Wang Pengcheng, Amato Nicholas J, Wang Yinsheng
Environmental Toxicology Graduate Program and ‡Department of Chemistry, University of California , Riverside, California 92521-0403, United States.
Biochemistry. 2017 Jul 25;56(29):3725-3732. doi: 10.1021/acs.biochem.7b00146. Epub 2017 Jul 10.
Reactive oxygen species (ROS), resulting from endogenous metabolism and/or environmental exposure, can induce damage to the 2-deoxyribose moiety in DNA. Specifically, a hydrogen atom from each of the five carbon atoms in 2-deoxyribose can be abstracted by hydroxyl radical, and improper chemical repair of the ensuing radicals formed at the C1', C3', and C4' positions can lead to the stereochemical inversion at these sites to yield epimeric 2-deoxyribose lesions. Although ROS-induced single-nucleobase lesions have been well studied, the biological consequences of the C3'-epimeric lesions of 2'-deoxynucleosides, i.e., 2'-deoxyxylonucleosides (dxN), have not been comprehensively investigated. Herein, we assessed the impact of dxN lesions on the efficiency and fidelity of DNA replication in Escherichia coli cells by conducting a competitive replication and adduct bypass assay with single-stranded M13 phage containing a site-specifically incorporated dxN. Our results revealed that, of the four dxN lesions, only dxG constituted a strong impediment to DNA replication, and intriguingly, dxT and dxC conferred replication bypass efficiencies higher than those of the unmodified counterparts. In addition, the three SOS-induced DNA polymerases (Pol II, Pol IV, and Pol V) did not play any appreciable role in bypassing these lesions. Among the four dxNs, only dxA directed a moderate frequency of dCMP misincorporation. These results provided important insights into the impact of the C3'-epimeric lesions on DNA replication in E. coli cells.
活性氧(ROS)由内源性代谢和/或环境暴露产生,可诱导DNA中2-脱氧核糖部分受损。具体而言,2-脱氧核糖中五个碳原子上的每个氢原子都可被羟基自由基夺取,而对在C1'、C3'和C4'位置形成的后续自由基进行不当的化学修复会导致这些位点的立体化学反转,从而产生差向异构的2-脱氧核糖损伤。尽管ROS诱导的单核苷酸碱基损伤已得到充分研究,但2'-脱氧核苷的C3'-差向异构损伤,即2'-脱氧木糖核苷(dxN)的生物学后果尚未得到全面研究。在此,我们通过对含有位点特异性掺入dxN的单链M13噬菌体进行竞争性复制和加合物绕过试验,评估了dxN损伤对大肠杆菌细胞中DNA复制效率和保真度的影响。我们的结果表明,在四种dxN损伤中,只有dxG对DNA复制构成严重阻碍,有趣的是,dxT和dxC赋予的复制绕过效率高于未修饰的对应物。此外,三种SOS诱导的DNA聚合酶(Pol II、Pol IV和Pol V)在绕过这些损伤方面没有发挥任何明显作用。在四种dxN中,只有dxA导致中等频率的dCMP错掺入。这些结果为C3'-差向异构损伤对大肠杆菌细胞中DNA复制的影响提供了重要见解。