Department of Gynecological Oncology, Zhongnan Hospital of Wuhan University, School of Pharmaceutical Sciences, Wuhan University, Wuhan, 430071, China.
State Key Laboratory of Biocatalysis and Enzyme Engineering, Hubei Hongshan Laboratory, Hubei Collaborative Innovation Center for Green Transformation of Bio-Resources, Hubei Key Laboratory of Industrial Biotechnology, School of Life Sciences, Hubei University, Wuhan, 430062, China.
Eur J Med Chem. 2023 May 5;253:115328. doi: 10.1016/j.ejmech.2023.115328. Epub 2023 Apr 6.
Drug resistance is a major challenge in conventional endocrine therapy for estrogen receptor (ER) positive breast cancer (BC). BC is a multifactorial disease, in which simultaneous aromatase (ARO) inhibition and ERα degradation may effectively inhibit the signal transduction of both proteins, thus potentially overcoming drug resistance caused by overexpression or mutation of target proteins. In this study, guided by the X-ray structure of a hit compound 30a in complex with ER-Y537S, a structure-based optimization was performed to get a series of multiacting inhibitors targeting both ERα and ARO, and finally a novel class of potent selective estrogen receptor degraders (SERDs) based on a three-dimensional oxabicycloheptene sulfonamide (OBHSA) scaffold equipped with aromatase inhibitor (AI) activity were identified. Of these dual-targeting SERD-AI hybrids, compound 31q incorporating a 1H-1,2,4-triazole moiety showed excellent ERα degradation activity, ARO inhibitory activity and remarkable antiproliferative activity against BC resistant cells. Furthermore, 31q manifested efficient tumor suppression in MCF-7 tumor xenograft models. Taken together, our study reported for the first time the highly efficient dual-targeting SERD-AI hybrid compounds, which may lay the foundation of translational research for improved treatment of endocrine-resistant BC.
耐药性是雌激素受体 (ER) 阳性乳腺癌 (BC) 常规内分泌治疗的主要挑战。BC 是一种多因素疾病,同时抑制芳香酶 (ARO) 和 ERα 降解可能有效地抑制这两种蛋白的信号转导,从而潜在地克服由于靶蛋白过表达或突变引起的耐药性。在这项研究中,根据与 ER-Y537S 复合物的命中化合物 30a 的 X 射线结构,进行了基于结构的优化,以获得一系列针对 ERα 和 ARO 的多作用抑制剂,最终基于具有芳香酶抑制剂 (AI) 活性的三维氧杂双环庚烷磺酰胺 (OBHSA) 支架,鉴定了一类新型强效选择性雌激素受体降解剂 (SERD)。在这些双靶向 SERD-AI 杂合物中,包含 1H-1,2,4-三唑部分的化合物 31q 表现出优异的 ERα 降解活性、ARO 抑制活性和对 BC 耐药细胞的显著增殖抑制活性。此外,31q 在 MCF-7 肿瘤异种移植模型中表现出有效的肿瘤抑制作用。总之,我们的研究首次报道了高效的双靶向 SERD-AI 杂合化合物,这可能为改善内分泌耐药性 BC 的治疗奠定转化研究的基础。