(342an) Electronic Structure Modeling of Electric Field Driven Catalysis and Electrocatalytic Kinetics
- Conference: AIChE Annual Meeting
- Year: 2021
- Proceeding: 2021 Annual Meeting
- Group: Computational Molecular Science and Engineering Forum
- Time: Tuesday, November 9, 2021 - 3:30pm-5:00pm
Electrochemical systems are notoriously challenging for modelling these influences due to presence of a micro-scale charge separation, referred to as the interfacial double layer, with the dual impact of solvation and electric field effects. Approximations are needed to efficiently address these influences computationally. With a Helmholtz model, the magnitude of these electric fields can be related directly to applied bias and approximate width of double layer and the potential of zero charge. However, these estimates are clearly dependent on the choice of model parameters (width of double layer, potential of zero charge and parameters in an explicit/implicit solvation model). Therefore, testing the sensitivity of activation barrier estimates to these parameters and their correlation is essential to making mechanistic conclusions. In this poster, we will share results on the field sensitivity of barrier estimates with a series of electrochemical interface models, and apply these to examine elementary reactions relevant to the oxygen reduction reaction, ammonia electrosynthesis, and carbon dioxide electro-reduction.