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

MPS-Authors
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Prieto,  Mauricio
Chemical Physics, Fritz Haber Institute, Max Planck Society;

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Gottlob,  Daniel M.
Chemical Physics, Fritz Haber Institute, Max Planck Society;

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Tanase,  Liviu Cristian
Chemical Physics, Fritz Haber Institute, Max Planck Society;

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Menzel,  Dietrich
Chemical Physics, Fritz Haber Institute, Max Planck Society;
Physik-Department E20, Technical University München;

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Schmidt,  Thomas
Chemical Physics, Fritz Haber Institute, Max Planck Society;

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Freund,  Hans-Joachim
Chemical Physics, Fritz Haber Institute, Max Planck Society;

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jacs.1c03197.pdf
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Citation

Prieto, M., Mullan, T., Schlutow, M., Gottlob, D. M., Tanase, L. C., Menzel, D., et al. (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(23), 8780-8790. doi:10.1021/jacs.1c03197.


Cite as: http://hdl.handle.net/21.11116/0000-0008-AA07-1
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 (Eaapp) 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 Eaapp 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.