In an effort to dramatically increase the capacity and electronic conductivity of organic-based redox active materials for electrochemical/electrical energy storage applications, polypyrrole (PPy) has been used as an anchoring backbone to form a family of dimethoxybenzene-(DMB-), bis(methylthio)benzene- (BMTB-), N, N, N', N'-tetramethylphenylenediamine-(TMPD-), and N, N, N', N'-tetramethylbenzidine-(TMB-) functionalized redox-active polymers. PPy was deliberately modified to provide an electronically conducting backbone with redox active pendants (RAPs) to enable immobilization (via electropolymerization) of the polymers onto current collectors. The RAPs dramatically increase the capacities of the materials by the reversible exchange of multiple electrons per formula unit. The electropolymerization of the pyrrole-anchored RAP monomers was achieved via cyclic voltammetry. The stability of the electropolymerized films was highly dependent upon the redox potential of the RAPs. The effects of charge density, during the electropolymerization process, were studied by varying the structure of the monomers. By the systematic characterization of the electrochemical properties of the electropolymerized films, the electrochemical behavior of these polymers provides validation of our targeted design to maximize the energy density of organic electrode materials for electrical energy storage applications. With limited fossil fuel reserves and accelerating climate change, the world is shifting towards using renewable and sustainable energy sources. This shift requires dramatic improvements in the fields of carbon-neutral, renewable energy conversion, and, most importantly, the subsequent electrical energy storage technologies. As a result, electrical energy storage (EES) technologies such as batteries and electrochemical capacitors represent one of the fastest developing fields for use in areas such as transportation, electronics, and grid energy storage.1,2 Among these technologies, lithium-ion batteries (LIBs) exhibit among the best combined properties in terms of energy and power density. [3][4][5] In these devices, lithium-intercalated materials (LIM), especially LiC 6 , are used as the anode, as they represent safer alternatives to lithium metal anodes which are prone to lithium dendrite growth that severely compromises safety.6-11 Numerous lithium transition-metal oxides (LiM x O y ) have been developed as cathode materials and have dramatically increased the energy density of the devices. 4,12 However, the use of LIM as anodes and LiM x O y cathodes is limited, at least in part, by the availability of lithium and transition metals.2,13 Moreover, the limited ability of LiM x O y cathodes to undergo multiple electron transfers per formula unit and their moderate working voltages limit the energy density of these materials.
12In addition, the use of intercalation materials often places limits on the operational C-rates, effectively limiting power density. Organic molecules represent attractive alternatives as they are co...