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Preparation and Photochemical Properties of Functionalized Graphene with Ruthenium Complexes

Author: SunYing
Tutor: SongXiMing
School: Liaoning University
Course: Inorganic Chemistry
Keywords: Ruthenium complex graphene polymer ionic liquid
CLC: O613.71
Type: Master's thesis
Year: 2011
Downloads: 173
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Abstract


Graphene have attracted more and more attention due to its many unique chemical and physical properties as an potential material in recent years. In order to further develop its applications, many novel graphene hybrid materials have been prepared through immobilizing different kinds of functional compounds onto the surface of graphene. Tris(2,2’-bipyridine)ruthenium ([Ru(bpy)3]2+) have been fully investigated and used in many fields especially as a photosensitizer because of their remarkable photochemical and photophysical properties. However, ruthenium(II) -graphene hybrid materials haven’t been reported until now. In this thesis, four photoactive ruthenium(II)-graphene hybrid materials were obtained successfully through immobilizing three kinds of ruthenium complexes onto the surface of graphene respectively with covalent or noncovalent bonds.Firstly, three kinds of ruthenium(II) complexes 1a、2a and 1b containing amine group were synthesized and then three novel covalently functionalized graphene 1a-GO 2a-GO and 1b-GO with above three different kinds of Ruthenium(II) complexes respectively were obtained by the amidation reaction. The resulting electron donor-acceptor conjugates was characterized by IR, UV-Vis absorption spectrum and TEM.They also exhibited wide spectral region and more excellent solubility(1a: 380 mg/L; 2a: 323 mg/L mg/L; 1b: 251 mg/L). In their emission spectra, 636 nm for 1a, 630 nm for 1b were observed, but no emission for 2a was found which may be owing to the photoinduced intramolecular electron transfer and energy transfer. Upon excitation of ruthenium complex moieties at their corresponding maximum absorbance band of ruthenium complex 1a, 2a and 1b, the fluorescence emission of the ruthenium complex moieties in the ruthenium(II) -graphene 1a-GO and 1b-GO exhibited different degrees of quenching compared with their correspinding reference ruthenium complex 1a and 1b. The observed luminescence quenching indicates that there is a strong interaction between the excited state of ruthenium complex moieties and graphene moieties in the hybrid materials. Possible pathways for the fluorescence quenching of the excited ruthenium complex moieties may be attributed to two possible competitive processes: photoinduced electron transfer and energy transfer. In the future work, we will further investigate the quenching phenomenon in 1a-GO 2a-GO and 1b-GO by electrochemical method, nanosecond laser flash photolysis and theory calculation etc.Secondly, a novel copolymer poly(Ru-BVImCl) was synthesized through copolymerizing monomer tris(2,2’-bipyridine)ruthenium complex with monomer ionic liquid BVIm Cl. It’s structure was characterized by 1H NMR, GPC and UV-vis spectra. And then the functionalized graphene GO-poly(Ru-BVImCl) with poly(Ru-BVImCl) through a kind of noncovalent method (π-πstacking) in the presence of hydrazinehydrate to give a polymer modified graphene. The resulting hybrid material was characterized by IR and UV-Vis absorption spectrum and emission spectrum.It’s emission spectrum showed that the fluorescence from the Ruthenium(II) complexes moieties was almost half quenched by reduced graphenes,indicating the strong electronic interaction between ruthenium complex moieties and the extendedπ-system of reduced graphene.In addtion, this material exhibited much lower solubility (142.15 mg/L) than that of Ru-graphene 1a-GO because the oxidized graphene was reduced by hydrazinehydrate during the immobilization reaction.

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CLC: > Mathematical sciences and chemical > Chemistry > Inorganic Chemistry > Non-metallic elements and their compounds > Part Ⅳ family of non-metallic elements (carbon and silicon ) and its compounds > Carbon C
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