Instituto Superior de Tecnologías y Ciencias Aplicadas, Universidad de La Habana, Avenida Salvador Allende 1110, La Habana CP 10600, Cuba.
Laboratory of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg 1, Zurich CH-8093, Switzerland.
J Chem Inf Model. 2020 Apr 27;60(4):2115-2125. doi: 10.1021/acs.jcim.9b01064. Epub 2020 Mar 16.
The aim of this work is to describe the molecular inclusion of chlordecone with α-, β-, and γ-cyclodextrin in aqueous solution using quantum mechanics. The guest-host complexes of chlordecone and cyclodextrins are modeled in aqueous solution using the multiple minima hypersurface methodology with a PM6-D3H4X semiempirical Hamiltonian, and the lowest energy minima obtained are reoptimized using the M06-2X density functional and the intermolecular interactions described using quantum theory of atoms in molecules (QTAIM). The studied complexes are classified according to the degree of inclusion, namely, total occlusion, partial occlusion, and external interaction. More stable complexes are obtained when γ-CD is used as the host molecule. The interactions characterized through QTAIM analysis are all of electrostatic nature, predominantly of dispersive type. In this work, a method based on the counterpoise correction is also discussed to mitigate the basis set superposition error in density functional theory calculations when using an implicit solvation model.
这项工作的目的是使用量子力学描述六氯环戊二烯与 α-、β-和 γ-环糊精在水溶液中的分子包容作用。使用 PM6-D3H4X 半经验哈密顿量的多最小势能面方法，在水溶液中对六氯环戊二烯和环糊精的主体-客体配合物进行建模，并用 M06-2X 密度泛函重新优化获得的最低能量最小位能，并使用分子中的原子量子理论 (QTAIM) 描述分子间相互作用。根据包容程度对研究的配合物进行分类，即完全包容、部分包容和外部相互作用。当 γ-CD 用作主体分子时，会得到更稳定的配合物。通过 QTAIM 分析表征的相互作用都是静电性质的，主要是分散类型的。在这项工作中，还讨论了一种基于对位补偿的方法，以减轻在使用隐式溶剂化模型时密度泛函理论计算中的基组叠加误差。
