Supramolecular carbon nanotube-fullerene donor-acceptor hybrids for photoinduced electron transfer

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dc.contributor Wichita State University. Department of Chemistry en_US
dc.contributor.author D'Souza, Francis en_US
dc.contributor.author Chitta, Raghu en_US
dc.contributor.author Sandanayaka, Atula S. D. en_US
dc.contributor.author Subbaiyan, Navaneetha K. en_US
dc.contributor.author D'Souza, Lawrence en_US
dc.contributor.author Araki, Yasuyaki en_US
dc.contributor.author Ito, Osamu en_US
dc.date.accessioned 2012-02-06T17:15:43Z
dc.date.available 2012-02-06T17:15:43Z
dc.date.issued 2007-12-26 en_US
dc.identifier 18052162 en_US
dc.identifier 7503056 en_US
dc.identifier.citation Journal of the American Chemical Society. 2007 Dec 26; 129(51): 15865-71. en_US
dc.identifier.issn 1520-5126 en_US
dc.identifier.issn 0002-7863 en_US
dc.identifier.uri http://dx.doi.org/10.1021/ja073773x en_US
dc.identifier.uri http://hdl.handle.net/10057/4253
dc.description Click on the DOI link below to access the article (may not be free). en_US
dc.description.abstract Photoinduced electron transfer in a self-assembled single-wall carbon nanotube (SWNT)-fullerene(C60) hybrid with SWNT acting as an electron donor and fullerene as an electron acceptor has been successfully demonstrated. Toward this, first, SWNTs were noncovalently functionalized using alkyl ammonium functionalized pyrene (Pyr-NH3+) to form SWNT/Pyr-NH3+ hybrids. The alkyl ammonium entity of SWNT/Pyr-NH3+ hybrids was further utilized to complex with benzo-18-crown-6 functionalized fullerene, crown-C60, via ammonium-crown ether interactions to yield SWNT/Pyr-NH3+/crown-C60 nanohybrids. The nanohybrids were isolated and characterized by TEM, UV-visible-near IR, and electrochemical methods. Free-energy calculations suggested possibility of electron transfer from the carbon nanotube to the singlet excited fullerene in the SWNT/Pyr-NH3+/crown-C60 nanohybrids. Accordingly, steady-state and time-resolved fluorescence studies revealed efficient quenching of the singlet excited-state of C60 in the nanohybrids. Further studies involving nanosecond transient absorption studies confirmed electron transfer to be the quenching mechanism, in which the electron-transfer product, fullerene anion radical, was possible to spectrally characterize. The rates of charge separation, kCS, and charge recombination, kCR, were found to be 3.46 x 10(9) and 1.04 x 10(7) s-1, respectively. The calculated lifetime of the radical ion-pair was found to be over 100 ns, suggesting charge stabilization in the novel supramolecular nanohybrids. The present nanohybrids were further utilized to reduce hexyl-viologen dication (HV2+) and a sacrificial electron donor, 1-benzyl-1,4-dihydronicotinamide, in an electron-pooling experiment, offering additional proof for the occurrence of photoinduced charge-separation and potential utilization of these materials in light-energy harvesting applications. en_US
dc.format.extent 15865-71 en_US
dc.language.iso eng en_US
dc.publisher American Chemical Society en_US
dc.relation.ispartofseries Journal of the American Chemical Society en_US
dc.relation.ispartofseries J. Am. Chem. Soc. en_US
dc.source NLM en_US
dc.title Supramolecular carbon nanotube-fullerene donor-acceptor hybrids for photoinduced electron transfer en_US
dc.type Article en_US
dc.coverage.spacial United States en_US
dc.description.version peer reviewed en_US
dc.rights.holder Copyright © 2007 American Chemical Society en_US

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