Xu Wenyan, Ouellette Adam, Ghosh Souradyuti, O'Neill Tylor C, Greenberg Marc M, Zhao Linlin
Department of Chemistry, Johns Hopkins University , Baltimore, Maryland 21218, United States.
Biochemistry. 2015 Dec 22;54(50):7409-22. doi: 10.1021/acs.biochem.5b01027. Epub 2015 Dec 14.
5'-(2-Phosphoryl-1,4-dioxobutane) (DOB) is an oxidized abasic site that is produced by several antitumor agents and γ-radiolysis. DOB reacts reversibly with a dA opposite the 3'-adjacent nucleotide to form DNA interstrand cross-links (ICLs), genotoxic DNA lesions that can block DNA replication and transcription. Translesion synthesis (TLS) is an important step in several ICL repair pathways to bypass unhooked intermediates generated by endonucleolytic incision. The instability of DOB-ICLs has made it difficult to learn about their TLS-mediated repair capability and mutagenic potential. We recently developed a method for chemically synthesizing oligonucleotides containing a modified DOB-ICL analogue. Herein, we examined the capabilities of several highly relevant eukaryotic TLS DNA polymerases (pols), including human pol η, pol κ, pol ι, pol ν, REV1, and yeast pol ζ, to bypass this DOB-ICL analogue. The prelesion, translesion, and postlesion replication efficiency and fidelity were examined. Pol η showed moderate bypass activity when encountering the DOB-ICL, giving major products one or two nucleotides beyond the cross-linked template nucleotide. In contrast, DNA synthesis by the other pols was stalled at the position before the cross-linked nucleotide. Steady-state kinetic data and liquid chromatography-mass spectrometry sequencing of primer extension products by pol η unambiguously revealed that pol η-mediated bypass is highly error-prone. Together, our study provides the first set of in vitro evidence that the DOB-ICL is a replication-blocking and highly miscoding lesion. Compared to several other TLS pols examined, pol η is likely to contribute to the TLS-mediated repair of the DOB-ICL in vivo.
5'-(2-磷酸基-1,4-二氧代丁烷)(DOB)是一种氧化脱碱基位点,由多种抗肿瘤药物和γ辐射分解产生。DOB与3'-相邻核苷酸对面的dA可逆反应,形成DNA链间交联(ICL),这是一种可阻断DNA复制和转录的基因毒性DNA损伤。跨损伤合成(TLS)是几种ICL修复途径中的重要步骤,用于绕过由核酸内切酶切割产生的未解开中间体。DOB-ICL的不稳定性使得了解其TLS介导的修复能力和诱变潜力变得困难。我们最近开发了一种化学合成含有修饰的DOB-ICL类似物的寡核苷酸的方法。在此,我们研究了几种高度相关的真核TLS DNA聚合酶(pols)的能力,包括人pol η、pol κ、pol ι、pol ν、REV1和酵母pol ζ,以绕过这种DOB-ICL类似物。我们检测了损伤前、损伤中和损伤后复制的效率和保真度。当遇到DOB-ICL时,pol η表现出适度的绕过活性,产生的主要产物比交联模板核苷酸多一或两个核苷酸。相比之下,其他pols的DNA合成在交联核苷酸之前的位置停滞。pol η的稳态动力学数据和引物延伸产物的液相色谱-质谱测序明确显示,pol η介导的绕过极易出错。总之,我们的研究提供了第一组体外证据,表明DOB-ICL是一种复制阻断且高度错编码的损伤。与其他几种检测的TLS pols相比,pol η可能在体内对DOB-ICL的TLS介导修复起作用。