The increasing concentration of carbon dioxide (CO₂) in the atmosphere is a major contributor to global climate change. Electrochemical CO₂ reduction (CO₂ER) has emerged as a promising solution, enabling the conversion of CO₂ into valuable products such as alcohols, fuels and acids. The performance of CO₂ER systems strongly depend on the choice of electrolyte, which affects CO₂ solubility, ion transport, and the overall reaction environment. This study explores both non-aqueous (organic solvents) and aqueous (with ionic liquids as additives) electrolytes to gain deeper insights into their role in CO₂ electrochemical reduction. A data-driven strategy is employed by combining high-throughput density functional theory (DFT), COSMO-RS calculations, and molecular dynamics (MD) simulations to screen and evaluate a wide range of chemical systems. These simulations are efficiently managed through MISPR, an open-source workflow tool that automates DFT and MD processes for systematic property analysis. In the non-aqueous systems, more than 3000 organic solvents from 11 chemical classes are examined to understand how their molecular features influence key properties such as viscosity, CO₂ solubility, and ion mobility. The comparison between protic and aprotic solvents highlights significant differences in transport and solvation behavior, which impact reaction performance. Alongside, aqueous systems with ionic liquids as additives are also being explored for their potential to enhance CO₂ solubility, improve conductivity, and expand the electrochemical window. By examining both types of electrolytes, this work offers a flexible approach to guide the design of improved electrolyte systems. The insights gained from these simulations help build a foundation for tuning solvation behavior and optimizing electrolyte performance for efficient and sustainable CO₂ conversion.
