Water in biodegradable glucose–water–urea deep eutectic solvent: modifications of structure and dynamics in a crowded environment

Baksi, Atanu; Rajbangshi, Juriti; Biswas, Ranjit

doi:10.1039/d1cp00734c

Cited by 10 publications

(9 citation statements)

References 72 publications

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“…In a recent in silico study, a NADES composed of glucose, urea, and water in a weight ratio of 6:4:1 is probed at a slightly elevated temperature. The investigation reported an enhancement in distortion in the orientational order of water in the ternary mixture compared to that in bulk water . These alterations in the “inter-” and intracomponent interactions in binary and ternary mixtures can impact the structure and dynamics of biomolecules like protein and nucleic acids. − The denaturation of protein in the presence of urea is inhibited if choline chloride or TMAO is added in an appropriate ratio. , …”

Section: Introductionmentioning

confidence: 99%

In Silico Elucidation of Molecular Picture of Water–Choline Chloride Mixture

2021

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Choline chloride (ChCl) is a component of several deep eutectic solvents (DESs) having numerous applications. Recent studies have reported manifold promising use of aqueous choline chloride solution as an alternative to DES, where water plays the role of the hydrogen-bond donor. The characteristic physical properties of the DESs and aqueous DES originate from the "inter-" and intraspecies hydrogen-bond network formed by the constituents. However, a detailed molecular-level picture of choline chloride and water mixture is largely lacking in the literature. This motivates us to carry out extensive all-atom molecular dynamics simulations of the ChCl−water mixture of varying compositions. Our analyses clearly show an overall increase in the interspecies association with an increase in ChCl concentration. At higher concentrations, the trimethylammonium groups of choline are stabilized by a nonpolar interaction, whereas the hydroxyl groups preferentially interact with water. Chloride ions are found to be involved in two types of interactions: one where chloride ions intercalate two or more choline cations, and the other one where they are surrounded by five to six water molecules forming solvated chloride ions. However, the relative fractions of these two types of associations depend on the concentration of ChCl in the mixture. Another important structural aspect is the disruption of the hydrogen-bonded water network due to the presence of both choline cations and chloride ions. However, chloride ions participate to partially restore the tetrahedral arrangement of partners around water molecules.

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Section: Introductionmentioning

confidence: 99%

In Silico Elucidation of Molecular Picture of Water–Choline Chloride Mixture

2021

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“…Note that these structural H-bond relaxation times (⟨τ C HB ⟩) are easily experimentally accessible, unlike continuous H-bond relaxation times (⟨τ S HB ⟩). This ⟨τ C HB ⟩ are known 79 , 80 , 87 , 88 , 98 − 100 to be strongly coupled to the translational diffusion of H-bonded molecules. Significant fluctuations in structural H-bond relaxation of water–water and TBA–water H bonds at x TBA ∼0.15 have been found where anomalies have been reported in experiments for various aqueous amphiphilic solutions.…”

Section: Resultsmentioning

confidence: 99%

“…Note that these structural H-bond relaxation times (⟨τ C HB ⟩) are easily experimentally accessible, unlike continuous H-bond relaxation times (⟨τ S HB ⟩). This ⟨τ C HB ⟩ are known ,,,,− to be strongly coupled to the translational diffusion of H-bonded molecules. Significant fluctuations in structural H-bond relaxation of water–water and TBA–water H bonds at x TBA ∼0.15 have been found where anomalies have been reported in experiments for various aqueous amphiphilic solutions. − This suggests a correlation between hydrogen-bond fluctuation dynamics and experimentally observed dynamic anomaly at a composition nearly twice as large as the composition where structural anomalies have been found.…”

Section: Resultsmentioning

confidence: 99%

Dynamical Anomaly of Aqueous Amphiphilic Solutions: Connection to Solution H-Bond Fluctuation Dynamics?

