First-Principles Based Modelling of Electrocatalysis Beyond Potential of Zero Charge

Explore advanced computational approaches for modeling electrocatalytic systems in this 51-minute conference talk that examines first-principles methods for understanding electrochemical interfaces beyond the potential of zero charge. Discover how implicit solvation approaches have been revitalized in interfacial electrochemistry, particularly when combined with ab initio thermodynamics to simulate electrode polarization at potentials beyond the PZC. Learn about fully-grand canonical (FGC) calculations and their applications in computing thermodynamic cyclic voltammograms, understanding why only FGC calculations can accurately capture non-Nernstian peak shifts and double layer effects on CV shape. Examine the catalytic implications of potential-induced variations in adsorption energies and their effects on detailed reaction mechanisms. Understand how machine-learned potentials enable predictive-quality explicit solvation simulations and global geometry optimization to address the operando evolution of electrodes, providing insights into the dynamic behavior of electrocatalytic systems under realistic operating conditions.