Li Xin, Rinkevicius Zilvinas, Tu Yaoquan, Tian He, Agren Hans
Department of Theoretical Chemistry, School of Biotechnology, Royal Institute of Technology, S-106 91 Stockholm, Sweden.
J Phys Chem B. 2008 Sep 11;112(36):11347-52. doi: 10.1021/jp802238f. Epub 2008 Aug 14.
We present a combined molecular dynamics simulation and density functional theory investigation of the nuclear magnetic shielding constant of the (113)Cd(II) ion solvated in aqueous solution. Molecular dynamics simulations are carried out for the cadmium-water system in order to produce instantaneous geometries for subsequent determination of the nuclear magnetic shielding constant at the density functional theory level. The nuclear magnetic shielding constant is computed using a perturbation theory formalism, which includes nonrelativistic and leading order relativistic contributions to the nuclear magnetic shielding tensor. Although the NMR shielding constant varies significantly with respect to simulation time, the value averaged over increasing number of snapshots remains almost constant. The paramagnetic nonrelativistic contribution is found to be most sensitive to dynamical changes in the system and is mainly responsible for the thermal and solvent effects in solution. The relativistic correction features very little sensitivity to the chemical environment, and can be disregarded in theoretical calculations when a Cd complex is used as reference compound in (113)Cd NMR experiments, due to the mutual cancelation between individual relativistic corrections.
我们展示了一项结合分子动力学模拟和密度泛函理论的研究,该研究针对水溶液中溶剂化的(113)Cd(II)离子的核磁共振屏蔽常数。对镉 - 水体系进行分子动力学模拟,以生成瞬时几何结构,用于随后在密度泛函理论层面测定核磁共振屏蔽常数。使用微扰理论形式计算核磁共振屏蔽常数,其中包括对核磁共振屏蔽张量的非相对论和主导阶相对论贡献。尽管核磁共振屏蔽常数随模拟时间有显著变化,但随着快照数量增加而平均的值几乎保持不变。发现顺磁非相对论贡献对体系中的动态变化最为敏感,并且主要负责溶液中的热效应和溶剂效应。相对论校正对化学环境的敏感性非常小,并且在(113)Cd核磁共振实验中当使用镉配合物作为参考化合物时,由于各个相对论校正之间的相互抵消,在理论计算中可以忽略不计。