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Observation of All the Intermediate Steps of a Chemical Reaction on an Oxide Surface by Scanning Tunneling Microscopy

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Interdisciplinary Nanoscience Center (iNANO) and Department of Physics and Astronomy, Aarhus University, DK-8000 Aarhus C, Denmark
* Address correspondence to [email protected], [email protected], [email protected]
Cite this: ACS Nano 2009, 3, 3, 517–526
Publication Date (Web):February 9, 2009
https://doi.org/10.1021/nn8008245
Copyright © 2009 American Chemical Society
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    By means of high-resolution scanning tunneling microscopy (STM), we have revealed unprecedented details about the intermediate steps for a surface-catalyzed reaction. Specifically, we studied the oxidation of H adatoms by O2 molecules on the rutile TiO2(110) surface. O2 adsorbs and successively reacts with the H adatoms, resulting in the formation of water species. Using time-lapsed STM imaging, we have unraveled the individual reaction intermediates of HO2, H2O2, and H3O2 stoichiometry and the final reaction product—pairs of water molecules, [H2O]2. Because of their different appearance and mobility, these four species are discernible in the time-lapsed STM images. The interpretation of the STM results is corroborated by density functional theory calculations. The presented experimental and theoretical results are discussed with respect to previous reports where other reaction mechanisms have been put forward.

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