Molecular hybrid materials formed from polyoxometalates dispersed in conducting polymers represent an innovative concept in energy storage. This work reports in detail the first practical realization of electrodes based on these materials for energy storage in electrochemical supercapacitors. The molecular hybrids PAni/H4SiW12O40, PAni/H3PW12O40, and PAni/H3PMo12O40 (PAni: polyaniline) have been prepared electrochemically on platinum or carbon substrates, with PAni/H3PMo12O40 being the prototypical example presenting the best energy‐storage performance in the series. This hybrid displays the combined activity of its organic and inorganic components to store and release charge in solid‐state electrochemical capacitor cells, leading to a promising value of 120 F g–1 and good cyclability beyond 1000 cycles.

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In this work, we show a comparative study based on the effects of specific chemical functional groups (-OH, -NH 2 ), grafted on Vulcan carbon (VC) with the incorporation of a specific polyoxometalate (POM), PMo 12 (H 3 PMo 12 O 40 ), to improve electrochemical performance. We observed a decrease in the specific surface area of the grafted matrices (VC-OH and VC-NH 2 ) [1], and the same trend was observed for PMo 12 (POM) incorporation. Our electrochemical studies showed low concentrations of POM in unmodified VCs and higher POM concentrations for grafted matrices (VC-OH and VC-NH 2 ) after 500 voltammetric cycles, especially for the VC grafted with -OH groups (VC-OH-POM). Mechanisms have been proposed for POM interaction with the grafted groups in carbon, emphasizing the role of aqueous medium and redox activity of POM. Cyclic voltammograms suggested the POM anchoring through -OH groups with a strong interaction as a covalent bond, resulting in a surface coverage of 1.66 × 10 −11 mol cm −2. Surface modifications could be extrapolated to other carbons, and the materials could be employed for different potential applications such as photocatalysis, amperometric sensors, fuel cells, and supercapacitors.

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