Modeling Electrocatalysis Without the Pain - Past, Present, and Future

Explore the evolution and future of computational approaches to electrocatalytic reaction modeling in this 55-minute conference talk from IPAM's Bridging Scales from Atomistic to Continuum in Electrochemical Systems Workshop. Learn about the challenges of achieving atomistic accuracy in electrocatalysis modeling, which traditionally requires expensive molecular dynamics coupled with density functional theory (DFT). Discover how theoretical approaches have evolved from the widely used limiting-potential framework that neglects kinetic barriers to more sophisticated methodologies. Examine the presenter's current approach that combines DFT with a microsolvation framework implemented in VASPsol++ code, enabling computation of complete free-energy landscapes including activation barriers in a thermodynamically consistent manner. See practical applications of this methodology to CO2 electrolysis and gain mechanistic insights into C2 product selectivity. Understand future research directions including the development of advanced implicit electrolyte models that incorporate quantum-mechanical coupling to capture hydrogen bonding and charge transfer, extension to implicit adlayer models, and construction of coarse-grained machine-learning tight-binding frameworks for stochastic sampling. Learn about the quasiatomic orbital formalism used to extract atomic integrals and encode wavefunction structure via exponential-operator ansatz, offering a pathway to linear-scaling electronic structure calculations with chemical accuracy and making predictive electrocatalysis modeling more practical.