Synthesis of a Structurally Controlled Polyacrylonitrile Gel for Energy-Storage Devices by an Organotellerium-Mediated Radical Copolymerization and Subsequent Cross-Linking Reaction

A new polyacrylonitrile (PAN)-based chemically cross linked gel swollen with adiponitrile was prepared for the first time. The host polymer, PAN-copolymer, was prepared by copolymerization of acrylonitrile (AN) and a methacrylamide-bearing amine functional group under organotellurium-mediated radical polymerization (TERP). Excellent control over the molecular weight and dispersity was observed. Then, the copolymers were cross-linked with a bifunctional crosslinker, hexamethylene diisocyanate (HDI), in adiponitrile to obtain the corresponding gel. The rheological study strongly supported the quantitative formation of cross-linking points and a homogeneous gel network. Alkyl dinitriles, such as adiponitrile, have wide electrochemical stability windows, which are suitable for increasing the energy density in energy-storage devices, i.e., Li-ion batteries and super capacitors. In addition, a polymer-gel electrolyte has significant advantages over liquid electrolytes due to its high safety and deformability. Therefore, the current work opens the potential for the development of new energy-storage devices.