Hydration Control Through Intramolecular Degrees of Freedom: Molecular Dynamics of [Cu(II)(Imidazole)4],The Journal of Physical Chemistry B

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Hydration Control Through Intramolecular Degrees of Freedom: Molecular Dynamics of [Cu(II)(Imidazole)4]
The Journal of Physical Chemistry B ( IF 2.8 ) Pub Date : 2017-09-18 00:00:00 , DOI: 10.1021/acs.jpcb.7b05949
Akshaya K. Das ₁ , Markus Meuwly ₁

Affiliation

Structural characterization of the copper-coordination shell is important in catalysis and biology. Cu-containing domains are prevalent in biological systems and play important roles in oxidation and electron transport process. Here, the solution structure, solvent organization, and dynamics around aqueous [Cu(II)(Imidazole)₄] were characterized using atomistic simulations. Asymmetric axial water coordination around the metal atom was found which agrees with results from Minuit X-ray absorption near-edge structure (MXAN) experiments. The simulations reveal that exchange of the axial water occurs on the 25 to 50 ps time scale and is facilitated by and coupled to the flexibility of the copper-out of plane motion relative to the nitrogen atoms. Both concerted and stepwise water exchange of the two axially coordinated water molecules with first-shell water molecules are observed. The results suggest that axial access of a copper center can be fine-tuned by the degree of flexibility of its first coordination sphere.

中文翻译：

通过分子内自由度进行水合控制：[Cu（II）（咪唑）₄ ]的分子动力学

铜配位壳的结构表征在催化和生物学中很重要。含铜域在生物系统中普遍存在，并在氧化和电子传输过程中起重要作用。在这里，溶液的结构，溶剂的组织和周围[Cu（II）（Imidazole）₄水溶液的动力学用原子模拟来表征。发现金属原子周围的不对称轴向水配位与Minuit X射线吸收近边缘结构（MXAN）实验的结果一致。模拟表明，轴向水的交换发生在25到50 ps的时间尺度上，并且相对于氮原子而言，平面运动的铜向外的柔韧性促进并与之耦合。观察到两个轴向配位的水分子与第一壳水分子的协调和逐步的水交换。结果表明，铜中心的轴向通道可以通过其第一个配位球的柔韧性进行微调。

更新日期：2017-09-19

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