Abstract
Fullerene-containing materials have the ability to store and release electrical energy. Therefore, fullerenes may ultimately find use in high-voltage equipment devices or as super capacitors for high electric energy storage due to this ease of manipulating their excellent dielectric properties and their high volume resistivity. A series of structured fullerene (C60) polymer nanocomposites were assembled using the thiol-ene click reaction, between alkyl thiols and allyl functionalized C60 derivatives. The resulting high-density C60-urethane-thiol-ene (C60-Thiol-Ene) networks possessed excellent mechanical properties. These novel networks were characterized using standard techniques, including infrared spectroscopy (FTIR), differential scanning calorimetry (DSC), dynamic mechanical analysis (DMA), and thermal gravimetric analysis (TGA). The dielectric spectra for the prepared samples were determined over a broad frequency range at room temperature using a broadband dielectric spectrometer and a semiconductor characterization system. The changes in thermo-mechanical and electrical properties of these novel fullerene-thiol-ene composite films were measured as a function of the C60 content, and samples characterized by high dielectric permittivity and low dielectric loss were produced. In this process, variations in chemical composition of the networks were correlated to performance characteristics.
Highlights
C60 fullerene-containing polymers are receiving increased attention due to their remarkable properties and anticipated applications
There is a sequential buildup of the network from the reaction of hydroxylated fullerene with allyl isocyanate to produce a reactive “ene” monomer and its subsequent reaction with an alkyl “thiol” in the prototypical thiol-ene reaction
A large number of commercially available thiols and enes permits the tailoring of polymer network properties for a variety of applications, and the attractive polymerization rates and uniform polymer networks produced make the thiol-ene matrix an ideal choice for polymer-particle composites [12,13,15]
Summary
C60 fullerene-containing polymers are receiving increased attention due to their remarkable properties and anticipated applications. An interesting feature of these C60-polymer nanocomposites lies in the possibility of tuning the physical properties and resulting potential applications of the composite through modification of the chemical linkages among the matrix constituents Demonstrating this versatility, there are interesting reports of C60’s incorporation into polymer composites as blends to create photo-active and stimuli-responsive coatings [3], C60-derivative-styrene blends [4] and covalent C60-styrene copolymers [5], C60-polyurethanes via reaction of the hydroxylated C60 [6,7], and composites prepared in polyethylene and polyamide matrix materials [8,9]. Multiple relaxations were characterized from the dielectric analysis of this system and assigned to the glass transition temperature (Tg), crankshaft motions of the ether segments, reorientation of the hydroxylated fullerene cages, and other local motions Overall these fullerene-polymer networks could be rendered quite polarizable, but were complicated by a rather challenging synthetic strategy. We report the synthesis and essential characterization of C60-urethane-thiol-ene (C60-Thiol-Ene) networks, thermal stability, mechanical, and dielectric properties
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