Flexible and green energy storage devices have a wide range of applications in prospective electronics and connected devices. In this study, a new eco-friendly bilayer separator and primary and secondary paper supercapacitors based on manganese dioxide (MnO2)/carbon black (CB) are developed. The bilayer separator is prepared via a two-step fabrication process involving freeze-thawing and nonsolvent-induced phase separation. The prepared bilayer separator exhibits superior porosity of 46%, wettability of 46.5°, and electrolyte uptake of 194% when compared with a Celgard 2320 trilayer separator (39%, 55.58°, and 110%). Moreover, lower bulk resistance yields a higher ionic conductivity of 0.52 mS cm-1 in comparison to 0.22 mS cm-1 for the Celgard separator. Furthermore, the bilayer separator exhibits improved mean efficiency of 0.44% and higher specific discharge capacitance of 13.53%. The anodic and cathodic electrodes are coated on a paper substrate using MnO2/CB and zinc metal-loaded CB composites. The paper supercapacitor demonstrates a high specific capacitance of 34.1 mF cm-2 and energy and power density of 1.70 μWh cm-2 and 204.8 μW cm-2 at 500 μA, respectively. In summary, the concept of an eco-friendly bilayer cellulose separator with paper-based supercapacitors offers an environmentally friendly alternative to traditional energy storage devices.
Keywords: cellulose; eco-friendly; flexible; paper energy storage; separator; supercapacitor.