Utility of chemical computations in predicting solution free energies of metal ions

Chaudhari, Mangesh I.; Pratt, Lawrence R.; Rempe, Susan B.

doi:10.1080/08927022.2017.1342127

Title: Utility of chemical computations in predicting solution free energies of metal ions

Journal Article · Sun Jun 25 00:00:00 EDT 2017 · Molecular Simulation

DOI:https://doi.org/10.1080/08927022.2017.1342127· OSTI ID:1485840

Chaudhari, Mangesh I. ^[1]; Pratt, Lawrence R. ^[2]; Rempe, Susan B. ^[1]

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Tulane Univ., New Orleans, LA (United States)

In this paper, we study quasi-chemical theory (QCT) for the free energies of divalent alkaline earth ions (Ba2+, Sr2+, Ca2+, Mg2+) in water, emphasizing that: (a) interactions between metal ions and proximal water molecules are as strong as traditional chemical effects; (b) QCT builds directly from accessible electronic structure calculations but rests on fully elaborated molecular statistical thermodynamics; (c) QCT offers choices of convenience in identifying coordination numbers for analysis. We investigate utilisation of direct QCT with inner-shell conditioning n_λ=$$\overline{n}$$, alternative to the traditional n_λ=0 conditioning motivated by a generalised van der Waals view. The alternative n_λ=$$\overline{n}$$ works well: deleterious non-Gaussian effects of van der Waals repulsive interactions are not serious, and the alternative conditioning improves the convenience of QCT calculations. Additionally, comparison between ab initio and force field molecular dynamics (AIMD and FFMD) with standard models suggests that FFMD likely exaggerates the anharmonicity in the thermal motion of inner-shell ion-water clusters. Together with the general encouraging support for the harmonic approximations implied by the n_λ=$$\overline{n}$$ conditioning, that observation helps explain the remarkable success of the cluster-based QCT solution free energies, which do not require assessment of all inner-shell occupancies by simulation.

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Research Organization:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: AC04-94AL85000; AC02-05CH11231; AC52-06NA25396

OSTI ID:: 1485840

Report Number(s):: SAND-2018-11510J; 669384

Journal Information:: Molecular Simulation, Vol. 44, Issue 2; ISSN 0892-7022

Publisher:: Taylor & FrancisCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 14 works

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