Thermodynamic Oxidation and Reduction Potentials of Photocatalytic Semiconductors in Aqueous Solution
Abstract
An approach is introduced to calculate the thermodynamic oxidation and reduction potentials of semiconductors in aqueous solution. Here, by combining a newly developed ab initio calculation method for compound formation energy and band alignment with electrochemistry experimental data, this approach can be used to predict the stability of almost any compound semiconductor in aqueous solution. Thirty photocatalytic semiconductors have been studied, and a graph (a simplified Pourbaix diagram) showing their valence/conduction band edges and oxidation/reduction potentials relative to the water redox potentials is produced. On the basis of this graph, the thermodynamic stabilities and trends against the oxidative and reductive photocorrosion for compound semiconductors are analyzed, which shows the following: (i) some metal oxides can be resistant against the oxidation by the photogenerated holes when used as the n-type photoanodes; (ii) all the nonoxide semiconductors are susceptible to oxidation, but they are resistant to the reduction by the photogenerated electrons and thus can be used as the p-type photocathodes if protected from the oxidation; (iii) doping or alloying the metal oxide with less electronegative anions can decrease the band gap but also degrade the stability against oxidation.
- Authors:
-
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); East China Normal Univ., Shanghai (China)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
- OSTI Identifier:
- 1511339
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 24; Journal Issue: 18; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; oxidation potential; photocorrosion; photoelectrode semiconductor; reduction potential; stability
Citation Formats
Chen, Shiyou, and Wang, Lin -Wang. Thermodynamic Oxidation and Reduction Potentials of Photocatalytic Semiconductors in Aqueous Solution. United States: N. p., 2012.
Web. doi:10.1021/cm302533s.
Chen, Shiyou, & Wang, Lin -Wang. Thermodynamic Oxidation and Reduction Potentials of Photocatalytic Semiconductors in Aqueous Solution. United States. https://doi.org/10.1021/cm302533s
Chen, Shiyou, and Wang, Lin -Wang. Fri .
"Thermodynamic Oxidation and Reduction Potentials of Photocatalytic Semiconductors in Aqueous Solution". United States. https://doi.org/10.1021/cm302533s. https://www.osti.gov/servlets/purl/1511339.
@article{osti_1511339,
title = {Thermodynamic Oxidation and Reduction Potentials of Photocatalytic Semiconductors in Aqueous Solution},
author = {Chen, Shiyou and Wang, Lin -Wang},
abstractNote = {An approach is introduced to calculate the thermodynamic oxidation and reduction potentials of semiconductors in aqueous solution. Here, by combining a newly developed ab initio calculation method for compound formation energy and band alignment with electrochemistry experimental data, this approach can be used to predict the stability of almost any compound semiconductor in aqueous solution. Thirty photocatalytic semiconductors have been studied, and a graph (a simplified Pourbaix diagram) showing their valence/conduction band edges and oxidation/reduction potentials relative to the water redox potentials is produced. On the basis of this graph, the thermodynamic stabilities and trends against the oxidative and reductive photocorrosion for compound semiconductors are analyzed, which shows the following: (i) some metal oxides can be resistant against the oxidation by the photogenerated holes when used as the n-type photoanodes; (ii) all the nonoxide semiconductors are susceptible to oxidation, but they are resistant to the reduction by the photogenerated electrons and thus can be used as the p-type photocathodes if protected from the oxidation; (iii) doping or alloying the metal oxide with less electronegative anions can decrease the band gap but also degrade the stability against oxidation.},
doi = {10.1021/cm302533s},
journal = {Chemistry of Materials},
number = 18,
volume = 24,
place = {United States},
year = {Fri Aug 31 00:00:00 EDT 2012},
month = {Fri Aug 31 00:00:00 EDT 2012}
}
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Figure 1: A schematic plot of the band alignment of the p-type photocathode and n-type photoanode semiconductors relative to the water redox potentials in the Z-scheme.φox shows the oxidation potential of the photoanode in aqueous solution, and φre shows the reduction potential of the photocathode.
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