Insights into Reaction Kinetics in Confined Space: Real Time Observation of Water Formation under a Silica Cover.

ABSTRACT: We offer a comprehensive approach to determine how physical confinement can affect the water formation reaction. By using free-standing crystalline SiO₂ bilayer supported on Ru(0001) as a model system, we studied the water formation reaction under confinement in situ and in real time. Low-energy electron microscopy reveals that the reaction proceeds via the formation of reaction fronts propagating across the Ru(0001) surface. The Arrhenius analyses of the front velocity yield apparent activation energies (E_a^app) of 0.32 eV for the confined and 0.59 eV for the nonconfined reaction. DFT simulations indicate that the rate-determining step remains unchanged upon confinement, therefore ruling out the widely accepted transition state effect. Additionally, H₂O accumulation cannot explain the change in E_a^app for the confined cases studied because its concentration remains low. Instead, numerical simulations of the proposed kinetic model suggest that the H₂ adsorption process plays a decisive role in reproducing the Arrhenius plots.

SUBMITTER: Prieto MJ 

PROVIDER: S-EPMC8297729 | biostudies-literature | 2021 Jun

REPOSITORIES: biostudies-literature