Flexible core/shelled PPy@PANI nanotube porous films for hybrid supercapacitors

Abstract Flexibility of the films and the limited ion transport in the vertical direction of film highly restrict the development of flexible supercapacitors. Herein, we have developed hybrid porous films consisting of N-doped holey graphene nanosheets (NHGR) with abundant in-plane nanopores and the vertically aligned polyaniline nanowires arrays on polypyrrole nanotubes (PPy@PANI) via a two-step oxidative polymerization strategy and vacuum filtration. The rational design can efficiently shorten the diffusion path of electrons/ions, alleviate volume variation of electrodes during cycling, enhance electric conductivity of the hybrids, and while offer abundant active interfacial sites for electrochemical reaction. Benefiting from the distinctive structural and compositional merits, the obtained PPy@PANI/NHGR film electrode manifests an excellent electrochemical properties in terms of specific capacity (1348 mF cm −2 at a current density of 1 mA cm −2 ), rate capability (81.2% capacitance retention from 1 to 30 mA cm −2 ), and cycling stability (capacitance retention of 73.7% at 20 mA cm −2 after 7000 cycles). Matched with NHGR negative electrode, the assembled flexible all-solid-state asymmetric supercapacitor displays a remarkable areal capacitance of 359 mF cm −2 at 5 mA cm −2 , maximum areal energy density of 112.2 μ Wh cm −2 at 3.747 mW cm −2 , and good flexibility at various bending angles while preserving stable cycling performance. The result shows the PPy@PANI/NHGR film with high flexibility and 3D ions transport channels is highly attractive for flexible energy storage devices.