Preferential solvation of Ca2+ in aqueous ammonia solution: Classical and combined ab initio quantum mechanical/molecular mechanical molecular dynamics simulations

Literature Information

Publication Date 2002-01-08
DOI 10.1039/B107786D
Impact Factor 3.676
Authors

Anan Tongraar, Kritsana Sagarik, Bernd Michael Rode


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Abstract

Classical and combined quantum mechanical/molecular mechanical (QM/MM) molecular dynamics simulations have been performed to investigate the solvation structure of Ca2+ in 18.4% aqueous ammonia solution. The classical molecular dynamics simulation has been carried out based on pairwise additive potentials. For the QM/MM scheme, the first solvation sphere of Ca2+ is treated by Born–Oppenheimer ab initio quantum mechanics using LANL2DZ basis sets, while the rest of the system is described based on classical pairwise additivity. The results indicate the importance of the QM treatment in obtaining a reliable geometrical arrangement as well as the correct coordination number of the solvated ion. Within the first solvation sphere of Ca2+, the QM/MM simulation reveals a polyhedral structure with an average coordination number of 7.2, consisting of 5.2 water and 2 ammonia molecules, compared to the corresponding value of 9.7 composed of 6.7 water and 3 ammonia molecules obtained by classical pair potential simulation. The preference for ligands is discussed on the basis of detailed simulation results.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
Articles per Year: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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