(169av) Tackling Energy Conversion Challenges through Simulations in Synergy with Experiments

The challenges posed by climate change have increased global interest in sustainable fuel production, particularly the advancement of electrochemical carbon dioxide or carbon monoxide reduction (CO2R or COR) technologies. In this regard, my research leverages the accuracy of molecular dynamics (MD) and density functional theory (DFT) simulations to augment experimental efforts in our group to enhance the selectivity and efficiency of CO2R and COR processes. By intricately analyzing the solvation dynamics and structural properties of a variety of aprotic solvents, we aim to systematically modulate the competing hydrogen evolution reaction (HER), often a significant barrier in both CO2R and COR efficiencies. The DFT and MD simulations offer atomistic insights into the solvation structure and dynamics within these solvents, enabling the identification of key descriptors that predict experimental HER and CO2R or COR selectivity. This approach allows for a targeted modification of solvent environments, guiding the design of electrolytes that favor CO₂ conversion to CO and CO to ethylene formation over HER even in the presence of water. The use of these sophisticated computational tools not only sheds light on fundamental mechanistic pathways but also paves the way for the rational design of more selective and efficient CO2R catalysts. Through this focused inquiry into the molecular underpinnings of electrolyte behavior, our work contributes to overcoming one of the significant challenges in the field of energy conversion, thereby supporting the transition towards a more sustainable and carbon-neutral energy landscape.