TY - JOUR
T1 - Biomimetic multifunctional porous chalcogels as solar fuel catalysts
AU - Yuhas, Benjamin D.
AU - Smeigh, Amanda L.
AU - Samuel, Amanda P.S.
AU - Shim, Yurina
AU - Bag, Santanu
AU - Douvalis, Alexios P.
AU - Wasielewski, Michael R.
AU - Kanatzidis, Mercouri G.
PY - 2011/5/18
Y1 - 2011/5/18
N2 - 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.
AB - 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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U2 - 10.1021/ja111275t
DO - 10.1021/ja111275t
M3 - Article
C2 - 21410264
AN - SCOPUS:79955908848
SN - 0002-7863
VL - 133
SP - 7252
EP - 7255
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 19
ER -
