Molecular Photoelectrode for Water Oxidation Inspired by Photosystem II
(2019) Journal of the American chemical society — Vol. 141, n° 19, p. 7926-7933 (2019)
Files
PSII_Resubmission_Final.pdf
Open Access - Adobe PDF
- 1.83 MB
Details
- Authors
Sampaio, Renato N. 
Meyer, Thomas J.
- 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%. 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.
- Affiliations
Citations
Wang, D., Sampaio, R. N., Troian-Gautier, L., Marquard, S. L., Farnum, B. H., Sherman, B. D., Sheridan, M. V., Dares, C. J., Meyer, G. J., & Meyer, T. J. (2019). Molecular Photoelectrode for Water Oxidation Inspired by Photosystem II. Journal of the American chemical society, 141(19), 7926-7933. https://doi.org/10.1021/jacs.9b02548 (Original work published 2019)