Molecular Photoelectrode for Water Oxidation Inspired by Photosystem II
Abstract
In artificial photosynthesis, the sun drives water splitting into H2 and O2 or converts CO2 into a useful form of carbon. In most schemes, water oxidation is typically the limiting half-reaction. Here, we introduce a molecular approach to the design of a photoanode that incorporates an electron acceptor, a sensitizer, an electron donor, and a water oxidation catalyst in a single molecular assembly. The strategy mimics the key elements in Photosystem II by initiating light-driven water oxidation with integration of a light absorber, an electron acceptor, an electron donor, and a catalyst in a controlled molecular environment on the surface of a conducting oxide electrode. Visible excitation of the assembly results in the appearance of reductive equivalents at the electrode and oxidative equivalents at a catalyst that persist for seconds in aqueous solutions. Steady-state illumination of the assembly with 440 nm light with an applied bias results in photoelectrochemical water oxidation with a per-photon absorbed efficiency of 2.3%. Here, the results are notable in demonstrating that light-driven water oxidation can be carried out at a conductive electrode in a structure with the functional elements of Photosystem II including charge separation and water oxidation.
- Authors:
-
[1];
[1];
[2];
[3];
[1];
[4];
[1];
[1]
- Univ. of North Carolina, Chapel Hill, NC (United States)
- Auburn Univ., AL (United States)
- Texas Christian Univ., Fort Worth, TX (United States)
- Florida International Univ., Miami, FL (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Alliance for Molecular PhotoElectrode Design for Solar Fuels (AMPED); University of North Carolina, Chapel Hill, NC (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1566599
- Grant/Contract Number:
- SC0001011
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 141; Journal Issue: 19; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysis (homogeneous); catalysis (heterogeneous); electrocatalysis; solar (fuels); photosynthesis (natural and artificial); defects; charge transport; materials and chemistry by design; mesostructured materials; synthesis (novel materials); synthesis (self-assembly); charge transfer; electrodes; catalysts; oxidation water oxidation
Citation Formats
Wang, Degao, Sampaio, Renato N., Troian-Gautier, Ludovic, Marquard, Seth L., Farnum, Byron H., Sherman, Benjamin D., Sheridan, Matthew V., Dares, Christopher J., Meyer, Gerald J., and Meyer, Thomas J. Molecular Photoelectrode for Water Oxidation Inspired by Photosystem II. United States: N. p., 2019.
Web. doi:10.1021/jacs.9b02548.
Wang, Degao, Sampaio, Renato N., Troian-Gautier, Ludovic, Marquard, Seth L., Farnum, Byron H., Sherman, Benjamin D., Sheridan, Matthew V., Dares, Christopher J., Meyer, Gerald J., & Meyer, Thomas J. Molecular Photoelectrode for Water Oxidation Inspired by Photosystem II. United States. https://doi.org/10.1021/jacs.9b02548
Wang, Degao, Sampaio, Renato N., Troian-Gautier, Ludovic, Marquard, Seth L., Farnum, Byron H., Sherman, Benjamin D., Sheridan, Matthew V., Dares, Christopher J., Meyer, Gerald J., and Meyer, Thomas J. Thu .
"Molecular Photoelectrode for Water Oxidation Inspired by Photosystem II". United States. https://doi.org/10.1021/jacs.9b02548. https://www.osti.gov/servlets/purl/1566599.
@article{osti_1566599,
title = {Molecular Photoelectrode for Water Oxidation Inspired by Photosystem II},
author = {Wang, Degao and Sampaio, Renato N. and Troian-Gautier, Ludovic and Marquard, Seth L. and Farnum, Byron H. and Sherman, Benjamin D. and Sheridan, Matthew V. and Dares, Christopher J. and Meyer, Gerald J. and Meyer, Thomas J.},
abstractNote = {In artificial photosynthesis, the sun drives water splitting into H2 and O2 or converts CO2 into a useful form of carbon. In most schemes, water oxidation is typically the limiting half-reaction. Here, we introduce a molecular approach to the design of a photoanode that incorporates an electron acceptor, a sensitizer, an electron donor, and a water oxidation catalyst in a single molecular assembly. The strategy mimics the key elements in Photosystem II by initiating light-driven water oxidation with integration of a light absorber, an electron acceptor, an electron donor, and a catalyst in a controlled molecular environment on the surface of a conducting oxide electrode. Visible excitation of the assembly results in the appearance of reductive equivalents at the electrode and oxidative equivalents at a catalyst that persist for seconds in aqueous solutions. Steady-state illumination of the assembly with 440 nm light with an applied bias results in photoelectrochemical water oxidation with a per-photon absorbed efficiency of 2.3%. Here, the results are notable in demonstrating that light-driven water oxidation can be carried out at a conductive electrode in a structure with the functional elements of Photosystem II including charge separation and water oxidation.},
doi = {10.1021/jacs.9b02548},
journal = {Journal of the American Chemical Society},
number = 19,
volume = 141,
place = {United States},
year = {Thu Apr 25 00:00:00 EDT 2019},
month = {Thu Apr 25 00:00:00 EDT 2019}
}
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Works referencing / citing this record:
A stable dye-sensitized photoelectrosynthesis cell mediated by a NiO overlayer for water oxidation
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