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Photoluminescence of as-synthesized and heat-treated phenyl-containing polysilylcarbodiimides: role of crosslinking and free carbon formation in polymer-derived ceramics

Mera, Gabriela and Menapace, Ilaria and Widgeon, Scarlett and Sen, Sabyasachi and Riedel, Ralf (2013):
Photoluminescence of as-synthesized and heat-treated phenyl-containing polysilylcarbodiimides: role of crosslinking and free carbon formation in polymer-derived ceramics.
In: Applied Organometallic Chemistry, Wiley-VCH Verlag GmbH & Co. KGaA, pp. 630-638, 27, (11), ISSN 02682605,
[Online-Edition: http://dx.doi.org/10.1002/aoc.2993],
[Article]

Abstract

For the first time, photoluminescence properties of four polysilylcarbodiimides, comprised of a phenyl pendant group attached at the silicon atom and a second substituent being either phenyl (S1), methyl (S2), hydrogen (S3) or vinyl (S4), are reported. Distinctive fluorescence emissions are detected in the polymers with one phenyl group at the silicon atom (S2, S3 and S4), due to a phenyl excimer emission. The polymer with two phenyl groups attached at the same silicon atom (S1) shows, besides the phenyl excimer emission, also a vibrationally structured emission stemming from the Ph-SiX2-Ph unit. Moreover, the polysilylcarbodiimides were heat-treated at different temperatures up to 500°C in argon flow. In this case, the amount of crosslinking is identified to be responsible for a bathochromic shift of the maximum emission spectra with increasing annealing temperature. After annealing at 300°C, polymers S2 and S3 present a red-shifted emission due to rearrangement reactions of the basic polymer structure. Furthermore, the presence of free carbon formed during the annealing procedure in the form of polycyclic aromatic hydrocarbons, as well-defined fragments of graphene, are proven to contribute to the photoluminescence properties of the heat-treated polysilylcarbodiimides.

Item Type: Article
Erschienen: 2013
Creators: Mera, Gabriela and Menapace, Ilaria and Widgeon, Scarlett and Sen, Sabyasachi and Riedel, Ralf
Title: Photoluminescence of as-synthesized and heat-treated phenyl-containing polysilylcarbodiimides: role of crosslinking and free carbon formation in polymer-derived ceramics
Language: English
Abstract:

For the first time, photoluminescence properties of four polysilylcarbodiimides, comprised of a phenyl pendant group attached at the silicon atom and a second substituent being either phenyl (S1), methyl (S2), hydrogen (S3) or vinyl (S4), are reported. Distinctive fluorescence emissions are detected in the polymers with one phenyl group at the silicon atom (S2, S3 and S4), due to a phenyl excimer emission. The polymer with two phenyl groups attached at the same silicon atom (S1) shows, besides the phenyl excimer emission, also a vibrationally structured emission stemming from the Ph-SiX2-Ph unit. Moreover, the polysilylcarbodiimides were heat-treated at different temperatures up to 500°C in argon flow. In this case, the amount of crosslinking is identified to be responsible for a bathochromic shift of the maximum emission spectra with increasing annealing temperature. After annealing at 300°C, polymers S2 and S3 present a red-shifted emission due to rearrangement reactions of the basic polymer structure. Furthermore, the presence of free carbon formed during the annealing procedure in the form of polycyclic aromatic hydrocarbons, as well-defined fragments of graphene, are proven to contribute to the photoluminescence properties of the heat-treated polysilylcarbodiimides.

Journal or Publication Title: Applied Organometallic Chemistry
Volume: 27
Number: 11
Publisher: Wiley-VCH Verlag GmbH & Co. KGaA
Uncontrolled Keywords: polysilylcarbodiimides, photoluminescence, crosslinking, polycyclic aromatic hydrocarbons, polymer-derived ceramics
Divisions: 11 Department of Materials and Earth Sciences > Material Science > Dispersive Solids
11 Department of Materials and Earth Sciences > Material Science
11 Department of Materials and Earth Sciences
Date Deposited: 21 Feb 2014 08:33
Official URL: http://dx.doi.org/10.1002/aoc.2993
Identification Number: doi:10.1002/aoc.2993
Funders: This work was financially supported by the European Community FP6 (MCRTN-019601, PolyCerNet). , This work was financially supported by the grant funded under the LOEWE-Zentrum AdRIA (Adaptronik Research, Innovation, Application), by the state of Hesse, Germany., This work was financially supported by the Materials World Network Program between Deutsche Forschungsgemeinschaft (DFG), Bonn, Germany and the National Science Foundation (NSF., This work was financially supported by the Fonds der Chemischen Industrie, Frankfurt, Germany.
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