New Hybrid Method for the Calculation of the Solvation Free Energy of Small Molecules in Aqueous Solutions

Wu, W.; Kieffer, John

doi:10.1021/acs.jctc.8b00615

Cited by 15 publications

(15 citation statements)

References 31 publications

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“…A recent report has proposed further extension of the hybrid method to include a larger number of explicit solvent molecules in the calculation of solvation free energies for very simple ions. 103 Molecular dynamics simulations using well established force field were carried out with ions such as NH 4 + and up to 256 water molecules to establish the number of solvent molecules required to account for most of the ion-solvent interactions. A total number of 12 water molecules were finally chosen for small ions to account for the first and second solvation shell, but detailed pK a values were not calculated.…”

Section: S C H E M Ementioning

confidence: 99%

Hybrid discrete‐continuum solvation methods

Pliego

Riveros

2019

WIREs Comput Mol Sci

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Hybrid discrete‐continuum approaches for solvation have been widely applied for diverse problems in chemistry suck as pKa calculation in aqueous and nonaqueous solvents, activation free energy barriers for ionic processes in solution, and surface reactions. A special version of this approach, the cluster‐continuum quasichemical model, has also been used for establishing a single‐ion solvation free energy scale in different solvents compatible with the tetraphenylarsonium tetraphenylborate assumption. The use of discrete‐continuum solvation methods can lead to meaningful improvement with respect to pure continuum solvation models for modeling diverse chemical process in solution. In the case of pKa calculations, there are cases where the root mean squared error is as large as 7 pKa units with pure continuum solvation model and becomes around 1 pKa unit with the hybrid approach. For complex reactions in solution, errors as large as 10 kcal/mol for activation free energies with the pure continuum approach can be substantially reduced with the inclusion of explicit solvent molecules. A discussion of the theory of hybrid discrete‐continuum methods is also presented and further development is expected in the coming years. This article is categorized under: Structure and Mechanism > Reaction Mechanisms and Catalysis Software > Quantum Chemistry Molecular and Statistical Mechanics > Free Energy Methods

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Section: S C H E M Ementioning

confidence: 99%

Hybrid discrete‐continuum solvation methods

Pliego

Riveros

2019

WIREs Comput Mol Sci

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“…However, these models can easily incur errors in excess of 20 kJ mol -1 for charged solutes, and they are less amenable to systematic improvement. [4][5][6][7][8][9][10] While various hybrid implicit-explicit schemes have proposed, [10][11][12][13][14] e.g. explicit account for a few solvent molecules in the first solvation shell, this introduces other issues related to configurational sampling and the harmonic treatment of floppy vibrational modes.…”

Section: Introductionmentioning

confidence: 99%

How accurate are approximate quantum chemical methods at modelling solute–solvent interactions in solvated clusters?

Chen

Chan

Shao

et al. 2020

Phys. Chem. Chem. Phys.

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“…Specifically, QCT literature cites the absence of phase potentials in theoretical predictions and reports data in closest agreement with the absolute solvation data of Marcus, 23 while other computational studies using a similar thermodynamic cycle and cluster-continuum approach have reported closer agreement with the real solvation scale. 51,52 Of course, solvation energies will depend on how many solvent molecules are used and where they are placed. Kemp and Gordon demonstrated that the effective fragment potential method coupled with MC simulations can be used to study the solvation of F − and Cl − anions.…”

Section: Introductionmentioning

confidence: 99%

Machine Learning-Guided Approach for Studying Solvation Environments

Basdogan

Groenenboom

Henderson

et al. 2019

J. Chem. Theory Comput.

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Molecular-level understanding and characterization of solvation environments are often needed across chemistry, biology, and engineering. Toward practical modeling of local solvation effects of any solute in any solvent, we report a static and all-quantum mechanics-based cluster-continuum approach for calculating single-ion solvation free energies. This approach uses a global optimization procedure to identify low-energy molecular clusters with different numbers of explicit solvent molecules and then employs the smooth overlap for atomic positions learning kernel to quantify the similarity between different low-energy solute environments. From these data, we use sketch maps, a nonlinear dimensionality reduction algorithm, to obtain a two-dimensional visual representation of the similarity between solute environments in differently sized microsolvated clusters. After testing this approach on different ions having charges 2+, 1+, 1−, and 2−, we find that the solvation environment around each ion can be seen to usually become more similar in hand with its calculated single-ion solvation free energy. Without needing either dynamics simulations or an a priori knowledge of local solvation structure of the ions, this approach can be used to calculate solvation free energies within 5% of experimental measurements for most cases, and it should be transferable for the study of other systems where dynamics simulations are not easily carried out.

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New Hybrid Method for the Calculation of the Solvation Free Energy of Small Molecules in Aqueous Solutions

Cited by 15 publications

References 31 publications

Hybrid discrete‐continuum solvation methods

Hybrid discrete‐continuum solvation methods

How accurate are approximate quantum chemical methods at modelling solute–solvent interactions in solvated clusters?

Machine Learning-Guided Approach for Studying Solvation Environments

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