Department of Therapeutic Radiology, Yale University School of Medicine, New Haven, Connecticut 06520-8034, United States.
University of Arizona Cancer Center, University of Arizona, Tucson, Arizona 85724-5044, United States.
Biochemistry. 2024 Oct 1;63(19):2414-2424. doi: 10.1021/acs.biochem.4c00263. Epub 2024 Sep 19.
DNA polymerase β (Pol β) fills single nucleotide gaps during base excision repair. Deficiencies in Pol β can lead to increased mutagenesis and genomic instability in the cell, resulting in cancer. Our laboratory has previously shown that the I260 M somatic mutation of Pol β, which was first identified in prostate cancer, has reduced nucleotide discrimination in a sequence context-dependent manner. I260 M incorporates the incorrect G opposite A in this context more readily than WT. To identify the molecular mechanism of the reduced fidelity of I260M, we studied incorporation using single turnover kinetics and the nature and rates of conformational changes using steady-state fluorescence and Förster resonance energy transfer (FRET). Our data indicate that the I260 M mutation affects the fingers region of rat Pol β by creating a "collapsed" state in both the open (in the absence of nucleotide) and closed (prior to chemistry) states. I260 M is a temperature-sensitive mutator and binds nucleotides tighter than the WT protein, resulting in reduced fidelity compared to the WT. Additionally, we have generated a kinetic model of WT and I260 M using FRET and single turnover data, which demonstrates that I260 M precatalytic conformation changes differ compared to the WT as it is missing a precatalytic noncovalent step. Taken together, these results suggest that the collapsed state of I260 M may decrease its ability for nucleotide discrimination, illustrating the importance of the "fingers closing" conformational change for polymerase fidelity and accurate DNA synthesis.
DNA 聚合酶 β(Pol β)在碱基切除修复过程中填补单核苷酸间隙。Pol β 的缺陷会导致细胞中突变和基因组不稳定性增加,从而导致癌症。我们的实验室之前曾表明,首先在前列腺癌中发现的 Pol β 的 I260M 体细胞突变以序列上下文依赖的方式降低了核苷酸的区分能力。I260M 比 WT 更容易将不正确的 G 掺入到这种情况下的 A 中。为了确定 I260M 降低保真度的分子机制,我们使用单转换动力学研究了掺入情况,并使用稳态荧光和Förster 共振能量转移(FRET)研究了构象变化的性质和速率。我们的数据表明,I260M 突变通过在开放(无核苷酸)和关闭(化学前)状态下都创建“塌陷”状态来影响大鼠 Pol β 的手指区域。I260M 是温度敏感的诱变剂,与 WT 蛋白相比结合核苷酸更紧密,导致与 WT 相比保真度降低。此外,我们使用 FRET 和单转换数据为 WT 和 I260M 生成了一个动力学模型,该模型表明,与 WT 相比,I260M 的预催化构象变化不同,因为它缺少预催化的非共价步骤。总之,这些结果表明,I260M 的塌陷状态可能会降低其核苷酸区分能力,说明了“手指闭合”构象变化对于聚合酶保真度和准确 DNA 合成的重要性。