Ab initio molecular dynamics simulations at elevated temperature are carried out to investigate the microscopic structure of liquid mixtures (deep eutectic solvents) composed of 1:1 and 1:2 choline chloride:ethylene glycol ([Ch]Cl:EG) and 1:2:1 choline chloride:ethylene glycol:water ([Ch]Cl:EG:water). In the present study, we aim to understand the composition effect on the choline chloride:ethylene glycol deep eutectic solvent and whether there is a specific composition in these solvents with marked special behavior at the microscopic level. The role of hydrogen bonds between all components was investigated through distribution functions. The structures are governed by the balance of hydrogen bond networks and the different populations of the EG molecule conformations. In the water-containing system, water competes for association with the anion. Also, the charge distribution analysis, which is consistent with structural analysis, indicates that the results are not impacted by changing composition. In addition, the charge transfer observed between ions, EG, and water molecules appears to be significant.
With the increasing application of template assisted syntheses in deep eutectic solvents and successful application of hydrophobic deep eutectic solvents in extraction processes, where microheterogeneity plays a major role, suggestions for novel deep eutectic solvents which exhibit strong microheterogeneity are desirable. Therefore, classical molecular dynamics simulations were carried out on deep eutectic solvent systems constructed of choline chloride and some of its derivatives mixed with ethylene glycol in a molar composition of 1 : 2 since this is the optimal parent composition. The derivatives consisted of a series of elongated alkyl side chains and elongated alcohol side chains. Of these series only choline chloride ethylene glycol has been investigated experimentally, the other systems are suggested and theoretically investigated as possible target for synthesis. Our domain analysis supported by the clear distinction of polar and nonpolar parts from the electrostatic potentials reveals that strong microheterogeneity within these novel hypothetical deep eutectic solvents exists. Rather stretched than crumbled side chains maximize possible interaction sites for both polar and nonpolar parts which make the suggested compounds valuable objectives for experiments in order to exploit the microheterogeneity in deep eutectic solvents.
Deep eutectic solvents show great potential as CO2 absorbents, which is highly desirable for the sustainable development of CO2 reduction and prevention of global climate changes. Ab initio molecular dynamics simulations in the isothermal–isobaric ensemble at pressures of 1 MPa and 5 MPa and at the corresponding experimental density are carried out to investigate the CO2 absorption in choline chloride: ethylene glycol deep eutectic solvent. Based on the structural analysis, there is a strong anion and hydrogen bond donor effect and a minor cation effect on CO2 solvation in the solvent. Instead of cooperation, a competition between the anion and the hydrogen bond donor (ethylene glycol) for the interaction with CO2 is indicated. While at a lower pressure, the ethylene glycol–CO2 interaction dominates, at a higher pressure, it is the chloride–CO2 interaction. Thus, it is possible to use the same advantages within the deep eutectic solvent as the CO2 absorbent as in ionic liquids, but in the hydrogen bond, a donor can be exploited.
We present a novel cluster analysis implemented in our open-source software TRAVIS and its application to realistic and complex chemical systems. The underlying algorithm is exclusively based on atom distances. Using a two-dimensional model system, we first introduce different cluster analysis functions and their application to single snapshots and trajectories including periodicity and temporal propagation. Using molecular dynamics simulations of pure water with varying system size, we show that our cluster analysis is size-independent. Furthermore, we observe a similar clustering behavior of pure water in classical and ab initio molecular dynamics simulations, showing that our cluster analysis is universal. In order to emphasize the application to more complex systems and mixtures, we additionally apply the cluster analysis to ab initio molecular dynamics simulations of the [C2C1Im][OAc] ionic liquid and its mixture with water. Using that, we show that our cluster analysis is able to analyze the clustering of the individual components in a mixture as well as the clustering of the ionic liquid with water.
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