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dc.contributor.author장진호-
dc.date.accessioned2018-02-28T04:40:15Z-
dc.date.available2018-02-28T04:40:15Z-
dc.date.issued2012-09-
dc.identifier.citationJournal of the American Chemical Society,Vol.134 No.39 [2012],p16265-16274en_US
dc.identifier.issn0002-7863-
dc.identifier.urihttp://pubs.acs.org/doi/10.1021/ja3057997-
dc.identifier.urihttp://hdl.handle.net/20.500.11754/41105-
dc.description.abstractThe electrochemistry, spectroscopy, and electrogenerated chemiluminescence (ECL) of a series of g-stacked poly(fluorenemethylene) oligomers (Fn, n = 1-6) were investigated. The pendant cofacially oriented fluorene moieties are essentially in contact with each other by Van der Waals interaction promoting electronic delocalization in these species. All six compounds give successive cyclic voltammetric one-electron (1e) oxidations in 1:1 acetonitrile/benzene (MeCN/Bz), and the multiple le transfer properties of all these compounds were confirmed by chronoamperometric experiments with an ultramicroelectrode and digital simulations. The potentials for oxidation of the successive le transfers can be explained in terms of electrostatic interactions among the fluorenes. The monomer (F1) shows one irreversible wave, while F2 shows two reversible le waves. F3 shows only two reversible le oxidation waves, which is consistent with the large energy to remove a third electron because of the greater electrostatic repulsion, so the third wave is shifted toward more positive potentials. Both F4 and F5 show three reversible le oxidation waves, while F6 shows four reversible le waves. The removal of the first electron from an oligomer becomes easier as n increases. The stability of the radical cations also increases with n. The removal of consecutive electrons from Fn can be correlated with the distance between fluorene moieties. No reduction peaks were observed except for some broad ones at similar to-3.2 V vs SCE in THF, which is consitent with the wide highest occupied molecular orbital-lowest unoccupied molecular orbital gap in these compounds (absorbance at about 300 nm). No characteristic annihilation ECL signal was observed for these compounds in 1:1 MeCN/Bz mixed solvent. However, the ECL of F6 in the presence of the coreactant C2O42- showed a long-wavelength ECL emission that was proposed to be electrolyzed byproduct from the radical cation.en_US
dc.description.sponsorshipWe acknowledge support from the Robert A. Welch Foundation (Grant F-0021) and the National Science Foundation (Grant CHE-1111518). H. L. Qi thanks the National Natural Science Foundation of China (Grants 20805028 and 21027007) and the National Scholarship Fund of China Scholarship Council (Grant 2010687526) for support. We also thank Dr. Fu-Ren F. Fan for valuable discussion and Dr. Alexander B. Nepomnyashchii and Dr. Jungdon Suk for primary study of these compounds.en_US
dc.language.isoenen_US
dc.publisherACS AMERICAN CHEMICAL SOCIETYen_US
dc.subjectENERGY-TRANSFERen_US
dc.subject2-ELECTRON TRANSFERSen_US
dc.subjectSINGLET-STATEen_US
dc.subjectHOST MATERIALen_US
dc.subjectFLUORENEen_US
dc.subjectOXIDATIONen_US
dc.subjectACETONITRILEen_US
dc.subjectDERIVATIVESen_US
dc.subjectMOLECULESen_US
dc.subjectEFFICIENTen_US
dc.titleElectrochemistry and electrogenerated chemiluminescence of π-stacked poly (fluorenemethylene) oligomers. Multiple, interacting electron transfersen_US
dc.typeArticleen_US
dc.identifier.doi10.1021/ja3057997-
dc.relation.journalJOURNAL OF THE AMERICAN CHEMICAL SOCIETY-
dc.contributor.googleauthorQi, Honglan-
dc.contributor.googleauthorChang, Jinho-
dc.contributor.googleauthorAbdelwahed, Sameh H-
dc.contributor.googleauthorThakur, Khushabu-
dc.contributor.googleauthorRathore, Rajendra-
dc.contributor.googleauthorBard, Allen J-
dc.relation.code2012205895-
dc.sector.campusS-
dc.sector.daehakCOLLEGE OF NATURAL SCIENCES[S]-
dc.sector.departmentDEPARTMENT OF CHEMISTRY-
dc.identifier.pidaxceriar-
Appears in Collections:
COLLEGE OF NATURAL SCIENCES[S](자연과학대학) > CHEMISTRY(화학과) > Articles
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