Huber Stefan, Huettner Johannes Philip, Hacker Kristina, Bernhardt Günther, König Jörg, Buschauer Armin
Pharmaceutical and Medicinal Chemistry II, Institute of Pharmacy, University of Regensburg, Regensburg, Germany.
Pharmacology and Toxicology, Institute of Pharmacy, University of Regensburg, Regensburg, Germany.
PLoS One. 2015 Jul 21;10(7):e0133743. doi: 10.1371/journal.pone.0133743. eCollection 2015.
The alkylating agent bendamustine is approved for the treatment of hematopoietic malignancies such as non-Hodgkin lymphoma, chronic lymphocytic leukemia and multiple myeloma. As preliminary data on recently disclosed bendamustine esters suggested increased cytotoxicity, we investigated representative derivatives in more detail. Especially basic esters, which are positively charged under physiological conditions, were in the crystal violet and the MTT assay up to approximately 100 times more effective than bendamustine, paralleled by a higher fraction of early apoptotic cancer cells and increased expression of p53. Analytical studies performed with bendamustine and representative esters revealed pronounced cellular accumulation of the derivatives compared to the parent compound. In particular, the pyrrolidinoethyl ester showed a high enrichment in tumor cells and inhibition of OCT1- and OCT3-mediated transport processes, suggesting organic cation transporters to be involved. However, this hypothesis was not supported by the differential expression of OCT1 (SLC22A1) and OCT3 (SLC22A3), comparing a panel of human cancer cells. Bendamustine esters proved to be considerably more potent cytotoxic agents than the parent compound against a broad panel of human cancer cell types, including hematologic and solid malignancies (e.g. malignant melanoma, colorectal carcinoma and lung cancer), which are resistant to bendamustine. Interestingly, spontaneously immortalized human keratinocytes, as a model of "normal" cells, were by far less sensitive than tumor cells against the most potent bendamustine esters.
烷化剂苯达莫司汀被批准用于治疗造血系统恶性肿瘤,如非霍奇金淋巴瘤、慢性淋巴细胞白血病和多发性骨髓瘤。由于最近披露的苯达莫司汀酯的初步数据表明细胞毒性增加,我们对代表性衍生物进行了更详细的研究。特别是在生理条件下带正电荷的碱性酯,在结晶紫和MTT试验中比苯达莫司汀有效约100倍,同时早期凋亡癌细胞的比例更高,p53表达增加。对苯达莫司汀和代表性酯进行的分析研究表明,与母体化合物相比,衍生物在细胞内有明显的积累。特别是吡咯烷基乙酯在肿瘤细胞中高度富集,并抑制OCT1和OCT3介导的转运过程,提示有机阳离子转运体参与其中。然而,通过比较一组人类癌细胞中OCT1(SLC22A1)和OCT3(SLC22A3)的差异表达,这一假设并未得到支持。苯达莫司汀酯被证明是比母体化合物更有效的细胞毒性剂,对包括血液系统和实体恶性肿瘤(如恶性黑色素瘤、结直肠癌和肺癌)在内的多种人类癌细胞类型均有活性,而这些细胞类型对苯达莫司汀耐药。有趣的是,作为“正常”细胞模型的自发永生化人类角质形成细胞对最有效的苯达莫司汀酯的敏感性远低于肿瘤细胞。