Design of a Cellulose-Based Supercapacitor Based on Polymerization-Doping Phase Inversion of a Polydopamine-Modified Separator and a Polypyrrole/Graphene-Doped Membrane Electrode.

The cellulose-based polydopamine modified separator (LID-PDA) and polydopamine/graphene/polypyrrole modified electrode (LID-PDA-GR/PPy) were successfully fabricated by dissolving-regenerating and phase-inversion methods via dopamine polymerization and doping modification of graphene (GR) and polypyrrole (PPy) in a lithium chloride/N,N-dimethylacetamide solvent system. The structure and physical properties of the LID-PDA film material play a positive role in its application in supercapacitor separators and electrodes. The effect of PPy content on the electrochemical performance of the electrode shows that the LID-PDA-GR/PPy-30 electrode has the best performance (2.2 Ω, 237.2 F/g at 0.5 A/g). The cellulose-based supercapacitor assembled from the LID-PDA-GR/PPy-30 electrode and LID-PDA separator shows good electrochemical energy storage properties (439.0 F/g at 0.2 A/g, 36.2 Wh/kg corresponding to 2.2 kW/kg). Based on the microstructural properties of natural and renewable cellulose substrates, combining polymerization and doping to realize the complementarity between materials is meaningful for the application and development of energy storage materials.

Construction of Biomass-Derived Hybrid Organogel Electrodes with a Cross-Linking Conductive Network for High-Performance All-Solid-State Supercapacitors.

The biomass-based inter-transmission network architecture is expected to act on all-solid-state supercapacitors (ASSSCs) by building excellent conductive paths and achieving high ionic conductivity to promote their development as future electronic devices. Here, biomass-derived hybrid organogel electrodes constructed by incorporating polyaniline (PANI) into cellulose/dealkaline lignin (C/DL) film architectures exhibit an impressive specific capacitance (582 F g-1 at 1 A g-1) due to the effective dispersion and doping of PANI. Moreover, the specific capacitance of the best C/DL-PANI electrode is nearly 19 times higher than that of a cellulose-PANI electrode, which is attributed to the contribution of DL to the pseudocapacitance. ASSSCs assembled using the C/DL-PANI electrodes and the DL gel electrolyte exhibit excellent specific capacitance (344 F g-1 at 1 A g-1), Coulombic efficiency (∼100% for 5000 cycles), cycle stability (85.7% for 5000 cycles at 1 A g-1), and energy density (58.1 W h kg-1 at 0.5 kW kg-1). The ASSSCs showed a comparable or even higher electrochemical performance than the reported PANI-based or biomass-based ASSSCs, which can be due to the conductive network of the biomass-derived electrodes, the migration of ions between the electrodes through the gel electrolyte ion pathway, and the interfacial synergy. This innovative work paves the way for the development of ASSSC applications based on biomass materials.

Raw cellulose/polyvinyl alcohol blending separators prepared by phase inversion for high-performance supercapacitors.

The development of a biodegradable cellulose-based separator with excellent performance has been of great research significance and application potential for the green development of supercapacitors. Herein, the regenerated porous cellulose/Polyvinyl alcohol films (CP-10, CP-15, CP-20, CP-25) with different mass ratio were successfully fabricated by a simple blending and phase inversion process. Their electrochemical properties as separators in assembled supercapacitor were evaluated. Fourier transform infrared spectroscopy and x-ray diffraction analysis indicate that intermolecular and intramolecular hydrogen bonding existed between cellulose and polyvinyl alcohol of the CP films. Compared with other CP films, the CP-20 film shows higher mechanical strength (28.02 MPa), better wettability (79.06°), higher porosity (59.69%) and electrolyte uptake (281.26 wt%). These properties of CP-20 are expected to show better electrochemical performance as separator. Indeed, the electrochemical tests, including electrochemical impedance spectroscopy, cyclic voltammetry, galvanostatic charge discharge, demonstrate that the SC-20 capacitor (with CP-20 as separator) shows the lowest equivalent series resistance of 0.57 Ω, the highest areal capacitance of 1.98 F cm-2 at 10 mV s-1, specific capacitance of 134.41 F g-1 and charge-discharge efficiency of 98.62% at 1 A g-1 among the four capacitors with CP films as separators. Comparing the assembled SC-40 and SC-30 with two commercial separators (TF4040 and MPF30AC) and SC-PVA with Polyvinyl alcohol (PVA) separator, the CV and GCD curves of SC-20 maintain the quasi rectangular and symmetrical triangular profiles respectively at different scan rates in potential window of 0-1 V. SC-20 exhibits the highest value of 28.24 Wh kg-1 at 0.5 A g-1 with a power density of 0.26 kW kg-1, and 13.41 Wh kg-1 at 10 A g-1 with a power density of 6.04 kW kg-1. SC-20 also shows the lowest voltage drop and the highest areal and specific capacitance. Moreover, SC-20 maintains the highest value of 86.81% after 4000 cycles compared to 21.18% of SC-40, 75.07% of SC-30, and 6.66% of SC-PVA, showing a superior rate capability of a supercapacitor. These results indicate that CP films can be served as promising separators for supercapacitors.