Thermodynamic Modeling and Molecular Dynamics Simulations of Deep Eutectic Solvents

Deep eutectic solvents (DES) are a novel class of environmentally friendly solvents known for their low toxicity, adjustable viscosity, and solvating capabilities, making them an interesting option for green chemistry applications. However, the fundamental thermodynamic behavior, molecular interactions, and phase equilibria of DES are not yet fully understood, presenting challenges for their systematic design and broader utilization. This thesis aims to address these gaps through an approach that integrates thermodynamic modeling, molecular dynamics (MD) simulations, and the application of FAIR (Findable, Accessible, Interoperable, and Reusable) data principles. A theoretical framework for modeling DES is proposed to address key issues such as determining eutectic points and predicting phase behavior. An adaptation of the Bragg-Williams model is introduced, offering a simplified method for parameterizing eutectic systems while maintaining reasonable accuracy. The model is evaluated through case studies to provide insight into the DES phase equilibria. On the basis of these findings, MD simulations were used to explore molecular-level interactions and dynamics in DES, focusing on hydrogen bonding networks that significantly influence their structural and thermodynamic properties. To promote reproducibility and transparency, workflows aligned with the FAIR principles are developed to manage MD simulation metadata. These workflows are applied to investigate the interactions of DES with biomolecules and materials, providing a perspective on how DES affects structural stability, molecular mobility, and reactivity under various conditions. Case studies include examining the influence of DES on enzyme stability, the dynamics of reactive NADES systems, and structural changes in thymol-based DES under pressure. In addition, the study explores molecular electrostatics using the Generalized Born model, offering new perspectives on the electrostatic properties of DES. The combination of electrostatic modeling with MD simulations highlights the interdisciplinary nature of the work and its contributions to understanding the interactions of DES with biomolecules and materials. This research contributes to understanding of DES through modeling and simulation approaches. By addressing challenges in thermodynamic modeling, molecular simulation, and data management, it provides a basis for future studies and supports the potential application of DES in green chemistry and sustainable science.