A highly reactive mononuclear Zn(II) complex for phosphodiester cleavage
A highly reactive mononuclear Zn(II) complex for phosphodiester cleavage
复制标题
DOI：
10.1021/ja054003t
复制
发表时间：
2005-10-05
影响因子：
15
通讯作者：
Williams, NH
中科院分区：
文献类型：
--
作者：
Feng, GQ;Mareque-Rivas, JC;Williams, NH
通过向配体引入三个氢键供体，用于催化磷酸二酯裂解的四齿、三足配体的Zn（II）络合物的活性增强750倍。抑制研究表明，Zn−水络合物是动力学活性形式，它与过渡态结合的形式解离常数为3 × 108 M-1。这些配体修饰对过渡态亲和力的影响与金属离子本身提供的速率加速相当。总的来说，这个单核配合物比迄今报道的最具反应性的双核Zn（II）配合物更活跃。
The activity of a Zn(II) complex of a tetradentate, tripodal ligand for catalyzing phosphodiester cleavage is enhanced 750-fold by introducing three hydrogen bond donors to the ligand. Inhibition studies show that the Zn−aqua complex is the kinetically active form and that it binds the transition state with a formal dissociation constant of 3 × 108M-1. The effect of these ligand modifications on the transition-state affinity is comparable to the rate acceleration provided by the metal ion itself. Overall, this mononuclear complex is more active than the most reactive dinuclear Zn(II) complexes reported to date.