Journal
DALTON TRANSACTIONS
Volume 39, Issue 16, Pages 3985-3989Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/b922087a
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Funding
- National Institutes of Health [R01 GM32715, T32 GM008283]
- NATIONAL INSTITUTE OF GENERAL MEDICAL SCIENCES [T32GM008283, R01GM032715] Funding Source: NIH RePORTER
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Photosynthetic water oxidation occurs naturally at a tetranuclear manganese center in the photosystem II protein complex. Synthetically mimicking this tetramanganese center, known as the oxygen-evolving complex (OEC), has been an ongoing challenge of bioinorganic chemistry. Most past efforts have centered on water-oxidation catalysis using chemical oxidants. However, solar energy applications have drawn attention to electrochemical methods. In this paper, we examine the electrochemical behavior of the biomimetic water-oxidation catalyst [(H2O)(terpy)Mn(mu-O)(2)Mn(terpy)(H2O)](NO3)(3) [terpy = 2,2': 6',2 ''-terpyridine] (1) in water under a variety of pH and buffered conditions and in the presence of acetate that binds to 1 in place of one of the terminal water ligands. These experiments show that 1 not only exhibits proton-coupled electron-transfer reactivity analogous to the OEC, but also may be capable of electrochemical oxidation of water to oxygen.
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