Repository: Freie Universit├Ąt Berlin, Math Department

Insights into reaction kinetics in confined space: real time observation of water formation under a silica cover

Prieto, M. J. and Mullan, T. and Schlutow, M. and Gottlob, D. M. and Tanase, L. C. and Menzel, D. and Sauer, J. and Usvyat, D. and Schmidt, T. and Freund, H.-J. (2021) Insights into reaction kinetics in confined space: real time observation of water formation under a silica cover. Journal of the American Chemical Society, 143 . pp. 8780-8790.

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Abstract

We offer a comprehensive approach to determine howphysical confinement can affect the water formation reaction. By using free-standing crystalline SiO2bilayer supported on Ru(0001) as a model system,we studied the water formation reaction under confinement in situ and inreal time. Low-energy electron microscopy reveals that the reaction proceedsvia the formation of reaction fronts propagating across the Ru(0001) surface.The Arrhenius analyses of the front velocity yield apparent activationenergies (Eaapp) of 0.32 eV for the confined and 0.59 eV for the nonconfinedreaction. DFT simulations indicate that the rate-determining step remainsunchanged upon confinement, therefore ruling out the widely acceptedtransition state effect. Additionally, H2O accumulation cannot explain thechange inEaappfor the confined cases studied because its concentrationremains low. Instead, numerical simulations of the proposed kinetic modelsuggest that the H2adsorption process plays a decisive role in reproducing the Arrhenius plots

Item Type:Article
Subjects:Mathematical and Computer Sciences > Mathematics > Applied Mathematics
Divisions:Department of Mathematics and Computer Science > Institute of Mathematics > Geophysical Fluid Dynamics Group
ID Code:2375
Deposited By: Ulrike Eickers
Deposited On:27 Sep 2019 12:05
Last Modified:27 Jun 2021 07:57

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