Hydration structure and water exchange reaction of Nickel(II) ion: Classical and QM/MM Simulations

被引:58
作者
Inada, Y [1 ]
Mohammed, AM
Loeffler, HH
Rode, BM
机构
[1] Univ Innsbruck, Dept Theoret Chem, Inst Gen Inorgan & Theoret Chem, A-6020 Innsbruck, Austria
[2] Nagoya Univ, Res Ctr Mat Sci, Nagoya, Aichi 4648602, Japan
[3] Univ Addis Ababa, Dept Chem, Addis Ababa, Ethiopia
关键词
D O I
10.1021/jp0155314
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Classical molecular dynamics (MD), classical Monte Carlo (MC), and combined quantum mechanical/molecular mechanical (QM/MM) MD simulations were carried out to investigate the hydration structure of the Ni(II) ion in water using a newly constructed 2-body potential and a function correcting for 3-body effects. A 6-coordinate hydration structure with a maximum probability of the Ni-O distance at 2.25, 2.21, and 2.14 Angstrom was observed by the classical MD, classical MC, and QM/MM-MD simulation with 3-body corrections, respectively, while an 8-coordinate structure was observed by the classical MD and MC simulations using only 2-body pair potentials. The average structure parameters obtained by the Hertree-Fock level QM/MM-MD simulation are in agreement with the experimental values. The validity of the 3-body correction function is discussed on the basis of the results for the classical and QM/MM simulations. During the classical MD simulation, a water exchange reaction was observed for the 6-coordinate Ni(II) ion. The water exchange reaction proceeded via a 5-coordinate intermediate with the lifetime of ca. 2.5 ps. The observed dissociative mechanism of the water exchange reaction is in accordance with experimental evidence.
引用
收藏
页码:6783 / 6791
页数:9
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