Abstract
Artificial photosynthesis provides a basis for storing solar energy in chemical bonds (1, 2), with water oxidation a critical step (3, 4). The half reaction for the oxidation of water, 2H2O → O2 + 4e− + 4H+, provides protons and electrons for the production of a fuel at a cathode (4, 5). In carrying out the reaction, it is necessary to develop highly stable molecular catalysts that cycle through multiple oxidation states during water oxidation cycles. Better mechanistic understanding of water oxidation is an important element in the correlation of structure and function in the design of high efficiency catalysts for long-term water oxidation. Since the first molecular water oxidation catalyst, the “blue dimer,” described (6), many examples, based largely on complexes of Ru and Ir, have appeared that demonstrate catalytic water oxidation, including mechanistic details about how the reactions occur (7, 8). Recently, catalysts based on earth-abundant elements like Fe or Co have also been prepared with the thought of scale-up at the device level in artificial photosynthetic schemes (9⇓–11). A structure of interest has been the Co4O4 cluster, with a structure related to the reaction center in natural photosynthesis, the latter based on the Mn … [↵][1]1To whom correspondence may be addressed. Email: tjmeyer{at}unc.edu. [1]: #xref-corresp-1-1
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