Hierarchical electrodes with superior cycling performance using porous material based on cellulose nanofiber as flexible substrate

The development and application of flexible electrodes with extended cycle life have long been a focal point in the field of energy research. In this study, positively charged polyethylene imine (PEI) and conductive polymer poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) with negative charge were alternately deposited onto a cellulose nanofiber (CNF) porous material utilizing pressure gradient-assisted layer-by-layer (LbL) self-assembly technology. The flexible substrate, characterized by a three-dimensional porous structure reinforced with stiff CNF, not only facilitated high charge storage but also enhanced the electrode's cycling life by reducing the volume changes of PEDOT:PSS. Furthermore, the exceptional wettability of PEI by the electrolyte could promote efficient charge transport within the electrode. The electrode with 10 PEI/PEDOT:PSS bilayer exhibits a capacitance of 63.71 F g- 1 at the scan rate of 5 mV s- 1 and a remarkable capacitance retention of 128 % after 3000 charge-discharge cycles. The investigation into the nanoscale layers of the LbL multilayer structure indicated that the exceptional cyclic performance was primarily attributed to the spatial constraints imposed by the rigid porous substrate layered structure on the deformation of PEDOT:PSS. This work is expected to make a significant contribution to the development of electrodes with high charge storage capacity and ultra-long cycling life.