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A Coupled Molecular Dynamics and XANES Data Analysis Investigation of Aqueous Cadmium(II)

机译:镉(II)的分子动力学和XANES数据耦合研究

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The flexible nature of the first hydration shell of the cadmium(II) ion has been definitively assessed through an extensive study, combining X-ray absorption near-edge structure (XANES) spectroscopy and molecular dynamics (MD) simulations. The structural and dynamic properties of the cadmium(II) hydration shell have been determined from long-time MD simulations, and the influence of water—water interactions has been evaluated using the SPC/E and TIP5P water models. Comparison of the theoretical results with EXAFS data suggests that the TIP5P simulation provides a better description of the cadmium(II) hydration properties. XANES spectra have been computed starting from MD trajectories, without carrying out any minimization in the structural parameter space. The octahedral solvation of cadmium(II) in aqueous solution cannot be reconciled with the XANES results, while a flexible hydration shell is fully consistent with the experimental data, which unambiguously show the presence of a dominant percentage of heptahydrated species.
机译:通过广泛的研究,结合X射线吸收近边缘结构(XANES)光谱学和分子动力学(MD)模拟,对镉(II)离子的第一个水合壳的柔性性质进行了确定的评估。镉(II)水化壳的结构和动力学特性已通过长期的MD模拟确定,并且已使用SPC / E和TIP5P水模型评估了水与水相互作用的影响。理论结果与EXAFS数据的比较表明,TIP5P模拟提供了对镉(II)水化性质的更好描述。 XANES光谱是从MD轨迹开始计算的,没有在结构参数空间中进行任何最小化。镉(II)在水溶液中的八面体溶剂化与XANES结果不一致,而柔软的水合壳与实验数据完全一致,这清楚地表明存在主要百分比的七水合物种。

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