title: Biomimetic multifunctional porous chalcogels as solar fuel catalysts.
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.
authors.affiliation: Department of Chemistry and Argonne-Northwestern Solar Energy Research (ANSER) Center, Northwestern University, Evanston, Illinois 60208-3113, USA.
authors.forename: Benjamin D
authors.initials: BD
authors.lastname: Yuhas
authors.forename: Amanda L
authors.initials: AL
authors.lastname: Smeigh
authors.forename: Amanda P S
authors.initials: AP
authors.lastname: Samuel
authors.forename: Yurina
authors.initials: Y
authors.lastname: Shim
authors.forename: Santanu
authors.initials: S
authors.lastname: Bag
authors.forename: Alexios P
authors.initials: AP
authors.lastname: Douvalis
authors.forename: Michael R
authors.initials: MR
authors.lastname: Wasielewski
authors.forename: Mercouri G
authors.initials: MG
authors.lastname: Kanatzidis
mesh_terms: D001674:Bioelectric Energy Sources; D032701:Biomimetics; D002384:Catalysis; D018011:Chalcogens / Q000737:chemistry*; D008855:Microscopy, Electron, Scanning; D015394:Molecular Structure; D055668:Photochemical Processes; D016062:Porosity; D012993:Solar Energy
chemical_list: D018011:Chalcogens