2019/07/15 by Kevin G. Kleiner, Aparna Nair-Kanneganti, Kleiner, Kevin G. +8
Chemistry · Energy · Physics and Astronomy · #Chemical Physics (physics.chem-ph) #Electrocatalysts for Energy Conversion #Electrochemical Analysis and Applications #FOS: Physical sciences #Materials Science (cond-mat.mtrl-sci) #Spectroscopy and Quantum Chemical Studies #cond-mat.mtrl-sci #physics.chem-ph
paper · pdf · doi:10.48550/arxiv.1907.06721
Further research is needed to confirm the results
openalex publication_date 2019/07/15 · openalex created_date 2019/07/23 · arxiv created 2020/06/27 · arxiv updated 2020/06/30 · openalex updated_date 2026/07/28
We demonstrate the applicability of extended Lagrangian Born-Oppenheimer quantum-based molecular dynamics (XL-BOMD) to model electron transfer reactions occurring on solid-liquid interfaces. Specifically, we consider the reduction of O2 as catalyzed at the interface of an N-doped graphene sheet and H2O at fuel cell cathodes. This system is a good testbed for next-generation computational chemistry methods since the electrochemical functionalities strongly depend on atomic-scale quantum mechanics. As opposed to prior iterations of first principles molecular dynamics, XL-BOMD only requires a full self-consistent-charge relaxation during the initial time step. The electronic ground state and total energy are stabilized thereafter through nuclear and electronic equations of motion assisted by an inner-product kernel updated with low-rank approximations. A species charge analysis reveals that the kernel-based XL-BOMD simulation can capture an electron transfer between the PGM-free catalyst and a solvated O2 molecule mediated by H2O, which results in the molecular dissociation of O2.