Approaching actinide(+III) hydration from first principles.
Approaching actinide(+III) hydration from first principles.
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DOI：
10.1039/b614092k
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发表时间：
2007-01
期刊：
影响因子：
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通讯作者：
J. Wiebke;A. Moritz;X. Cao;M. Dolg
中科院分区：
文献类型：
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作者：
J. Wiebke;A. Moritz;X. Cao;M. Dolg
一个系统的计算方法，一个密度泛函理论水平上的An（III）水合，使用准相对论5 f-在核心赝势和价只基组的An（III）子系统，提出。计算了[An（III）（OH（2））（h）]（3+）的分子结构、结合能、水合能和水合吉布斯自由能（h = 7，8，9）和[An（III）（OH（2））（h-1）* OH（2）]（3+）（h = 8，9），在COSMO隐式溶剂化模型内使用大的（7s 6p 5d 2f 1g）/[6s 5 p4 d2 f1 g] An（III）和cc-pVQZ O和H基组。一个（III）优选的初级水合数被发现是8为所有的An（III）在梯度校正的密度泛函理论水平。二阶Møller-Plesset微扰理论预测Ac（III）-Md（III）和No（III）-Lr（III）的优先初级水合数分别为9和8。
A systematic computational approach to An(III) hydration on a density-functional level of theory, using quasi-relativistic 5f-in-core pseudopotentials and valence-only basis sets for the An(III) subsystems, is presented. Molecular structures, binding energies, hydration energies, and Gibbs free energies of hydration have been calculated for [An(III)(OH(2))(h)](3+) (h = 7, 8, 9) and [An(III)(OH(2))(h-1) * OH(2)](3+) (h = 8, 9), using large (7s6p5d2f1g)/[6s5p4d2f1g] An(III) and cc-pVQZ O and H basis sets within the COSMO implicit solvation model. An(III) preferred primary hydration numbers are found to be 8 for all An(III) at the gradient-corrected density-functional level of theory. Second-order Møller-Plesset perturbation theory predicts preferred primary hydration numbers of 9 and 8 for Ac(III)-Md(III) and No(III)-Lr(III), respectively.