Restricted growth of polyaniline nanofiber arrays between holey graphene sheets on carbon cloth towards improved charge storage capacity

The rapid−growing demand for flexible and wearable electronics has driven increased interest in developing porous electrodes with outstanding charge storage capacity especially areal capacity for polymeric and hybrid supercapacitors . Herein, unique porous polyaniline/holey graphene/carbon cloth (PANI/HG/CC) composite electrodes were constructed by combining rapid frozen interfacial polymerization and layer−by−layer spraying to restrict the growth of PANI nanofiber arrays between carbon−based materials. Benefiting from rapid charge transport, more electroactive sites and improved electrolyte penetration provided by hierarchical porous structure and highly oriented PANI nanofibers in the composite (P − G) by growing directly PANI array on the CC and applying graphene sheets as interlayer and cover layer, an areal specific capacitance of 3.22 F cm −2 at 5 mA cm −2 was achieved. A maximum areal energy density of up to 104.86 μWh cm −2 , and excellent capacity retention of 89.5 % at 20 mA cm −2 after 5000 cycles also were achieved for flexible symmetric all−solid−state supercapacitor . Furthermore, the zinc−ion hybrid supercapacitor (P − G||Zn) assembled with P − G cathode and Zn anode could display a capacity of 217.7 mAh g −1 at 0.2 A g −1 , and the maximum energy density of 130.6 Wh kg −1 at the power density of 120 W kg −1 . • Porous composite electrodes were constructed on the CC via rapid frozen interfacial polymerization. • Confined growth of polyaniline nanofiber arrays was restricted to between carbon materials. • Highly oriented growth of the nanofibers was promoted with the help of ice crystals. • Holey graphene provided not only buffer and cladding layer but also rapid charge transport pathway. • Both assembled polymeric and hybrid supercapacitors exhibited excellent charge storage capacity.