Journal
ACS NANO
Volume 3, Issue 3, Pages 517-526Publisher
AMER CHEMICAL SOC
DOI: 10.1021/nn8008245
Keywords
titania (TiO2); oxygen; water; HO2/H2O2 intermediates, hydroxyls; scanning tunneling microscopy (STM); density functional theory (DFT)
Categories
Funding
- Danish Ministry of Science, Technology, and Innovation through iNANO
- Danish Research Councils
- Danish Center for Scientific Computing
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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 O-2 molecules on the rutile TiO2(110) surface. O-2 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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