2024 AIChE Annual Meeting
(389c) Extending Wherewulff with Electric Field Effects
Authors
Kitchin, J., Carnegie Mellon University
Bender, J., Cornell University
Resasco, J., University of Texas At Austin
Just as important as the catalyst that we design to induce a reaction, the electrolyte environment that the catalyst operates in has been shown to have substantial effects on reactivity. In this work, we show how the modular nature of WhereWulff, which was originally designed for metal oxide simulations, has allowed us to integrate interfacial electric field effects within the implicit solvation formalism, in a way that is scalable across many materials and facets. Through its ContinueOptimizeFW routine, WhereWulff can model the solid-liquid interface as a parallel plate capacitor and derive the free energy of each structure as a function of applied potential (SHE). This additional layer of complexity trickles down to the downstream analyses tasks, which can now model the reactivity as a function of electrolyte conditions. Coverages and their configurational degrees of freedom are screened by a finetuned ML potential for minimal human interaction. We demonstrate how this new feature, in what was already an automated workflow, can help rationalize existence of cation effects and the effect of pH in the Oxygen Reduction Reaction (ORR). Finally, we cover some of the existing limitations of the leveraged methods.