Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 133, Issue 19, Pages 7252-7255Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja111275t
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- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001059]
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Biological systems that can capture and store solar energy are rich in a variety of chemical functionalities, incorporating light-harvesting components, electron-transfer cofactors, and redox-active catalysts into one supramolecule. Any artificial mimic of such systems designed for solar fuels production will require the integration of complex subunits into a larger architecture. We present porous chalcogenide frameworks that can contain both immobilized redox-active Fe4S4 clusters and light-harvesting photoredox dye molecules in close proximity. These multifunctional gels are shown to electrocatalytically reduce protons and carbon disulfide. In addition, incorporation of a photoredox agent into the chalcogels is shown to photochemically produce hydrogen. The gels have a high degree of synthetic flexibility, which should allow for a wide range of light-driven processes relevant to the production of solar fuels.
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