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dc.contributor.author
Martín, Roberto
dc.contributor.author
Jimenez, Liliana Beatriz
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dc.contributor.author
Alvaro, Mercedes
dc.contributor.author
Scaiano, Juan Cesar
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dc.contributor.author
Garcia, Hermenegildo
dc.date.available
2019-01-31T15:49:37Z
dc.date.issued
2010-06-21
dc.identifier.citation
Martín, Roberto; Jimenez, Liliana Beatriz; Alvaro, Mercedes; Scaiano, Juan Cesar; Garcia, Hermenegildo; Two-Photon Chemistry in Ruthenium 2,2’-Bipyridyl-Functionalized SingleWall Carbon Nanotubes; Wiley VCH Verlag; Chemistry- A European Journal; 16; 24; 21-6-2010; 7282-7292
dc.identifier.issn
0947-6539
dc.identifier.uri
http://hdl.handle.net/11336/69087
dc.description.abstract
Ruthenium polypyridyl complexes are widely used as light harvesters in dye-sensitized solar cells. Since one of the potential applications of single-wall carbon nanotubes (SWCNTs) and their derived materials is their use as active components in organic and hybrid solar cells, the study of the photochemistry of SWCNTs with tethered ruthenium polypyridyl complexes is important. A water-soluble ruthenium tris(bipyridyl) complex linked through peptidic bonds to SWCNTs (Ru-SWCNTs) was prepared by radical addition of thiol-terminated SWCNT to a terminal C=C double bond of a bipyridyl ligand of the ruthenium tris(bipyridyl) complex. The resulting macromolecular Ru-SWCNT (≈500nm, 15.6% ruthenium complex content) was water-soluble and was characterized by using TEM, thermogravimetric analysis, chemical analysis, and optical spectroscopy. The emission of Ru-SWCNT is 1.6 times weaker than that of a mixture of [Ru(bpy)3]2+ and SWCNT of similar concentration. Time-resolved absorption optical spectroscopy allows the detection of the [Ru(bpy)3]2,+-excited triplet and [Ru(bpy)3]+. The laser flash studies reveal that Ru-SWCNT exhibits an unprecedented two-photon process that is enabled by the semiconducting properties of the SWCNT. Thus, the effect of the excitation wavelength and laser power on the transient spectra indicate that upon excitation of two [Ru(bpy)3]2+ complexes of Ru-SWCNT, a disproportionation process occurs leading to delayed formation of [Ru(bpy) 3]+ and the performance of the SWCNT as a semiconductor. This two-photon delayed [Ru(bpy)3]+ generation is not observed in the photolysis of [Ru(bpy)3]3+; SWCNT acts as an electron wire or electron relay in the disproportionation of two [Ru(bpy)3]2+ triplets in a process that illustrates that the SWCNT plays a key role in the process. We propose a mechanism for this two-photon disproportionation compatible with i) the need for high laser flux, ii) the long lifetime of the [Ru(bpy)3]2+ triplets, iii) the semiconducting properties of the SWNT, and iv) the energy of the HOMO/LUMO levels involved.
dc.format
application/pdf
dc.language.iso
eng
dc.publisher
Wiley VCH Verlag
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dc.rights
info:eu-repo/semantics/openAccess
dc.rights.uri
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.subject
Carbon Nanotubes
dc.subject
Disproportionation
dc.subject
Time-Resolved Spectroscopy
dc.subject
Two-Photon Process
dc.subject.classification
Otras Ciencias Químicas
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dc.subject.classification
Ciencias Químicas
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dc.subject.classification
CIENCIAS NATURALES Y EXACTAS
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dc.title
Two-Photon Chemistry in Ruthenium 2,2’-Bipyridyl-Functionalized SingleWall Carbon Nanotubes
dc.type
info:eu-repo/semantics/article
dc.type
info:ar-repo/semantics/artículo
dc.type
info:eu-repo/semantics/publishedVersion
dc.date.updated
2019-01-14T15:01:18Z
dc.identifier.eissn
1521-3765
dc.journal.volume
16
dc.journal.number
24
dc.journal.pagination
7282-7292
dc.journal.pais
Alemania
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dc.journal.ciudad
Weinheim
dc.description.fil
Fil: Martín, Roberto. Universidad Politécnica de Valencia; España. Consejo Superior de Investigaciones Científicas; España
dc.description.fil
Fil: Jimenez, Liliana Beatriz. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina. University of Ottawa; Canadá
dc.description.fil
Fil: Alvaro, Mercedes. Universidad Politécnica de Valencia; España. Consejo Superior de Investigaciones Científicas; España
dc.description.fil
Fil: Scaiano, Juan Cesar. University of Ottawa; Canadá
dc.description.fil
Fil: Garcia, Hermenegildo. Universidad Politécnica de Valencia; España. Consejo Superior de Investigaciones Científicas; España
dc.journal.title
Chemistry- A European Journal
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dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/url/https://onlinelibrary.wiley.com/doi/full/10.1002/chem.200903506
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/doi/http://dx.doi.org/10.1002/chem.200903506
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