Crystallization and time-dependent changes in betaine-urea-water natural deep eutectic solvents

Lamya Al Fuhaid; Maria F. Nava-Ocampo; Szilárd S. Bucs; Robert Verpoorte; Young Hae Choi; Geert Jan Witkamp; Andreia S.F. Farinha

doi:10.1016/j.molliq.2023.122718

Crystallization and time-dependent changes in betaine-urea-water natural deep eutectic solvents

Lamya Al Fuhaid, Maria F. Nava-Ocampo, Szilárd S. Bucs, Robert Verpoorte, Young Hae Choi, Geert Jan Witkamp, Andreia S.F. Farinha^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

5 Scopus citations

Abstract

The ability to predict eutectic compositions resulting in a liquid (natural) deep eutectic solvent [(NA)DES] at room temperature or below widens their applicability range. This study examines the effect of the components’ molar ratio and water content on the stability and supramolecular network of betaine-urea-water (BUW) NADES. It also explores time-dependent changes in the solvents and possible methods to determine the stability. After being prepared at elevated temperatures (≥70 °C), some BUW crystallized upon cooling or seeding with pre-existing crystals, creating orthorhombic betaine hydrate crystals. BUW ratios yielding liquid NADES were determined by proton nuclear magnetic resonance (¹H NMR), identifying a solid–liquid boundary. Moreover, BUW conductivity decreased continually over time, suggesting a dynamic state of the solvents. Our results indicate that betaine crystallization depends on water and urea concentrations, supporting the reported synergistic effect. Additionally, this work demonstrates ¹H NMR as a method to predict BUW ratios forming liquid NADES.

Original language	English (US)
Article number	122718
Journal	Journal of Molecular Liquids
Volume	387
DOIs	https://doi.org/10.1016/j.molliq.2023.122718
State	Published - Oct 1 2023

Bibliographical note

Funding Information:
This work was supported by King Abdullah University of Science and Technology (KAUST), Thuwal, SA. The authors thank Dr. Youyou Yuan from the KAUST Imaging and Characterization Core Lab for resolving the crystal structure.

Publisher Copyright:
© 2023

Keywords

Bonding
Crystallization
DES
Metastability
Time-dependence

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
Atomic and Molecular Physics, and Optics
Condensed Matter Physics
Spectroscopy
Physical and Theoretical Chemistry
Materials Chemistry

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10.1016/j.molliq.2023.122718

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title = "Crystallization and time-dependent changes in betaine-urea-water natural deep eutectic solvents",

abstract = "The ability to predict eutectic compositions resulting in a liquid (natural) deep eutectic solvent [(NA)DES] at room temperature or below widens their applicability range. This study examines the effect of the components{\textquoteright} molar ratio and water content on the stability and supramolecular network of betaine-urea-water (BUW) NADES. It also explores time-dependent changes in the solvents and possible methods to determine the stability. After being prepared at elevated temperatures (≥70 °C), some BUW crystallized upon cooling or seeding with pre-existing crystals, creating orthorhombic betaine hydrate crystals. BUW ratios yielding liquid NADES were determined by proton nuclear magnetic resonance (1H NMR), identifying a solid–liquid boundary. Moreover, BUW conductivity decreased continually over time, suggesting a dynamic state of the solvents. Our results indicate that betaine crystallization depends on water and urea concentrations, supporting the reported synergistic effect. Additionally, this work demonstrates 1H NMR as a method to predict BUW ratios forming liquid NADES.",

keywords = "Bonding, Crystallization, DES, Metastability, Time-dependence",

author = "{Al Fuhaid}, Lamya and Nava-Ocampo, {Maria F.} and Bucs, {Szil{\'a}rd S.} and Robert Verpoorte and Choi, {Young Hae} and Witkamp, {Geert Jan} and Farinha, {Andreia S.F.}",

note = "Funding Information: This work was supported by King Abdullah University of Science and Technology (KAUST), Thuwal, SA. The authors thank Dr. Youyou Yuan from the KAUST Imaging and Characterization Core Lab for resolving the crystal structure. Publisher Copyright: {\textcopyright} 2023",

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AU - Al Fuhaid, Lamya

AU - Nava-Ocampo, Maria F.

AU - Bucs, Szilárd S.

AU - Verpoorte, Robert

AU - Choi, Young Hae

AU - Witkamp, Geert Jan

AU - Farinha, Andreia S.F.

N1 - Funding Information: This work was supported by King Abdullah University of Science and Technology (KAUST), Thuwal, SA. The authors thank Dr. Youyou Yuan from the KAUST Imaging and Characterization Core Lab for resolving the crystal structure. Publisher Copyright: © 2023

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N2 - The ability to predict eutectic compositions resulting in a liquid (natural) deep eutectic solvent [(NA)DES] at room temperature or below widens their applicability range. This study examines the effect of the components’ molar ratio and water content on the stability and supramolecular network of betaine-urea-water (BUW) NADES. It also explores time-dependent changes in the solvents and possible methods to determine the stability. After being prepared at elevated temperatures (≥70 °C), some BUW crystallized upon cooling or seeding with pre-existing crystals, creating orthorhombic betaine hydrate crystals. BUW ratios yielding liquid NADES were determined by proton nuclear magnetic resonance (1H NMR), identifying a solid–liquid boundary. Moreover, BUW conductivity decreased continually over time, suggesting a dynamic state of the solvents. Our results indicate that betaine crystallization depends on water and urea concentrations, supporting the reported synergistic effect. Additionally, this work demonstrates 1H NMR as a method to predict BUW ratios forming liquid NADES.

AB - The ability to predict eutectic compositions resulting in a liquid (natural) deep eutectic solvent [(NA)DES] at room temperature or below widens their applicability range. This study examines the effect of the components’ molar ratio and water content on the stability and supramolecular network of betaine-urea-water (BUW) NADES. It also explores time-dependent changes in the solvents and possible methods to determine the stability. After being prepared at elevated temperatures (≥70 °C), some BUW crystallized upon cooling or seeding with pre-existing crystals, creating orthorhombic betaine hydrate crystals. BUW ratios yielding liquid NADES were determined by proton nuclear magnetic resonance (1H NMR), identifying a solid–liquid boundary. Moreover, BUW conductivity decreased continually over time, suggesting a dynamic state of the solvents. Our results indicate that betaine crystallization depends on water and urea concentrations, supporting the reported synergistic effect. Additionally, this work demonstrates 1H NMR as a method to predict BUW ratios forming liquid NADES.

KW - Bonding

KW - Crystallization

KW - DES

KW - Metastability

KW - Time-dependence

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Crystallization and time-dependent changes in betaine-urea-water natural deep eutectic solvents

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

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