One-pot synthesis of electro-active polymer gels via Cu(0)-mediated radical polymerization and click chemistry

Recently, poly(2,2,6,6-tetramethylpiperidinyloxy-4-yl methacrylate) (PTMA) has attracted intensive attention for energy storage applications. Organic radical batteries built with this polymer display high power performance. However, the solubility of PTMA in commercial electrolytes shortens the lifespan and the overall performance of the battery. To circumvent this issue, we propose to immobilize PTMA in a three-dimensional network. Indeed, an electrolyte swollen network (gel) enables a good ionic diffusion and brings good mechanical properties to the cathodic material. Here we report on the synthesis of PTMA gels by a combination of Cu(0)-mediated reversible-deactivation radical polymerization and copper-catalyzed azide-alkyne cycloaddition (CuAAC). The structure of the accordingly obtained gels is characterized by NMR, SEC and FTIR and the mechanical properties of these materials are studied by rheology. Finally, their electrochemical performances are studied in the context of organic radical batteries.