Observation of All the Intermediate Steps of a Chemical Reaction on an Oxide Surface by Scanning Tunneling Microscopy
- Jesper Matthiesen
- ,
- Stefan Wendt
- ,
- Jonas Ø. Hansen
- ,
- Georg K. H. Madsen
- ,
- Estephania Lira
- ,
- Patrick Galliker
- ,
- Ebbe K. Vestergaard
- ,
- Renald Schaub
- ,
- Erik Lægsgaard
- ,
- Bjørk Hammer
- , and
- Flemming Besenbacher
Abstract
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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