Das Sonia G, Hermanson David L, Bleeker Nicholas, Lowman Xazmin, Li Yunfang, Kelekar Ameeta, Xing Chengguo
Department of Medicinal Chemistry, College of Pharmacy, University of Minnesota, 308 Harvard Street SE, Minneapolis, Minnesota 55455, USA.
ACS Chem Biol. 2013 Feb 15;8(2):327-35. doi: 10.1021/cb300460f. Epub 2012 Nov 5.
Multidrug resistance (MDR) is a major hurdle in the treatment of cancer, and there is a pressing need for new therapies. We have recently developed ethyl 2-amino-6-(3,5-dimethoxyphenyl)-4-(2-ethoxy-2-oxoethyl)-4H-chromene-3-carboxylate (CXL017), derived from a dual inhibitor of Bcl-2 and SERCA proteins, sHA 14-1, with selective cytotoxicity toward MDR cancer cell lines in vitro. In this study, we present new evidence for its therapeutic potential in treatment of MDR cancers and offer mechanistic insights toward its preferential targeting of drug-resistant cancer. CXL017 selectively suppressed the growth of tumors derived from the MDR cancer cell line, HL60/MX2, in vivo. In addition, even after chronic exposure to CXL017, HL60/MX2 failed to develop stable resistance to CXL017, whereas it acquired >2000-fold resistance to cytarabine (Ara-C), the major first-line chemotherapy for the treatment of acute myeloid leukemia (AML). Remarkably, instead of acquiring further cross-resistance, HL60/MX2 cells exposed to CXL017 were resensitized to standard therapies (10- to 100-fold). Western blotting analyses revealed that CXL017 exposure significantly down-regulated Mcl-1 and Bax and up-regulated Noxa, Bim, Bcl-X(L), SERCA2, and SERCA3 proteins, along with a reduction in endoplasmic reticulum (ER) calcium content. Given the well-established functions of Bcl-2 family proteins and ER calcium in drug resistance, our results suggest that the down-regulation of Mcl-1 and the up-regulation of Noxa and Bim along with the decrease in ER calcium content are likely responsible for CXL017-induced resensitization of MDR cancer cells. These data also demonstrate the unique potential of CXL017 to overcome MDR in cancer treatment.
多药耐药性(MDR)是癌症治疗中的一个主要障碍,迫切需要新的治疗方法。我们最近开发了2-氨基-6-(3,5-二甲氧基苯基)-4-(2-乙氧基-2-氧代乙基)-4H-色烯-3-羧酸乙酯(CXL017),它源自Bcl-2和SERCA蛋白的双重抑制剂sHA 14-1,在体外对多药耐药癌细胞系具有选择性细胞毒性。在本研究中,我们提供了其治疗多药耐药癌症的治疗潜力的新证据,并对其优先靶向耐药癌症提供了机制性见解。CXL017在体内选择性抑制了源自多药耐药癌细胞系HL60/MX2的肿瘤生长。此外,即使长期暴露于CXL017,HL60/MX2也未能对CXL017产生稳定耐药性,而它对阿糖胞苷(Ara-C)获得了>2000倍的耐药性,阿糖胞苷是治疗急性髓系白血病(AML)的主要一线化疗药物。值得注意的是,暴露于CXL017的HL60/MX2细胞非但获得进一步的交叉耐药性,反而对标准疗法重新敏感(10至100倍)。蛋白质免疫印迹分析显示,暴露于CXL017会显著下调Mcl-1和Bax,并上调Noxa、Bim、Bcl-X(L)、SERCA2和SERCA3蛋白,同时内质网(ER)钙含量降低。鉴于Bcl-2家族蛋白和内质网钙在耐药性方面已明确的功能,我们的结果表明,Mcl-1的下调以及Noxa和Bim的上调以及内质网钙含量的降低可能是CXL017诱导多药耐药癌细胞重新敏感的原因。这些数据也证明了CXL017在癌症治疗中克服多药耐药性的独特潜力。