor described to date, which activated the unfolded protein response, interfered with autophagy and induced cancer cell death. The consistent pattern of cancer cell killing by covalent and allosteric inhibitors provided critical validation of VCP as a cancer target.
VCP(也称为酵母中的 p97 或 Cdc48p)是一种 AAA(+)ATP 酶,可调节内质网相关降解。通过高通量筛选,我们开发了通过不同机制抑制 VCP 的化合物,包括活性位点半胱氨酸的共价修饰和新的别构机制。通过光亲和标记、结构分析和突变,我们将别构抑制剂的结合位点定位到跨越相邻原体的 D1 和 D2 结构域的区域,该区域包含核苷酸状态感应和 ATP 水解的重要元件。这些化合物诱导核苷酸结合亲和力增加。干扰单个亚基中的核苷酸周转和扭曲亚基间的通讯协同作用,损害 VCP 的酶活性。该别构类别的化学扩展鉴定出 NMS-873,这是迄今为止描述的最有效和最特异的 VCP 抑制剂,它能激活未折叠蛋白反应,干扰自噬并诱导癌细胞死亡。共价和别构抑制剂对癌细胞的一致杀伤模式为 VCP 作为癌症靶点提供了关键验证。