Knitting the catalytic pattern of artificial photosynthesis to a hybrid graphene nanotexture
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The artificial leaf project calls for new materials enabling multielectron catalysis with minimal overpotential, high turnover frequency, and long-term stability. Is graphene a better material than carbon nanotubes to enhance water oxidation catalysis for energy applications? Here we show that functionalized graphene with a tailored distribution of polycationic, quaternized, ammonium pendants provides an sp2 carbon nanoplatform to anchor a totally inorganic tetraruthenate catalyst, mimicking the oxygen evolving center of natural PSII. The resulting hybrid material displays oxygen evolution at overpotential as low as 300 mV at neutral pH with negligible loss of performance after 4 h testing. This multilayer electroactive asset enhances the turnover frequency by 1 order of magnitude with respect to the isolated catalyst, and provides a definite up-grade of the carbon nanotube material, with a similar surface functionalization. Our innovation is based on a noninvasive, synthetic protocol for graphene functionalization that goes beyond the ill-defined oxidation-reduction methods, allowing a definite control of the surface properties. © 2012 American Chemical Society.
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artificial photosynthesis; carbon nanostructures; functionalized graphene; polyoxometalates; water oxidation catalysis Artificial photosynthesis; Carbon Nanostructures; Functionalized; Polyoxometalates; Water oxidation; Ammonium compounds; Carbon nanotubes; Catalysis; Catalysts; Hybrid materials; Oxygen; Photosynthesis; Surface properties; Graphene; biomimetic material; graphite; nanomaterial; photosystem II, PSII X subunit; photosystem II, PSII-X subunit; article; chemistry; light; materials testing; photosynthesis; photosystem II; plant leaf; radiation exposure; surface property; ultrastructure; Biomimetic Materials; Graphite; Light; Materials Testing; Nanostructures; Photosynthesis; Photosystem II Protein Complex; Plant Leaves; Surface Properties
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