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Good mechanical stability was observed for type A and type C electrodes, whereas poor adherence characterized electrodes prepared from a ferric nitrate precursor, which separated from the substrate after two photocurrent measurements

Photoelectrochemical oxidation of water at transparent ferric oxide film electrodes

Chemical Physics Letters, no. 1 (2003): 194-200

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摘要

Thin film Fe2O3 photoanodes deposited onto conducting glass substrates were employed for the light-induced splitting of water. The effects of the employed precursor (inorganic or co-ordination compounds), dopants (Ti(IV) and Al(III)) and preparation conditions upon photoelectrochemical characteristics of the films are discussed. A photoel...更多

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简介
  • Apart from very few exceptions, semiconducting materials that are able to efficiently absorb visible light are unstable in aqueous solutions when polarized anodically where they most frequently undergo either photo-oxidation or photodecomposition.
  • This is the reason recent reports describing the extension of the response of a chemically stable photocatalyst, titanium dioxide, into the visible region of the solar spectrum have provoked a great deal of interest.
  • It is important to note recent reports[7] which describe the photooxidation of water at nanocrystalline BiVO4 (Eg of 2.4 eV) thinfilm electrodes, showing significant photon-to-current-conversion efficiencies in the 400-450 nm wavelength range
重点内容
  • Apart from very few exceptions, semiconducting materials that are able to efficiently absorb visible light are unstable in aqueous solutions when polarized anodically where they most frequently undergo either photo-oxidation or photodecomposition
  • Spray pyrolysis of Fe(III)-containing solutions onto a conducting glass substrate affords electrodes predominantly consisting of R-Fe2O3, a small amount of disorder in the dense submicron thick films is observed by Raman spectroscopy
  • Good mechanical stability was observed for type A and type C electrodes, whereas poor adherence characterized electrodes prepared from a ferric nitrate precursor, which separated from the substrate after two photocurrent measurements
  • Large photocurrents were observed following the addition of either Al3+ (1%) or Zn2+ (4%) in conjunction with Ti4+ (5%)
  • The Zn2+/Ti4+ doping of ferric oxide seems to affect the holediffusion length, which leads to a favorable negative shift of the photocurrent onset potential
  • Multiple doping of up to 5% Pt2+ in the presence of 2.5% titanium gives an improvement in the photocurrents with respect to Pt4+-doped electrodes of around 0.4 mA cm-2
  • A clear link could be established between the extent of crystallinity of the films, monitored by Raman spectroscopy, and their photoactivity
结果
  • Along with the spray time, the temperature of deposition had been previously found to be an important factor in thin-film formation.[13] Figure 1 shows the dependence of the photocurrent densities obtained from the type C electrodes upon the deposition temperature of the conducting glass substrate, which was measured directly by a K-type thermocouple.
  • Analysis of the composition of these electrodes by Raman spectroscopy showed (Figure 3) that both types of electrodes contained mainly R-Fe2O3, a small amount
结论
  • Spray pyrolysis of Fe(III)-containing solutions onto a conducting glass substrate affords electrodes predominantly consisting of R-Fe2O3, a small amount of disorder in the dense submicron thick films is observed by Raman spectroscopy.
  • Good mechanical stability was observed for type A and type C electrodes, whereas poor adherence characterized electrodes prepared from a ferric nitrate precursor, which separated from the substrate after two photocurrent measurements.
  • Other solvent choices resulted in electrodes that exhibited a poorer performance, usually due to an observed increase in disorder in the Fe2O3 films.
  • The most active films predominantly consist of well-crystallized R-Fe2O3 with the presence of only small amounts of substoichiometric iron oxide, most probably Fe3O4
总结
  • Introduction:

    Apart from very few exceptions, semiconducting materials that are able to efficiently absorb visible light are unstable in aqueous solutions when polarized anodically where they most frequently undergo either photo-oxidation or photodecomposition.
  • This is the reason recent reports describing the extension of the response of a chemically stable photocatalyst, titanium dioxide, into the visible region of the solar spectrum have provoked a great deal of interest.
  • It is important to note recent reports[7] which describe the photooxidation of water at nanocrystalline BiVO4 (Eg of 2.4 eV) thinfilm electrodes, showing significant photon-to-current-conversion efficiencies in the 400-450 nm wavelength range
  • Results:

    Along with the spray time, the temperature of deposition had been previously found to be an important factor in thin-film formation.[13] Figure 1 shows the dependence of the photocurrent densities obtained from the type C electrodes upon the deposition temperature of the conducting glass substrate, which was measured directly by a K-type thermocouple.
  • Analysis of the composition of these electrodes by Raman spectroscopy showed (Figure 3) that both types of electrodes contained mainly R-Fe2O3, a small amount
  • Conclusion:

    Spray pyrolysis of Fe(III)-containing solutions onto a conducting glass substrate affords electrodes predominantly consisting of R-Fe2O3, a small amount of disorder in the dense submicron thick films is observed by Raman spectroscopy.
  • Good mechanical stability was observed for type A and type C electrodes, whereas poor adherence characterized electrodes prepared from a ferric nitrate precursor, which separated from the substrate after two photocurrent measurements.
  • Other solvent choices resulted in electrodes that exhibited a poorer performance, usually due to an observed increase in disorder in the Fe2O3 films.
  • The most active films predominantly consist of well-crystallized R-Fe2O3 with the presence of only small amounts of substoichiometric iron oxide, most probably Fe3O4
基金
  • This work was supported by the Swiss Federal Office of Energy
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