Thermodynamic, Transport and Structural Properties of Deep Eutectic Solvent Mixtures Relevant to Capture and Conversion of CO2 to Value Added Products

A Molecular Dynamics Study

Master thesis (2021)

Authors

J. Langeveld Mechanical Engineering

Contributors

O. Moultos Engineering Thermodynamics - Mechanical, Maritime and Materials Engineering (supervisor 1)
N. Dawass Engineering Thermodynamics - Mechanical, Maritime and Materials Engineering (supervisor 1)
P. Dey Team Poulumi Dey - Mechanical, Maritime and Materials Engineering (supervisor 2)
T.J.H. Vlugt Engineering Thermodynamics - Mechanical, Maritime and Materials Engineering (supervisor 2)
Faculty
Mechanical Engineering
Copyright: © 2021 Jilles Langeveld
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Published Date

13-12-2021

Language

English

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Faculty

Mechanical Engineering

Abstract

The current industrial application of carbon capture utilization and storage (CCUS) is limited due to technological drawbacks such as high energy demand and environmental pollution. Ionic liquids (ILs) and deep eutectic solvents (DESs) are considered promising alternative solvents for the capture of carbon dioxide (CO2). DESs are often characterized by high viscosities, which hinders industrial application. This problem might be solved by mixing the DES with an organic solvent. This study aims to assess the DESs choline chloride-ethylene glycol (ethaline) and choline chloride-urea (reline) mixed with methanol and propylene carbonate (PC) for their suitability as a medium for the combined capture and electrochemical conversion of CO2. Molecular dynamics (MD) simulations are performed to obtain the densities, the viscosities, the self-diffusivities, the ionic conductivities and insight into the molecular interactions of these mixtures. Independent MD simulations are performed of these mixtures with low concentrations of the solutes CO2, oxalic acid and formic acid. Complementary studies within the Bio-cel project are conducted to characterize the solubility and electrochemical reaction of CO2 and the techno-economics.
The viscosities of the mixtures monotonically decrease for an increase of mole fraction of organic solvent, which is benign for the application of CCUS. The self-diffusivities of all constituents increase monotonically for an increase of mole fraction of organic solvent. The ionic conductivity is calculated based on the ion self-diffusivities. Ionic conductivity optima are found at a mole fraction of DES of approximately 0.6 for ethaline-PC and approximately 0.2 for ethaline-methanol and reline-methanol. For higher mole fractions of organic solvent, the ionic conductivity decreases due to a depletion of ions. Radial distribution functions (RDFs) are used to analyse the intermolecular interactions. RDF peaks between chloride-choline and chloride-ethylene glycol show an increase for an increasing mole fraction of organic solvent, which was unexpected. The numbers of hydrogen bonds decrease for addition of methanol to pure deep eutectic solvent. For addition of propylene carbonate, this decrease is less pronounced. The depletion of hydrogen bonds at low mole fractions of deep eutectic solvent is in correspondence with the decrease in viscosity and increase in self-diffusivities. The results indicate that, for the studied properties, deep eutectic solvents mixed with organic solvents are more favourable than pure deep eutectic solvents for the absorption and electrochemical conversion of CO2.