Atomistic Insights into the Oxidation of Flat and Stepped Platinum Surfaces Using Large-Scale Machine Learning Potential-based Grand-Canonical Monte Carlo

08 August 2022, Version 1
This content is a preprint and has not undergone peer review at the time of posting.


Understanding catalyst surface structure changes under reactive conditions has become an important topic with the increasing interest in operando measurement and modelling. In this work, we develop a workflow to build machine learning potentials (MLPs) for simulating complicated chemical systems with large spatial and time scales, in which the committee model strategy equips the MLP with uncertainty estimation, enabling active learning protocol. The methods are applied to constructing PtOx MLP based on explored configurations from bulk oxides to amorphous oxidised surfaces, which cover most ordered high-oxygen-coverage platinum surfaces within an accessible energy range. This MLP is used to perform large-scale grand canonical Monte Carlo simulations to track detailed structure changes during oxidations of flat and stepped Pt surfaces, which is normally inaccessible to costly ab initio calculations. These structural evolution trajectories reveal the stages of surface oxidation without laboriously manual construction of surface models. We identify the building blocks of oxide formation and elucidate the surface oxide formation mechanism on Pt surfaces. The insightful interpretations of the oxide formation are likely to be general for other metal surfaces. We demonstrate that these large-scale simulations would be a powerful tool to investigate realistic structures and the formation mechanisms of complicated systems.


Machine Learning Potential
Density Functional Theory
Grand Canonical Monte Carlo
Surface Oxidation

Supplementary materials

Supporting Information
Machine Learning Potential, Training Pipeline, Full List of Dataset, Lattice Constants and Surface Energies, Oxygen Diffusion Pathway on the Flat Pt(111) Surface, Uncertainty Estimation by Committee Model, Adsorption Sites on the Flat Pt(111) and Stepped Surfaces


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