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Cited by 443

The DOI matches its Crossref record; 71 of the 71 references it cites were found in a registry or an index.

Insights into Photoexcited Electron Scavenging Processes on TiO2 Obtained from Studies of the Reaction of O2 with OH Groups Adsorbed at Electronic Defects on TiO2(110)

Henderson, Michael A., Epling, William S., Peden, Charles H. F., Perkins, Craig L.·2003·The Journal of Physical Chemistry B
DOI 10.1021/jp0262113
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Abstract

In this study we show that molecular oxygen reacts with bridging OH (OH br ) groups formed as a result of water dissociation at oxygen vacancy defects on the surface of rutile TiO 2 (110). The electronic structure of an oxygen vacancy defect on TiO 2 (110) is essentially the same as that of electron trap states detected on photoexcited or sensitized TiO 2 photocatalysts, being Ti 3+ in nature. Electron energy loss spectroscopy (EELS) measurements, in agreement with valence band photoemission results in the literature, indicate that water dissociation at oxygen vacancy sites has little or no impact on the electronic structure of these sites. Temperature programmed desorption (TPD) measurements show that O 2 adsorbed at 120 K reacts with near unity reaction probability with OH br groups on TiO 2 (110) to form an unidentified intermediate that decomposes to generate terminal OH groups at nondefect sites. Commensurate with this process, the electronic defect associated with the original oxygen vacancy defect (Ti 3+ ) is oxidized. Vibrational EELS results indicate that the reaction between O 2 and OH br occurs at about 230 K, whereas electronic EELS results suggest that charge is transferred away from the vacancies at 90 K. Detailed TPD experiments in which the precoverage of water was varied indicate that chemisorption of O 2 at cation sites on the TiO 2 (110) surface is not required in order for the reaction between O 2 and OH br to occur, which implies a direct interaction between weakly bound (physisorbed) O 2 and the OH br groups. In agreement with this conclusion, we find that second-layer water, which selectively hydrogen-bonds to bridging O 2- sites and bridging OH groups, blocks the reaction of O 2 with OH br groups and prevents oxidation of the vacancy-related Ti 3+ electronic state. These results suggest that the electron scavenging role of O 2 in photocatalysis may involve a direct reaction between O 2 and trapped electrons located at bridging OH groups. Our studies suggest that the negative influence of high water concentrations in gas-phase heterogeneous photocatalysis studies results from hydrogen-bonded water blocking access of O 2 to trapped electrons located at surface OH groups.

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Metadata

Authors
Henderson, M. A., Epling, W. S., Peden, C. H. F., & Perkins, C. L.
Venue
The Journal of Physical Chemistry B
Publisher
American Chemical Society (ACS)
Published
2002-12-17
Volume
107
Issue
2
Pages
534-545
ISSN
  • 1520-5207 (ISSN-L)
  • 1520-6106
DOI
10.1021/jp0262113
OpenAlex
W2088993086
Cited by
443
References
71
FWCI
9.38
Type
journal article
Language
en
Open access
closed

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