Journal
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
Volume 9, Issue 36, Pages 12262-12273Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.1c03811
Keywords
deep eutectic systems; NADES; UV resonance Raman; nuclear magnetic resonance; hydrogen bond; solvation; structure; dynamics
Categories
Funding
- Elettra Sincrotrone Trieste [20185445, 20190397]
- European Regional Development Fund
- Interreg V-A Italy Austria 2014-2020
- Politecnico di Milano
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The study found that hydration affects the strength and distribution of hydrogen bonds, leading to changes in the structure of different deep eutectic solvents. Choline acetate solvents undergo a breakage of DES-DES interactions at low water concentrations, while Choline chloride:urea maintains its structure.
Unlike the archetypal deep eutectic solvent (DES) choline chloride:urea (ChCl:U), fundamental knowledge of the intermolecular network in choline acetate (ChOAc) DESs and how they change upon dilution is still missing. Here we jointly use UV resonance Raman (UVRR) and NMR spectroscopy to comparatively explore how the strength and distribution of hydrogen bonding and the solvation of the components are modified in ChOAc:U and ChCl:U with increasing hydration. Overall, Raman and NMR data indicate that ChOAc:U is continuously affected by hydration and, even at low water concentrations, undergoes a breakage of DES-DES interactions, with rapid solvation of the urea portion and full exchange of mobile protons. On the contrary, ChCl:U seems to maintain its structure as small interplays gradually occur between urea in the DES and the surrounding water molecules. The combined approach provides a multifaceted consistent description of the systems, outlining the crucial role of the anion in driving the structure and dynamics of the materials and then yielding valuable data toward the exploitation of DESs as tunable systems.
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