Baksi

Biswas

2022

ACS Omega

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We have investigated the possible connection between “dynamical anomaly” observed in time-resolved fluorescence measurements of reactive and nonreactive solute-centered relaxation dynamics in aqueous binary mixtures of different amphiphiles and the solution intra- and interspecies H-bond fluctuation dynamics. Earlier studies have connected the anomalous thermodynamic properties of binary mixtures at very low amphiphile concentrations to the structural distortion of water. This is termed as “structural anomaly.” Interestingly, the abrupt changes in the composition-dependent average rates of solute relaxation dynamics occur at amphiphile mole fractions approximately twice as large as those where structural anomalies appear. We have investigated this anomalous solution dynamical aspect by considering (water + tertiary butanol) as a model system and performed molecular dynamics simulations at several tertiary butanol (TBA) concentrations covering the extremely dilute to the moderately concentrated regimes. The “dynamical anomaly” has been followed via monitoring the composition dependence of the intra- and interspecies H-bond fluctuations and reorientational relaxations of TBA and water molecules. Solution structural aspects have been followed via examining the tetrahedral order parameter, radial and spatial distribution functions, numbers of H bonds per water and TBA molecules, and the respective populations participating in H-bond formation. Our simulations reveal abrupt changes in the H-bond fluctuations and reorientational dynamics and tetrahedral order parameter at amphiphile concentrations differing approximately by a factor of 2 and corroborates well with the steady-state and the time-resolved spectroscopic measurements. This work therefore explains, following a uniform and cogent manner, both the experimentally observed structural and dynamical anomalies in microscopic terms.

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“…Similarly, Baksi et al examined the structure of water in NA-DES containing glucose and urea. [40] They found a larger distortion in the structure and dynamics of the water in terms of reduction in tetrahedral arrangement and diffusion coefficient of water as compared to the neat water. These studies mostly focus on the structure of the solvent and co-solvent in the bulk mixture, but the relative arrangement of the constituent molecules around a central solute molecule, especially a hydrophobic one are still lacking.…”

Section: Introductionmentioning

confidence: 96%

“…Similarly, Baksi et al . examined the structure of water in NA‐DES containing glucose and urea [40] . They found a larger distortion in the structure and dynamics of the water in terms of reduction in tetrahedral arrangement and diffusion coefficient of water as compared to the neat water.…”

Section: Introductionmentioning

confidence: 99%

Structure and Orientation of Water and Choline Chloride Molecules around a Methane Hydrophobe: A Computer Simulation Study

et al. 2022

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Recent studies have reported manifold industrial applications of aqueous choline chloride (ChCl) solution as an alternative to deep eutectic solvent. ChCl also serves as a protecting cosolvent for proteins by restricting urea to approach the protein surface and thereby maintaining the water structure around the protein. However, a detailed molecular-level picture of the ChCl and water, even in the absence of urea around a representative hydrophobe is largely lacking. This motivates us to probe the effect of varying wt % of ChCl on the occupancy and orientations of the constituents around a representative solute like methane using computer simulations. Accumulation of water molecules and preferential exclusion of ChCl from the surface of methane perturb the tetrahedral geometry of water around it. We find a tangential alignment of the polar part of the ChCl molecules that interact with water, whereas its hydrophobic part is preferentially facing the methane. With an increase in ChCl wt %, a disruption in the tetrahedrality is evident for water molecules accompanied by a reduction in hydrogen bonds between water pairs in the solution. In short, ChCl induces crowding and modifies the microscopic arrangement and hydrogen bonding structure of the water around the methane and beyond.

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Water in biodegradable glucose–water–urea deep eutectic solvent: modifications of structure and dynamics in a crowded environment

Abstract: Molecular dynamics simulations have been performed on a highly viscous (η~255 cP) naturally abundant deep eutectic solvent (NADES) composed of glucose, urea and water at a weight ratio of 6:4:1...

Cited by 10 publications

References 72 publications

In Silico Elucidation of Molecular Picture of Water–Choline Chloride Mixture

In Silico Elucidation of Molecular Picture of Water–Choline Chloride Mixture

Dynamical Anomaly of Aqueous Amphiphilic Solutions: Connection to Solution H-Bond Fluctuation Dynamics?

Structure and Orientation of Water and Choline Chloride Molecules around a Methane Hydrophobe: A Computer Simulation Study

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