Department of Chemistry and Biochemistry, University of Colorado, UCB 215, Boulder, Colorado 80309, USA.
Biochemistry. 2011 Aug 23;50(33):7243-50. doi: 10.1021/bi2006916. Epub 2011 Jul 26.
We utilized a series of pyrimidine analogues modified at O(2), N-3, and N(4)/O(4) to determine if two B family DNA polymerases, human DNA polymerase α and herpes simplex virus I DNA polymerase, choose whether to polymerize pyrimidine dNTPs using the same mechanisms they use for purine dNTPs. Removing O(2) of a pyrimidine dNTP vastly decreased the level of incorporation by these enzymes and also compromised fidelity in the case of C analogues, while removing O(2) from the templating base had more modest effects. Removing the Watson-Crick hydrogen bonding groups of N-3 and N(4)/O(4) greatly impaired polymerization, both of the resulting dNTP analogues and of natural dNTPs opposite these pyrimidine analogues when present in the template strand. Thus, the Watson-Crick hydrogen bonding groups of a pyrimidine clearly play an important role in enhancing correct dNTP polymerization but are not essential for preventing misincorporation. These studies also indicate that DNA polymerases recognize bases extremely asymmetrically, both in terms of whether they are a purine or pyrimidine and whether they are in the template or are the incoming dNTP. The mechanistic implications of these results with regard to how polymerases discriminate between right and wrong dNTPs are discussed.
我们利用一系列嘧啶类似物修饰 O(2)、N-3 和 N(4)/O(4),以确定两种 B 族 DNA 聚合酶,人 DNA 聚合酶 α 和单纯疱疹病毒 I DNA 聚合酶,是否使用与嘌呤 dNTP 相同的机制来选择聚合嘧啶 dNTP。从嘧啶 dNTP 中去除 O(2)极大地降低了这些酶的掺入水平,并且在 C 类似物的情况下也损害了保真度,而从模板碱基中去除 O(2)的影响则更为温和。去除 N-3 和 N(4)/O(4)的 Watson-Crick 氢键供体基团极大地阻碍了聚合,无论是对产生的 dNTP 类似物还是对模板链中存在的这些嘧啶类似物的天然 dNTP 的聚合都是如此。因此,嘧啶的 Watson-Crick 氢键供体基团显然在增强正确的 dNTP 聚合中起着重要作用,但对于防止错误掺入并非必不可少。这些研究还表明,DNA 聚合酶在识别碱基方面非常不对称,无论是嘌呤还是嘧啶,无论是模板还是进入的 dNTP。这些结果对聚合酶如何区分正确和错误的 dNTP 的机制意义进行了讨论。