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Publication Detail
Correlating long-lived photogenerated hole populations with photocurrent densities in hematite water oxidation photoanodes
  • Publication Type:
    Journal article
  • Publication Sub Type:
    JOUR
  • Authors:
    Pendlebury SR, Cowan AJ, Barroso M, Sivula K, Ye JH, Gratzel M, Klug DR, Tang JW, Durrant JR
  • Publication date:
    04/2012
  • Pagination:
    6304, 6312
  • Journal:
    Energy & Environmental Science
  • Volume:
    5
  • Issue:
    4
  • Print ISSN:
    1754-5692
  • Keywords:
    CHARGE RECOMBINATION KINETICS, TITANIUM-DIOXIDE FILMS, CARRIER DYNAMICS, NANOSTRUCTURED ALPHA-FE2O3, SOLAR-CELLS, THIN-FILMS, ELECTRODES, PHOTOELECTROCHEMISTRY, TIO2, PHOTOOXIDATION
  • Author URL:
  • Notes:
    Times Cited: 3 ROYAL SOC CHEMISTRY THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND CAMBRIDGE Article 914WQ English Cited References Count: 49 Pendlebury, S. R Univ London Imperial Coll Sci Technol & Med, Dept Chem, S Kensington Campus, London SW7 2AZ, England
Abstract
Photogenerated charge carrier dynamics are investigated as a function of applied bias in a variety of different hematite photoanodes for solar water oxidation. Transient absorption spectroscopy is used to probe the photogenerated holes, while transient photocurrent measures electron extraction. We report a general quantitative correlation between the population of long-lived holes and the photocurrent amplitude. The yield of long-lived holes is shown to be determined by the kinetics of electron-hole recombination. These recombination kinetics are shown to be dependent upon applied bias, exhibiting decay lifetimes ranging from ca 5 mu s to 3 ms (at -0.4 and +0.4 V versus Ag/AgCl, respectively). For Si-doped nanostructured hematite photoanodes, electron extraction and electron-hole recombination are complete within similar to 20 ms, while water oxidation is observed to occur on a timescale of hundreds of milliseconds to seconds. The competition between electron extraction and electron-hole recombination is electron-density-dependent: the effect on recombination of applied bias and excitation intensity is discussed. The timescale of water oxidation is independent of the concentration of photogenerated holes, indicating that the mechanism of water oxidation on hematite is via a sequence of single-hole oxidation steps
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