New advancements in chemical separation processes are necessary to sustainably meet the increasing demand for electronics.
1 Particularly, progress is needed in solvent design under the influence of external stimuli.
2 Ionic liquids (ILs) offer an opportunity to investigate the effect of external stimuli such as external electric fields (EEFs) on separation media. ILs have thermophysical properties that make them attractive solvents for sustainable separation processes such as low volatility, high thermal stability, and tuneability of their thermophysical properties.
3 Moreover, their charged nature makes them a great test case to investigate how the direct effects of EEFs on nanoscale dynamics and structure can impact the thermophysical properties of solvents under external stimuli. We uncover structure-property relationships for the thermophysical properties of ILs under EEFs by exploring the effects of external stimuli on structure, dynamics, and thermophysical properties through molecular dynamics simulations. For effects on structure, we quantify the effect of EEFs on nanoscale organization through excess entropy and its immediate consequences to dynamics by testing scaling relationships between self-diffusion coefficients and excess entropy under EEFs.
4 Through excess entropy relationships, we are able to describe the entire dynamical landscape of a mixture and correlate systems that showcase distinct reactions to dynamics under external stimuli. With this understanding of dynamics, we also elucidate the emergent electrothermic properties of charged solvents in the presence of EEFs such as the electrostrictive and electrocaloric coefficients. Finally, with the implementation of novel methodologies to detect glass transition temperature from MD simulations, we explore the emergent phase-changing effect of EEF on ILs by correlating changes in excess entropy in the liquid phase to changes to the glass transition temperature.
5 Such analysis allows us to establish connections between the glass and liquid phases and showcases how MD simulations can be leveraged to investigate the emergent behavior of ILs under EEFs, gain insights on the effects of EEF on the structural organization, and establish a better understanding of their thermophysical properties. With this insight we construct structure-property relationships for transport and thermophysical properties of IL in the presence of an EEF. Unlocking the control of transport and thermophysical properties through the manipulation of IL structure and EEF and eventually allowing for the next paradigm of separation schemes.
References:
(1) Eggert, R.; Wadia, C.; Anderson, C.; Bauer, D.; Fields, F.; Meinert, L.; Taylor, P. Rare Earths: Market Disruption, Innovation, and Global Supply Chains. Annu Rev Environ Resour 2016, 41 (1), 199–222. https://doi.org/10.1146/annurev-environ-110615-085700.
(2) A Research Agenda for Transforming Separation Science; National Academies Press: Washington, D.C., 2019. https://doi.org/10.17226/25421.
(3) Welton, T. Ionic Liquids: A Brief History. Biophys Rev 2018, 10 (3), 691–706. https://doi.org/10.1007/S12551-018-0419-2.
(4) Dyre, J. C. Perspective: Excess-Entropy Scaling. J Chem Phys 2018, 149 (21). https://doi.org/10.1063/1.5055064.
(5) Carmona Esteva, F. J.; Zhang, Y.; Colón, Y. J.; Maginn, E. J. Molecular Dynamics Simulation of the Influence of External Electric Fields on the Glass Transition Temperature of the Ionic Liquid 1-Ethyl-3-Methylimidazolium Bis(Trifluoromethylsulfonyl)Imide. J Phys Chem B 2023, 127 (20), 4623–4632. https://doi.org/10.1021/acs.jpcb.3c00936.
Research Interests
My research interest include but are not limited to; molecular modeling of electrocatalytic systems for the reduction of carbon dioxide, methodologies for predicting thermophysical properties of systems from molecular dynamics simulations, the development of sustainable food processing and the study of glass forming systems.
