Roy Soma, Maiti Bappa, Banerjee Nilanjan, Kaulage Mangesh H, Muniyappa Kalappa, Chatterjee Subhrangsu, Bhattacharya Santanu
Department of Organic Chemistry, Indian Institute of Science, Bangalore 560012, India.
School of Applied & Interdisciplinary Sciences, Indian Association for the Cultivation of Science, Kolkata 700032, India.
ACS Pharmacol Transl Sci. 2023 Mar 24;6(4):546-566. doi: 10.1021/acsptsci.2c00205. eCollection 2023 Apr 14.
Xanthone is an important scaffold for various medicinally relevant compounds. However, it has received scant attention in the design of agents that are cytotoxic to cancer cells via targeting the stabilization of G-quadruplex (G4) nucleic acids. Specific G4 DNA recognition against double-stranded (ds) DNA is receiving epoch-making interest for the development of G4-mediated anticancer agents. Toward this goal, we have synthesized xanthone-based derivatives with various functionalized side-arm substituents that exhibited significant selectivity for G4 DNA as compared to dsDNA. The specific interaction has been demonstrated by performing various biophysical experiments. Based on the computational study as well as the competitive ligand binding assay, it is inferred that the potent compounds exhibit an end-stacking mode of binding with G4 DNA. Additionally, compound-induced conformational changes in the flanking nucleotides form the binding pocket for effective interaction. Selective action of the compounds on cancer cells suggests their effectiveness as potent anti-cancer agents. This study promotes the importance of structure-based screening approaches to get molecular insights for new scaffolds toward desired specific recognition of non-canonical G4 DNA structures.
呫吨酮是多种具有医学相关性的化合物的重要骨架。然而,在通过靶向稳定G-四链体(G4)核酸来设计对癌细胞具有细胞毒性的药物方面,它却很少受到关注。针对双链(ds)DNA的特异性G4 DNA识别对于G4介导的抗癌药物的开发正引起划时代的关注。为了实现这一目标,我们合成了带有各种功能化侧链取代基的呫吨酮基衍生物,与dsDNA相比,这些衍生物对G4 DNA表现出显著的选择性。通过进行各种生物物理实验证明了这种特异性相互作用。基于计算研究以及竞争性配体结合测定,推断出强效化合物与G4 DNA呈现末端堆积结合模式。此外,化合物诱导的侧翼核苷酸构象变化形成了有效相互作用的结合口袋。这些化合物对癌细胞的选择性作用表明它们作为强效抗癌药物的有效性。这项研究凸显了基于结构的筛选方法对于获得分子见解以寻找新骨架来实现对非经典G4 DNA结构的特异性识别的重要性。