Fabrication of 5 V High-Performance Solid-State Asymmetric Supercapacitor Device Based on MnO₂/Graphene/Ni Electrodes

To reach high energy density and excellent cycle stability, an asymmetric supercapacitor device combining a high-power electric double-layer capacitor (EDLC) anode and high energy density battery-type cathode has been designed and fabricated. A binder-free strategy was used to prepare cathode by coating graphene (G) on Ni foam (Ni), then electrodepositing MnO2, followed by calcination process. The potentiodynamic (PD) electrodeposition cycles of MnO2 onto graphene significantly impact the electrochemical properties. Benefiting from the hierarchical structure and binder-free process of the designed 75 C/G/Ni hybrid cathode, potentiostatic (PS) electrodeposition followed by PD electrodeposition for 75 cycles demonstrates a high specific capacitance of 691 F g−1 at 2 A g−1. The enhanced capacitive performance can be attributed to the synergistic effect between MnO2 nanosheets and graphene, in which graphene can serve as ideal support matrix and conductive channels. Furthermore, an asymmetric supercapacitor was fabricated with 75 C/G/Ni and (G + AC)/Ni as the cathode and anode, respectively, and a carboxymethyl cellulose–potassium hydroxide (CMC-KOH) gel electrolyte. The 75 C/G/Ni//(G + AC)/Ni asymmetric supercapacitor (ASC) exhibits a maximum energy density of 43 kW kg−1 at a power density of 302 W kg−1 with a potential window of 1.6 V and maintains good cycling stability of 88% capacitance retention at 2 A g−1 (over 5000 cycles). Four solid-state asymmetric supercapacitors stack connected in series display an effective 5.0 V working potential to increase the voltage and output energy as a device. The device was charged using a 18,650 Li battery with a voltage of +3.8 V for 30 s and discharged six white LEDs for 20 min. The facile fabrication and remarkable capacitive performance of the MnO2/G/Ni hybrid make it a promising electrode candidate in electrochemical energy conversion/storage devices