ABEEM/MM OH- Models for OH-(H2O)n Clusters and Aqueous OH-: Structures, Charge Distributions, and Binding Energies

Hua Shi; Li-Dong Gong; Cui Liu; Li-Nan Lu; Zhong-Zhi Yang

doi:10.1021/acs.jpca.0c03941

ABEEM/MM OH^- Models for OH^-(H₂O)_n Clusters and Aqueous OH^-: Structures, Charge Distributions, and Binding Energies

J Phys Chem A. 2020 Jul 16;124(28):5963-5978. doi: 10.1021/acs.jpca.0c03941. Epub 2020 Jul 2.

Authors

Hua Shi^{1

2}, Li-Dong Gong¹, Cui Liu¹, Li-Nan Lu¹, Zhong-Zhi Yang¹

Affiliations

¹ School of Chemistry and Chemical Engineering, Liaoning Normal University, Dalian, 116029, People's Republic of China.
² School of Marine Science and Environment, Dalian Ocean University, Dalian 116023, People's Republic of China.

PMID: 32520555
DOI: 10.1021/acs.jpca.0c03941

Abstract

Based on the atom-bond electronegativity equalization method fused into molecular mechanics (ABEEM/MM), two fluctuating charge models of OH^--water system were proposed. The difference between these two models is whether there is charge transfer between OH^- and its first-shell water molecules. The structures, charge distributions, charge transfer, and binding energies of the OH^-(H₂O)_n (n = 1-8, 10, 15, 23) clusters were studied by these two ABEEM/MM models, the OPLS/AA force field, the OPLS-SMOOTH/AA force field, and the QM methods. The results demonstrate that two ABEEM/MM models can search out all stable structures just as the QM methods, and the structures and charge distributions agree well with those from the QM calculations. The structures, the charge transfer, and the strength of hydrogen bonds in the first hydration shell are closely related to the coordination number of OH^-. Molecular dynamics simulations on the aqueous OH^- solution are performed at 298 and 278 K using ABEEM/MM-I model. The MD results show that the populations of three-, four-, and five-coordinated OH^- are 29.6%, 67.1%, and 3.4% at 298 K, respectively, and those of two-, three-, four-, and five-coordinated OH^- are 10.8%, 44.9%, 39.2%, and 4.9% at 278 K, respectively; the average hydrogen bond lengths and the hydrogen bond angle in the first shell increase with the temperature decreasing.