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Correlating long-lived photogenerated hole populations with photocurrent densities in hematite water oxidation photoanodes
Open accessAbstract
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 μs 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 ∼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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Cites
Photosynthetic energy conversion: natural and artificial
Barber, J. (2009) · Chem. Soc. Rev. · doi:10.1039/b802262n · Cited by 1,843
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Self-citationYang, W., Prabhakar, R. R., Tan, J., Tilley, S. D., & Moon, J. (2019) · Chemical Society Reviews · doi:10.1039/c8cs00997j · Cited by 787
Back Electron–Hole Recombination in Hematite Photoanodes for Water Splitting
Le Formal, F., Pendlebury, S. R., Cornuz, M., Tilley, S. D., Grätzel, M., & Durrant, J. R. (2014) · Journal of the American Chemical Society · doi:10.1021/ja412058x · Cited by 494
Self-citationAdaptive semiconductor/electrocatalyst junctions in water-splitting photoanodes
Lin, F., & Boettcher, S. W. (2014) · Nature Materials · doi:10.1038/nmat3811 · Cited by 490
Ye, C., Li, J.-X., Li, Z.-J., Li, X.-B., Fan, X.-B., Zhang, L.-P., Chen, B., Tung, C.-H., & Wu, L.-Z. (2015) · ACS Catalysis · doi:10.1021/acscatal.5b02185 · Cited by 490
Metadata
- Authors
- Pendlebury, S. R., Cowan, A. J., Barroso, M., Sivula, K., Ye, J., Grätzel, M., Klug, D. R., Tang, J., & Durrant, J. R.
- Venue
- Energy Environ. Sci.
- Publisher
- Royal Society of Chemistry (RSC)
- Published
- 2012
- Volume
- 5
- Issue
- 4
- Pages
- 6304-6312
- ISSN
- 1754-5692 (ISSN-L)
- 1754-5706
- OpenAlex
- W2149651531
- Cited by
- 234
- References
- 1
- FWCI
- 5.12
- Type
- journal article
- Language
- en
- Open access
- green
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- Pendlebury, S. R., Cowan, A. J., Barroso, M., Sivula, K., Ye, J., Grätzel, M., Klug, D. R., Tang, J., & Durrant, J. R. (2012). Correlating long-lived photogenerated hole populations with photocurrent densities in hematite water oxidation photoanodes. Energy Environ. Sci. https://doi.org/10.1039/c1ee02567h
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