Unprecedented Dual Role of Polyaniline for Enhanced Pseudocapacitance of Cobalt–Iron Layered Double Hydroxide

Creating nanosized pores in layered materials can increase the abundant active surface area and boost potential applications of energy storage devices. Herein, a unique synthetic strategy based on polyaniline (PANI) doped 2D cobalt–iron layered double hydroxide (CoFe‐LDH/P) nanomaterials are designed, and the formation of pores at low temperature (80 °C) is developed. It is found that the optimized concentration of PANI creates the nanopores on the CoFe‐LDH nanosheets among all other polymers. The well‐ordered pores of CoFe‐LDH/P allow the high accessibility of the redox‐active sites and promote effective ion diffusion. The optimized CoFe‐LDH/P2 cathode reveals a specific capacitance 1686 (1096 Cg−1) and 1200 Fg−1 (720 Cg−1) at 1 and 30 Ag−1 respectively, a high rate capability (71.2%), and a long cycle life (98% over 10 000 cycles) for supercapacitor applications. Charge storage analysis suggests that the CoFe‐LDH/P2 electrode displays a capacitive‐type storage mechanism (69% capacitive at 1 mV s−1). Moreover, an asymmetric aqueous supercapacitor (CoFe‐LDH/P2//AC) is fabricated, delivering excellent energy density (75.9 Wh kg−1 at 1124 W kg−1) with outstanding stability (97.5%) over 10 000 cycles. This work opens a new avenue for designing porous 2D materials at low temperature for aqueous energy storage devices. Polyaniline doped 2D cobalt–iron layered double hydroxides (CoFe‐LDHs) have a well‐defined 2D morphology, controllable nanopores, high specific surface area, and exhibit superior specific high pseudocapacitive charge storage.