Poly(ethylene glycol)–Fullerene Composite Films and Free-Standing Nanosheets for Flexible Electronic Devices and Sensors

A series of ultrathin (80–100 nm) poly(ethylene glycol)–fullerene (PEG-C60) composite films were fabricated by three different methods, denoted immersion, one-pot, and reflux. These films are composed of cross-linked amine-/epoxy-decorated STAR-PEGs and disk-shaped C60 clusters with an average diameter of 314–329 nm and narrow size distribution. The clusters are located either on the surface of the films (immersion) or embedded in their bulk, coupling either physically (one-pot) or chemically (reflux) to the PEG network. The content of C60 in the composite films varies depending on the preparation method and is highest (∼30%) in the case of reflux, featuring also a shift of the lowest unoccupied molecular orbital energy of C60 by ∼70 meV compared to the immersion case. These films exhibit distinct optical and electrochemical properties of C60, merged with some favorable characteristics of the PEG matrix and resulting, in particular, in good electrochemical conductivity and high elasticity. The films can be separated from the substrate, forming composite nanosheets, which can be either used as free-standing ones or transferred to a secondary substrate with the preservation of the original properties. Potential applications of PEG-C60 films and nanosheets include flexible electronic devices, photodetectors, and electrochemical sensors, including biosensors in particular.