2026-10-13T14:30:09Z https://api.figshare.com/v2/oai

oai:figshare.com:article/34037317 2026-10-01T00:12:20Z category_1 category_915 category_7 category_12 category_13 category_14 category_272 category_873 category_734 category_931 category_64 category_135 portal_63 item_type_6 month_year_10_2026

Modeling Reactions on the Solid–Liquid Interface with Next Generation Extended Lagrangian Quantum-Based Molecular Dynamics Rae A. Corrigan Grove (22377573) Kevin G. Kleiner (25147126) Joshua Finkelstein (10520232) Ivana Matanovic (1450015) Michael E. Wall (12078441) Travis E. Jones (1366464) Anders M. N. Niklasson (2851028) Christian F. A. Negre (8307897) Biophysics Physical Sciences not elsewhere classified Medicine Cell Biology Genetics Molecular Biology Environmental Sciences not elsewhere classified Chemical Sciences not elsewhere classified Biological Sciences not elsewhere classified Information Systems not elsewhere classified Cancer Computational Biology oxygen reduction reaction based molecular dynamics framework makes use electrostatic potential bias ideally polarizable electrode direct electron transfer 2 </ sub explicit atomistic treatment combining quantum accuracy electron transfer novel framework explicit solvation accuracy required atomistic insight lower bias higher bias electrochemical bias applied bias without adsorption varied overpotentials surface catalysis near nitrogen modeling reactions gain insight electrocatalytic processes doped graphene different mechanisms atom quantum We present a series of simulations of the oxygen reduction reaction (ORR) using a novel framework for atomistic simulations of surface catalysis under electrochemical bias. The framework makes use of quantum-mechanical extended Lagrangian Born–Oppenheimer molecular dynamics (XL-BOMD) simulations, which provide the speed and accuracy required for explicit atomistic treatment of both electrode and electrolyte. Simulations of solvated O₂ near nitrogen-doped graphene (NG) were performed to gain insight into the ORR, and different mechanisms were observed, depending on the applied bias. Under higher bias the ORR occurred by an outer-sphere mechanism, without adsorption of O₂ to NG. In this mechanism, electron transfer between the catalyst and the O₂ was mediated by the solvent. Under lower bias the ORR occurred by an inner-sphere mechanism involving adsorption of O₂ to NG, leading to direct electron transfer. Our extensive, all-atom quantum-mechanical molecular dynamics simulations also show clear differences between the kinetics of the ORR on this ideally polarizable electrode and commonly used kinetic theories, leading to new insights regarding mechanistic changes with varied overpotentials. Combining quantum accuracy with explicit solvation and electrostatic potential bias, XL-BOMD opens a route to predictive, atomistic insight into electrocatalytic processes, as demonstrated with the ORR. 2026-09-30T00:00:00Z Text Journal contribution 10.1021/acs.jpcc.6c06025.s001 https://figshare.com/articles/journal_contribution/Modeling_Reactions_on_the_Solid_Liquid_Interface_with_Next_Generation_Extended_Lagrangian_Quantum-Based_Molecular_Dynamics/34037317 CC BY-NC 4.0