Quantifying the Impact of Parametric Uncertainty on Automatic Mechanism Generation for CO₂ Hydrogenation on Ni(111).

ABSTRACT: Automatic mechanism generation is used to determine mechanisms for the CO₂ hydrogenation on Ni(111) in a two-stage process while considering the correlated uncertainty in DFT-based energetic parameters systematically. In a coarse stage, all the possible chemistry is explored with gas-phase products down to the ppb level, while a refined stage discovers the core methanation submechanism. Five thousand unique mechanisms were generated, which contain minor perturbations in all parameters. Global uncertainty assessment, global sensitivity analysis, and degree of rate control analysis are performed to study the effect of this parametric uncertainty on the microkinetic model predictions. Comparison of the model predictions with experimental data on a Ni/SiO₂ catalyst find a

SUBMITTER: Kreitz B 

PROVIDER: S-EPMC8549061 | biostudies-literature | 2021 Oct

REPOSITORIES: biostudies-literature