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Photocatalytic water oxidation with nonsensitized IrO2 nanocrystals under visible and UV light.

Authors
  • Frame, F Andrew1
  • Townsend, Troy K
  • Chamousis, Rachel L
  • Sabio, Erwin M
  • Dittrich, Th
  • Browning, Nigel D
  • Osterloh, Frank E
  • 1 Department of Chemistry, University of California, Davis, One Shields Ave, Davis, California 95616, USA.
Type
Published Article
Journal
Journal of the American Chemical Society
Publisher
American Chemical Society
Publication Date
May 18, 2011
Volume
133
Issue
19
Pages
7264–7267
Identifiers
DOI: 10.1021/ja200144w
PMID: 21524069
Source
Medline
License
Unknown

Abstract

Rutile IrO(2) is known as being among the best electrocatalysts for water oxidation. Here we report on the unexpected photocatalytic water oxidation activity of 1.98 nm ± 0.11 nm succinic acid-stabilized IrO(2) nanocrystals. From aqueous persulfate and silver nitrate solution the nonsensitized particles evolve oxygen with initial rates up to 0.96 μmol min(-1), and with a quantum efficiency of at least 0.19% (measured at 530 nm). The catalytic process is driven by visible excitations from the Ir-d(t(2g)) to the Ir-d(e(g)) band (1.5-2.75 eV) and by ultraviolet excitations from the O-p band to the Ir-d(e(g)) (>3.0 eV) band. The formation of the photogenerated charge carriers can be directly observed with surface photovoltage spectroscopy. The results shed new light on the role of IrO(2) in dye- and semiconductor-sensitized water splitting systems.

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