Free-standing PEDOT/polyaniline conductive polymer hydrogel for flexible solid-state supercapacitors

In comparison with inorganic and dry polymeric materials, conductive polymer hydrogels are promising soft electrode materials due to their unique solid-liquid interface. Nevertheless, the existing hydrogels lack either excellent electrochemical performance or mechanical resilience. Here we report a strategy to overcome this limitation by integrating two types of conducting polymers – polyaniline and PEDOT – through a molecular bridge provided by phytic acid. The acid replaces some of PSS, promoting transformation of PEDOT chains from the benzoic structure to the quinoid structure. The resulting hydrogel consists of a 3D network of PEDOT sheets where PANi are inlaid; it has highly improved mechanical properties in comparison with PEDOT hydrogel due to molecular interactions between PANi and PEDOT. A flexible solid-state supercapacitor based on PEDOT/PANi hydrogel delivered a high volumetric energy density of 0.25 mWh cm−3 at a power density of 107.14 mW cm−3, surpassing many of previously reported solid-state supercapacitors based on PEDOT and hydrogels of other conducting polymers and graphene oxide. This study represents a new direction for the development of conductive polymer composite hydrogels which combine excellent electrochemical performance with mechanical resilience.