The Program in Physical Biology, Eunice Kennedy Shriver National Institute of Child Health and Human Development, National Institutes of Health , Bethesda, Maryland 20892, United States.
Biochemistry. 2014 Jan 14;53(1):235-46. doi: 10.1021/bi401089y. Epub 2013 Dec 20.
Type II restriction endonucleases require metal ions to specifically cleave DNA at canonical sites. Despite the wealth of structural and biochemical information, the number of Mg(2+) ions used for cleavage by EcoRV, in particular, at physiological divalent ion concentrations has not been established. In this work, we employ a single-turnover technique that uses osmotic stress to probe reaction kinetics between an initial specific EcoRV-DNA complex formed in the absence of Mg(2+) and the final cleavage step. With osmotic stress, complex dissociation before cleavage is minimized and the reaction rates are slowed to a convenient time scale of minutes to hours. We find that cleavage occurs by a two-step mechanism that can be characterized by two rate constants. The dependence of these rate constants on Mg(2+) concentration and osmotic pressure gives the number of Mg(2+) ions and water molecules coupled to each kinetic step of the EcoRV cleavage reaction. Each kinetic step is coupled to the binding 1.5-2.5 Mg(2+) ions, the uptake of ∼30 water molecules, and the cleavage of a DNA single strand. We suggest that each kinetic step reflects an independent, rate-limiting conformational change of each monomer of the dimeric enzyme that allows Mg(2+) ion binding. This modified single-turnover protocol has general applicability for metalloenzymes.
II 型限制内切酶需要金属离子才能在特定的规范位点切割 DNA。尽管有丰富的结构和生化信息,但 EcoRV 在生理二价离子浓度下切割所需的 Mg(2+)离子数量尚未确定。在这项工作中,我们采用了一种单轮技术,该技术利用渗透压来探测在没有 Mg(2+)的情况下形成的初始特定 EcoRV-DNA 复合物与最终切割步骤之间的反应动力学。在渗透压的作用下,在切割之前复合物的解离最小化,反应速率被减慢到方便的分钟到小时的时间尺度。我们发现切割是通过两步机制发生的,可以用两个速率常数来描述。这些速率常数对 Mg(2+)浓度和渗透压的依赖性给出了与 EcoRV 切割反应的每个动力学步骤耦合的 Mg(2+)离子和水分子的数量。每个动力学步骤与结合 1.5-2.5 个 Mg(2+)离子、摄取约 30 个水分子和切割单链 DNA 相关。我们认为,每个动力学步骤反映了二聚酶每个单体的独立、限速构象变化,从而允许 Mg(2+)离子结合。这种改良的单轮技术具有普遍的适用性,适用于金属酶。