TY - JOUR
T1 - Knitting the catalytic pattern of artificial photosynthesis to a hybrid graphene nanotexture
AU - Quintana, Mildred
AU - López, Alejandro Montellano
AU - Rapino, Stefania
AU - Toma, Francesca Maria
AU - Iurlo, Matteo
AU - Carraro, Mauro
AU - Sartorel, Andrea
AU - MacCato, Chiara
AU - Ke, Xiaoxing
AU - Bittencourt, Carla
AU - Da Ros, Tatiana
AU - Van Tendeloo, Gustaaf
AU - Marcaccio, Massimo
AU - Paolucci, Francesco
AU - Prato, Maurizio
AU - Bonchio, Marcella
PY - 2013/1/22
Y1 - 2013/1/22
N2 - 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.
AB - 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.
KW - artificial photosynthesis
KW - carbon nanostructures
KW - functionalized graphene
KW - polyoxometalates
KW - water oxidation catalysis
UR - http://www.scopus.com/inward/record.url?scp=84872868718&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=84872868718&partnerID=8YFLogxK
U2 - 10.1021/nn305313q
DO - 10.1021/nn305313q
M3 - Article
C2 - 23244166
AN - SCOPUS:84872868718
VL - 7
SP - 811
EP - 817
JO - ACS Nano
JF - ACS Nano
SN - 1936-0851
IS - 1
ER -