Physical and numerical aspects of sodium ion solvation free energies via the cluster-continuum model

Otlyotov, A.; Itkis, D.M.; Yashina, L.V.; Cavallo, L.; Minenkov, Y.

Авторы: Otlyotov Arseniy, Itkis Daniil M., Yashina Lada V., Cavallo Luigi, Minenkov Yury
Журнал: Physical Chemistry Chemical Physics
Год издания: 2022
Издательство: Royal Society of Chemistry
Местоположение издательства: United Kingdom
DOI: 10.1039/d2cp03583a
Аннотация: Sodium cation solvation Gibbs free energies (∆Gsolv(Na+)) have been obtained in water, dimethylformamide, dimethyl sulfoxide, ethanol, acetone, acetonitrile and methanol through the “monomer cycle” cluster-continuum approach where the solvent reference state is described by infinitely separated molecules. The following steps have been found to be vital for arrival at reliable ∆Gsolv(Na+) values: a) meticulous conformational search involving dispersion corrected density functional theory (DFT-D) and continuum solvation model (CSM); b) gas-phase DFT-D geometry optimization followed by single-point (SP) domain-based local pair natural orbital coupled cluster including single, double, and partly triple excitations (DLPNO-CCSD(T)) calculations in conjunction with the complete basis set extrapolation; c) advanced statistical thermodynamic treatment of the low harmonic frequencies (<100 cm-1) to obtain robust gas-phase Gibbs free energy correction; d) gas-phase and dielectric continuum SP with non-electrostatic contributions included in CSM; e) evaluation of relative thermodynamic stability of the Na+(S)n clusters to identify the number of explicit solvent molecules n to be considered. Our refined computational protocol is promising as it reproduces accurate experimental ∆Gsolv(Na+) values for all considered solvents but acetone and acetonitrile for which predicted ∆Gsolv(Na+) are ca. 3 kcal mol-1 too positive and too negative, respectively.
Добавил в систему: Яшина Лада Валерьевна

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