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  4. Activation Energies for the Rate-Limiting Step in Water Photooxidation by Nanostructured alpha-Fe2O3 and TiO2
 
research article

Activation Energies for the Rate-Limiting Step in Water Photooxidation by Nanostructured alpha-Fe2O3 and TiO2

Cowan, Alexander J.
•
Barnett, Christopher J.
•
Pendlebury, Stephanie R.
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2011
Journal of the American Chemical Society

Competition between charge recombination and the forward reactions required for water splitting limits the efficiency of metal-oxide photocatalysts. A key requirement for the photochemical oxidation of water on both nanostructured alpha-Fe2O3 and TiO2 is the generation of photoholes with lifetimes on the order of milliseconds to seconds. Here we use transient absorption spectroscopy to directly probe the long-lived holes on both nc-TiO2 and alpha-Fe2O3 in complete PEC cells, and we investigate the factors controlling this slow hole decay, which can be described as the rate-limiting step in water oxidation. In both cases this rate-limiting step is tentatively assigned to the hole transfer from the metal oxide to a surface-bound water species. We demonstrate that one reason for the slow hole transfer on alpha-Fe2O3 is the presence of a significant thermal barrier, the magnitude of which is found to be independent of the applied bias at the potentials examined. This is in contrast to nanocrystalline nc-TiO2, where no distinct thermal barrier to hole transfer is observed.

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Type
research article
DOI
10.1021/ja200800t
Author(s)
Cowan, Alexander J.
Barnett, Christopher J.
Pendlebury, Stephanie R.
Barroso, Monica
Sivula, Kevin  
Graetzel, Michael  
Durrant, James R.
Klug, David R.
Date Issued

2011

Published in
Journal of the American Chemical Society
Volume

133

Start page

10134

End page

10140

Subjects

Transient Absorption-Spectroscopy

•

Carrier Dynamics

•

Oxygen Evolution

•

Films

•

Oxidation

•

Hematite

•

Oxide

•

Hydrogen

•

Holes

•

Nanoparticles

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LPI  
Available on Infoscience
January 13, 2012
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/76622
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