Sung Yu-Shien, Kerimoglu Baris, Ooi Aikseng, Tomat Elisa
Department of Chemistry and Biochemistry, The University of Arizona, 1306 E. University Blvd., Tucson, Arizona 85721-0041, United States.
Department of Pharmacology and Toxicology, College of Pharmacy, The University of Arizona, 1703 E. Mabel St., Tucson, Arizona 85721, United States.
ACS Med Chem Lett. 2022 Aug 18;13(9):1452-1458. doi: 10.1021/acsmedchemlett.2c00250. eCollection 2022 Sep 8.
Glycoconjugation strategies in anticancer drug discovery exploit the high expression of glucose transporters in malignant cells to achieve preferential uptake and hence attractive pharmacological characteristics of increased therapeutic windows and decreased unwanted toxicity. Here we present the design of glycoconjugated prochelators of aroylhydrazone AH1, an antiproliferative scavenger that targets the increased iron demand of rapidly proliferating malignant cells. The constructs feature a monosaccharide (d-glucose, d-glucosamine, or glycolytic inhibitor 2-deoxy-d-glucose) connected at the C2 or C6 position via a short linker, which masks the chelator through a disulfide bond susceptible to intracellular reduction. Cellular assays showed that the glycoconjugates rely on the GLUT1 transporter for uptake, lead to intracellular iron deprivation, and present antiproliferative activity. Ectopic overexpression of GLUT1 in malignant and normal cells increased the uptake and toxicity of the glycoconjugated prochelators, demonstrating that these compounds are well suited for targeting cells overexpressing glucose transporters and therefore for selective iron sequestration in malignant cells.
抗癌药物研发中的糖缀合策略利用恶性细胞中葡萄糖转运蛋白的高表达来实现优先摄取,从而获得具有增加治疗窗和降低不良毒性等诱人药理学特性。在此,我们展示了芳酰腙AH1糖缀合前螯合剂的设计,AH1是一种抗增殖清除剂,可靶向快速增殖的恶性细胞增加的铁需求。这些构建体的特征是通过短连接子在C2或C6位置连接单糖(d-葡萄糖、d-葡糖胺或糖酵解抑制剂2-脱氧-d-葡萄糖),该连接子通过易受细胞内还原作用的二硫键掩盖螯合剂。细胞实验表明,这些糖缀合物依赖GLUT1转运蛋白进行摄取,导致细胞内铁缺乏,并呈现抗增殖活性。在恶性细胞和正常细胞中异位过表达GLUT1会增加糖缀合前螯合剂的摄取和毒性,表明这些化合物非常适合靶向过表达葡萄糖转运蛋白的细胞,因此适合在恶性细胞中进行选择性铁螯合。