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Traditional layer-by-layer (LbL) assembled electrodes are mostly multilayer composites formed on two-dimensional membrane materials. In this case, the electroactive material cannot enter the interior of the substrate. With porous aerogels as the substrate, the LbL assembly of the electroactive material into the three-dimensional aerogel skeleton can be realised, greatly improving the utilisation and the electrochemical performance of the electroactive material. To create a promising aerogel electrode for high-performance energy storage devices, we herein report an aerogel based on wood pulp fibre (WPF) and cellulose nanocrystals (CNC), for use as a porous substrate for LbL assembly of nanostructural polyaniline (PANI) and graphene oxide (GO) or carboxylic multi-walled carbon nanotubes (CMCNT). Owing to the uniformly distributed multilayer nanoarchitecture, interpenetrating channels, and hydrophilic character of the cellulosic aerogel substrate, the produced electrodes of (PANI/CMCNT) 10 and (PANI/CMCNT) 10 both display high specific capacitances, favourable capacitance retention, good cycling stabilities, and structural flexibility. In the three-electrode test, their gravimetric specific capacitances are as high as 716.62 and 636.63 F g -1 , respectively. In addition, the assembled symmetric supercapacitors show good areal specific capacitances (1.95 and 1.49 F cm -2 ) in addition to high areal specific energies (168.64 and 113.57 mW h cm -2 , respectively). These results demonstrate that the integration of the LbL-assembled electroactive materials and porous cellulosic aerogel substrate can be a promising strategy to design high-efficiency green energy storage devices.

Layer-by-layer assembled polyaniline/carbon nanomaterial-coated cellulosic aerogel electrodes for high-capacitance supercapacitor applications