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

Jesper Matthiesen; Stefan Wendt; Jonas O. Hansen; Georg K. H. Madsen; Estephania Lira; Patrick Galliker; Ebbe K. Vestergaard; Renald Schaub; Erik Laegsgaard; Bjork Hammer; Flemming Besenbacher

doi:10.1021/nn8008245

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

Jesper Matthiesen, Stefan Wendt, Jonas O. Hansen, Georg K. H. Madsen, Estephania Lira, Patrick Galliker, Ebbe K. Vestergaard, Renald Schaub, Erik Laegsgaard, Bjork Hammer, Flemming Besenbacher

Research output: Contribution to journal › Article › peer-review

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.

Original language	English
Pages (from-to)	517-526
Number of pages	10
Journal	ACS Nano
Volume	3
Issue number	3
DOIs	https://doi.org/10.1021/nn8008245
Publication status	Published - Mar 2009

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

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.",

author = "Jesper Matthiesen and Stefan Wendt and Hansen, {Jonas O.} and Madsen, {Georg K. H.} and Estephania Lira and Patrick Galliker and Vestergaard, {Ebbe K.} and Renald Schaub and Erik Laegsgaard and Bjork Hammer and Flemming Besenbacher",

year = "2009",

month = mar,

doi = "10.1021/nn8008245",

language = "English",

volume = "3",

pages = "517--526",

journal = "ACS Nano",

issn = "1936-0851",

publisher = "American Chemical Society (ACS)",

number = "3",

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TY - JOUR

T1 - Observation of All the Intermediate Steps of a Chemical Reaction on an Oxide Surface by Scanning Tunneling Microscopy

AU - Matthiesen, Jesper

AU - Wendt, Stefan

AU - Hansen, Jonas O.

AU - Madsen, Georg K. H.

AU - Lira, Estephania

AU - Galliker, Patrick

AU - Vestergaard, Ebbe K.

AU - Schaub, Renald

AU - Laegsgaard, Erik

AU - Hammer, Bjork

AU - Besenbacher, Flemming

PY - 2009/3

Y1 - 2009/3

N2 - 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.

AB - 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.

U2 - 10.1021/nn8008245

DO - 10.1021/nn8008245

M3 - Article

SN - 1936-0851

VL - 3

SP - 517

EP - 526

JO - ACS Nano

JF - ACS Nano

IS - 3

ER -

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

Abstract

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