From the Genome Integrity and Structural Biology Laboratory, NIEHS, National Institutes of Health, Research Triangle Park, North Carolina 27709.
From the Genome Integrity and Structural Biology Laboratory, NIEHS, National Institutes of Health, Research Triangle Park, North Carolina 27709
J Biol Chem. 2019 May 3;294(18):7194-7201. doi: 10.1074/jbc.RA118.006809. Epub 2019 Mar 18.
DNA methylation is an epigenetic mark that regulates gene expression in mammals. One method of methylation removal is through ten-eleven translocation-catalyzed oxidation and the base excision repair pathway. The iterative oxidation of 5-methylcytosine catalyzed by ten-eleven translocation enzymes produces three oxidized forms of cytosine: 5-hydroxmethylcytosine, 5-formylcytosine, and 5-carboxycytosine. The effect these modifications have on the efficiency and fidelity of the base excision repair pathway during the repair of opposing base damage, and in particular DNA polymerization, remains to be elucidated. Using kinetic assays, we show that the catalytic efficiency for the incorporation of dGTP catalyzed by human DNA polymerase β is not affected when 5-methylcytosine, 5-hydroxmethylcytosine, and 5-formylcytosine are in the DNA template. In contrast, the catalytic efficiency of dGTP insertion decreases ∼20-fold when 5-carboxycytosine is in the templating position, as compared with unmodified cytosine. However, DNA polymerase fidelity is unaltered when these modifications are in the templating position. Structural analysis reveals that the methyl, hydroxymethyl, and formyl modifications are easily accommodated within the polymerase active site. However, to accommodate the carboxyl modification, the phosphate backbone on the templating nucleotide shifts ∼2.5 Å to avoid a potential steric/repulsive clash. This altered conformation is stabilized by lysine 280, which makes a direct interaction with the carboxyl modification and the phosphate backbone of the templating strand. This work provides the molecular basis for the accommodation of epigenetic base modifications in a polymerase active site and suggests that these modifications are not mutagenically copied during base excision repair.
DNA 甲基化是一种调节哺乳动物基因表达的表观遗传标记。一种去除甲基化的方法是通过 ten-eleven 易位催化的氧化和碱基切除修复途径。ten-eleven 易位酶催化的 5-甲基胞嘧啶的反复氧化产生三种氧化形式的胞嘧啶:5-羟甲基胞嘧啶、5-甲酰基胞嘧啶和 5-羧基胞嘧啶。这些修饰物在修复相反碱基损伤时,特别是在 DNA 聚合过程中,对碱基切除修复途径的效率和保真度的影响仍有待阐明。通过动力学测定,我们表明当 5-甲基胞嘧啶、5-羟甲基胞嘧啶和 5-甲酰基胞嘧啶存在于 DNA 模板中时,人 DNA 聚合酶 β 催化的 dGTP 掺入的催化效率不受影响。相比之下,当 5-羧基胞嘧啶处于模板位置时,dGTP 插入的催化效率与未修饰的胞嘧啶相比降低了约 20 倍。然而,当这些修饰物处于模板位置时,DNA 聚合酶保真度没有改变。结构分析表明,甲基、羟甲基和甲酰基修饰很容易适应聚合酶活性位点。然而,为了适应羧基修饰,模板核苷酸的磷酸骨架会移动约 2.5 Å 以避免潜在的空间/排斥冲突。这种改变的构象由赖氨酸 280 稳定,赖氨酸 280 与羧基修饰和模板链的磷酸骨架直接相互作用。这项工作为聚合酶活性位点中表观遗传碱基修饰的适应提供了分子基础,并表明这些修饰在碱基切除修复过程中不会被诱变复制。