Biomimetic multifunctional porous chalcogels as solar fuel catalysts |
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Authors: | Yuhas Benjamin D Smeigh Amanda L Samuel Amanda P S Shim Yurina Bag Santanu Douvalis Alexios P Wasielewski Michael R Kanatzidis Mercouri G |
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Institution: | Department of Chemistry and Argonne-Northwestern Solar Energy Research (ANSER) Center, Northwestern University, Evanston, Illinois 60208-3113, USA. |
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Abstract: | 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 Fe(4)S(4) 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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