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Force Fields for Deep Eutectic Mixtures: Application to Structure, Thermodynamics and 2D-Infrared Spectroscopy

Töpfer, Kai; Boittier, Eric; Devereux, Mike; Pasti, Andrea; Hamm, Peter; Meuwly, Markus (2024). Force Fields for Deep Eutectic Mixtures: Application to Structure, Thermodynamics and 2D-Infrared Spectroscopy. Journal of Physical Chemistry B, 128(44):10937-10949.

Abstract

Parametrizing energy functions for ionic systems can be challenging. Here, the total energy function for an eutectic system consisting of water, SCN–, K+ and acetamide is improved vis-a-vis experimentally measured properties. Given the importance of electrostatic interactions, two different types of models are considered: the first (model M0) uses atom-centered multipole whereas the other two (models M1 and M2) are based on fluctuating minimal distributed charges (fMDCM) that respond to geometrical changes of SCN–. The Lennard-Jones parameters of the anion are adjusted to best reproduce experimentally known hydration free energies and densities, which are matched to within a few percent for the final models irrespective of the electrostatic model. Molecular dynamics simulations of the eutectic mixtures with varying water content (between 0 and 100%) yield radial distribution functions and frequency correlation functions for the CN-stretch vibration. Comparison with experiments indicates that models based on fMDCM are considerably more consistent than those using multipoles. Computed viscosities from models M1 and M2 are within 30% of measured values and their change with increasing water content is consistent with experiments. This is not the case for model M0.

Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Scopus Subject Areas:Physical Sciences > Physical and Theoretical Chemistry
Physical Sciences > Surfaces, Coatings and Films
Physical Sciences > Materials Chemistry
Language:English
Date:7 November 2024
Deposited On:04 Feb 2025 18:47
Last Modified:05 Feb 2025 21:00
Publisher:American Chemical Society (ACS)
ISSN:1520-5207
OA Status:Closed
Publisher DOI:https://doi.org/10.1021/acs.jpcb.4c05480
PubMed ID:39446046
Project Information:
  • Funder: H2020
  • Grant ID: 801459
  • Project Title: Research and innovation program under the Marie Skłodowska-Curie
  • Funder:
  • Grant ID: 200020_219779
  • Project Title: Swiss National Science Foundation
  • Funder:
  • Grant ID: 200021_215088
  • Project Title: Swiss National Science Foundation
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