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Molecular Oxygen Adsorption Behaviors on the Rutile TiO2(110)-1×1 Surface: An in Situ Study with Low-Temperature Scanning Tunneling Microscopy

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Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, Anhui, China
[email protected]; [email protected]
Cite this: J. Am. Chem. Soc. 2011, 133, 6, 2002–2009
Publication Date (Web):January 19, 2011
https://doi.org/10.1021/ja110375n
Copyright © 2011 American Chemical Society
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    A knowledge of adsorption behaviors of oxygen on the model system of the reduced rutile TiO2(110)-1×1 surface is of great importance for an atomistic understanding of many chemical processes. We present a scanning tunneling microcopy (STM) study on the adsorption of molecular oxygen either at the bridge-bonded oxygen vacancies (BBOV) or at the hydroxyls (OH) on the TiO2(110)-1×1 surface. Using an in situ O2 dosing method, we are able to directly verify the exact adsorption sites and the dynamic behaviors of molecular O2. Our experiments provide direct evidence that an O2 molecule can intrinsically adsorb at both the BBOV and the OH sites. It has been identified that, at a low coverage of O2, the singly adsorbed molecular O2 at BBOV can be dissociated through an intermediate state as driven by the STM tip. However, singly adsorbed molecular O2 at OH can survive from such a tip-induced effect, which implies that the singly adsorbed O2 at OH is more stable than that at BBOV. It is interesting to observe that when the BBOVs are fully filled with excess O2 dosing, the adsorbed O2 molecules at BBOV tend to be nondissociative even under a higher bias voltage of 2.2 V. Such a nondissociative behavior is most likely attributed to the presence of two or more O2 molecules simultaneously adsorbed at a BBOV with a more stable configuration than singly adsorbed molecular O2 at a BBOV.

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