Chemistry Department, Georgetown University, Washington, DC, 20057, USA; Medicinal Chemistry Shared Resource (MCSR), Georgetown University Medical Center, Washington, DC, USA.
Lombardi Comprehensive Cancer Center, Georgetown University Medical Center, Washington, DC, USA.
Eur J Med Chem. 2023 May 5;251:115244. doi: 10.1016/j.ejmech.2023.115244. Epub 2023 Mar 2.
Ewing Sarcoma (ES) is a cancer of bone and soft tissues affecting mostly children and young adults. Aggressive progression and poor prognosis of this malignancy call for novel and targeted treatments. CD99 is a transmembrane protein that is abundantly expressed on ES cells and is a diagnostic marker for the disease. ES cells are selectively sensitive to CD99 inhibition compared to most normal cells and other tumors. Therefore, CD99 is a good molecular target for ES treatment. Clofarabine and cladribine are two FDA approved drugs that are administered for their inhibitory acts on DNA synthesis to treat relapsed or refractory acute lymphoblastic and myeloid leukemia. They have also been shown to directly bind to CD99 and inhibit ES growth through a distinct mechanism. In the current study, we designed, synthesized and tested new ES specific derivatives of both drugs that would continue to target CD99 but with expected reduction in cellular membrane permeability and rendered unsuitable for inhibiting DNA synthesis. By using commercially available clofarabine and cladribine purine nucleoside analogs, we modified the primary alcohol moiety at the deoxyribose C-5' terminal site to suppress phosphorylation and thus inhibition of subsequent DNA synthesis pathways. In addition, we incorporated a variety of polar groups in the ribose and purine rings to reduce membrane permeability and investigated the effects of configurational changes in the sugar moiety. Among 26 new derivatives, we identified two compounds, BK50164 and BK60106, that cause cell death specifically in ES primarily due to inhibition of CD99 but not via inhibition of DNA synthesis. These findings provide a road map for the future development selective CD99 inhibitors for targeted treatment of ES.
尤因肉瘤 (ES) 是一种影响儿童和年轻人的骨和软组织癌症。这种恶性肿瘤的侵袭性进展和不良预后需要新的靶向治疗。CD99 是一种跨膜蛋白,在 ES 细胞中大量表达,是该疾病的诊断标志物。与大多数正常细胞和其他肿瘤相比,ES 细胞对 CD99 抑制具有选择性敏感性。因此,CD99 是 ES 治疗的一个很好的分子靶点。克拉屈滨和 cladribine 是两种获得 FDA 批准的药物,它们通过抑制 DNA 合成来治疗复发或难治性急性淋巴细胞白血病和髓性白血病。它们还被证明可以直接与 CD99 结合,并通过一种独特的机制抑制 ES 生长。在本研究中,我们设计、合成并测试了这两种药物的新的 ES 特异性衍生物,这些衍生物将继续针对 CD99,但预计细胞膜通透性降低,不适合抑制 DNA 合成。通过使用市售的克拉屈滨和 cladribine 嘌呤核苷类似物,我们修饰了脱氧核糖 C-5'末端的伯醇部分,以抑制磷酸化,从而抑制后续的 DNA 合成途径。此外,我们在核糖和嘌呤环中引入了各种极性基团,以降低细胞膜通透性,并研究了糖部分构象变化的影响。在 26 种新衍生物中,我们鉴定出两种化合物 BK50164 和 BK60106,它们主要通过抑制 CD99 而不是通过抑制 DNA 合成导致 ES 细胞死亡。这些发现为未来开发针对 ES 的选择性 CD99 抑制剂提供了路线图。