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Structure, Organization, and Heterogeneity of Water-Containing Deep Eutectic Solvents


Töpfer, Kai; Pasti, Andrea; Das, Anuradha; Salehi, Seyedeh Maryam; Vazquez-Salazar, Luis Itza; Rohrbach, David; Feurer, Thomas; Hamm, Peter; Meuwly, Markus (2022). Structure, Organization, and Heterogeneity of Water-Containing Deep Eutectic Solvents. Journal of the American Chemical Society, 144(31):14170-14180.

Abstract

The spectroscopy and structural dynamics of a deep eutectic mixture (KSCN/acetamide) with varying water content is investigated from 2D IR (with the C-N stretch vibration of the SCN- anions as the reporter) and THz spectroscopy. Molecular dynamics simulations correctly describe the nontrivial dependence of both spectroscopic signatures depending on water content. For the 2D IR spectra, the MD simulations relate the steep increase in the cross-relaxation rate at high water content to the parallel alignment of packed SCN- anions. Conversely, the nonlinear increase of the THz absorption with increasing water content is mainly attributed to the formation of larger water clusters. The results demonstrate that a combination of structure-sensitive spectroscopies and molecular dynamics simulations provides molecular-level insights into the emergence of heterogeneity of such mixtures by modulating their composition.

Abstract

The spectroscopy and structural dynamics of a deep eutectic mixture (KSCN/acetamide) with varying water content is investigated from 2D IR (with the C-N stretch vibration of the SCN- anions as the reporter) and THz spectroscopy. Molecular dynamics simulations correctly describe the nontrivial dependence of both spectroscopic signatures depending on water content. For the 2D IR spectra, the MD simulations relate the steep increase in the cross-relaxation rate at high water content to the parallel alignment of packed SCN- anions. Conversely, the nonlinear increase of the THz absorption with increasing water content is mainly attributed to the formation of larger water clusters. The results demonstrate that a combination of structure-sensitive spectroscopies and molecular dynamics simulations provides molecular-level insights into the emergence of heterogeneity of such mixtures by modulating their composition.

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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 > Catalysis
Physical Sciences > General Chemistry
Life Sciences > Biochemistry
Physical Sciences > Colloid and Surface Chemistry
Uncontrolled Keywords:Colloid and Surface Chemistry, Biochemistry, General Chemistry, Catalysis
Language:English
Date:10 August 2022
Deposited On:04 Jan 2023 09:55
Last Modified:29 May 2024 01:41
Publisher:American Chemical Society (ACS)
ISSN:0002-7863
OA Status:Green
Publisher DOI:https://doi.org/10.1021/jacs.2c04169
PubMed ID:35895323
Project Information:
  • : FunderH2020
  • : Grant ID801459
  • : Project TitleFP-RESOMUS - Fellowship Program of the NCCR MUST (National Competence Center for Research in Molecular Ultrafast Science and Technology) and the Cluster of Excellence RESOLV
  • : FunderSwiss National Science Foundation
  • : Grant ID200021_117810
  • : Project Title
  • : FunderSwiss National Science Foundation
  • : Grant ID200020_188724
  • : Project Title
  • : FunderUniversity of Basel
  • : Grant ID
  • : Project Title