Hybrid Cluster-Continuum Method for Single-Ion Solvation Free Energy in Acetonitrile Solvent

The Journal of Physical Chemistry A, Journal Year: 2024, Volume and Issue: 128(31), P. 6440 - 6449

Published: July 25, 2024

A new hybrid discrete-continuum approach named the cluster-continuum static approximation (CCSA) has been proposed for acetonitrile solvent. The continuum part uses conductor-like polarizable model electrostatic and a surface area-dependent term nonelectrostatic solvation. CCSA includes only one explicit solvent molecule damping function, which makes method reduce to pure solvation in case of weaker potential mean force solute-solvent interaction. performance was tested 22 anions cations, including challenge species that cannot be adequately described by comparison done with widely used density (SMD) model. For anions, reduces same as SMD model, standard deviation signed error (SD-MSE) 2.7 kcal mol

Language: Английский

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Experimental Compilation and Computation of Hydration Free Energies for Ionic Solutes

The Journal of Physical Chemistry A, Journal Year: 2023, Volume and Issue: 127(48), P. 10268 - 10281

Published: Nov. 27, 2023

Although charged solutes are common in many chemical systems, traditional solvation models perform poorly calculating energies of ions. One major obstacle is the scarcity experimental data for solvated In this study, we release an experiment-based aqueous ionic energy set, IonSolv-Aq, that contains hydration free 118 anions and 155 cations, more than 2 times larger set singly ions contained 2012 Minnesota Solvation Database commonly used benchmarking studies. We discuss sources systematic uncertainty use to examine accuracy popular implicit COSMO-RS SMD predicting water. Our results indicate most modeling errors correctable with empirical parameters. two offsets: one across all depends on functional group ionization site. After correcting these offsets, predicted using 3.1 kcal mol-1 MAE against a challenging test 1.7 (about 3% relative error) filtered set. The performance similar, those same sets 2.7 mol-1. These underscore importance compiling improve model parametrization fairly assess performance.

Language: Английский

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Extending the MST Model to Large Biomolecular Systems: Parametrization of the ddCOSMO‐MST Continuum Solvation Model

Journal of Computational Chemistry, Journal Year: 2025, Volume and Issue: 46(2)

Published: Jan. 11, 2025

ABSTRACT Continuum solvation models such as the polarizable continuum model and conductor‐like screening are widely used in quantum chemistry, but their application to large biosystems is hampered by computational cost. Here, we report parametrization of Miertus–Scrocco–Tomasi (MST) for prediction hydration free energies neutral ionic molecules based on domain decomposition formulation COSMO (ddCOSMO), which allows a drastic reduction cost several orders magnitude. We also introduce novelties MST, like new definition atom types hybridization an automatic setup cavity charged regions. The parametrized at B3LYP/6‐31+G(d) PM6 levels theory compared performance IEFPCM/MST. Then, demonstrate robustness SAMPL2, SAMPL4, C10 datasets. ddCOSMO/MST provide errors ~0.8 ~3.2 kcal/mol neutrals ions, respectively, showing remarkable balanced accurate description cations anions.

Language: Английский

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DISSOLVE: Database of ionic solutes’ solvation free energies

Fluid Phase Equilibria, Journal Year: 2023, Volume and Issue: 571, P. 113801 - 113801

Published: March 16, 2023

Language: Английский

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Hydrogenation of CO2 to CH3OH catalyzed by a ruthenium-triphos complex: Theoretical free energy profile and microkinetic modeling

Journal of Catalysis, Journal Year: 2024, Volume and Issue: 431, P. 115386 - 115386

Published: Feb. 23, 2024

Language: Английский

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Car-Parrinello molecular dynamics study of CuF, AgF, CuPF6 and AgPF6 in acetonitrile solvent and Cluster-Continuum calculation of the solvation free energy of Cu(I), Ag(I) and Li(I)

Journal of Molecular Liquids, Journal Year: 2022, Volume and Issue: 359, P. 119368 - 119368

Published: May 13, 2022

Language: Английский

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Copper-Catalyzed Aromatic Fluorination of 2-(2-bromophenyl)pyridine via Cu(I)/Cu(III) Mechanism in Acetonitrile Solvent: Cluster-Continuum Free Energy Profile and Microkinetic Analysis

Molecular Catalysis, Journal Year: 2022, Volume and Issue: 529, P. 112560 - 112560

Published: Aug. 1, 2022

Language: Английский

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SN2 versus E2 reactions in a complex microsolvated environment: theoretical analysis of the equilibrium and activation steps of a nucleophilic fluorination

Journal of Molecular Modeling, Journal Year: 2022, Volume and Issue: 28(6)

Published: May 21, 2022

Language: Английский

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An influence of electronic structure theory method, thermodynamic and implicit solvation corrections on the organic carbonates conformational and binding energies

Journal of Computational Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 17, 2024

Abstract An impact of an electronic structure or force field method, gas‐phase thermodynamic correction, and continuum solvation model on organic carbonate clusters (S) n conformational binding energies is explored. None the tested (GFN‐FF, GAFF, MMFF94) standard semiempirical methods (PM3, AM1, RM1, PM6, PM6‐D3, PM6‐D3H4, PM7) can reproduce reference RI‐SCS‐MP2 energies. Tight‐binding GFN ‐xTB provide more realistic which are accurate enough to discard least stable conformers. The effect correction moderate be ignored if gas phase stability ranking a goal. influence stronger, especially reinforced with Gibbs free energy results in reduced spread cluster formation strongly depend particular approach vibrational thermochemistry difference between traditional harmonic modified scaled rigid – oscillator approximations reaching 10 kcal mol −1 .

Language: Английский

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QM/MM and molecular dynamics simulation of the structure and dissociation of CuF in acetonitrile solvent

Chemical Physics Letters, Journal Year: 2022, Volume and Issue: 793, P. 139468 - 139468

Published: Feb. 12, 2022

Language: Английский

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