Tunable capacitive charge storage of NiCoLDH@rGO for high-energy capacitor: Performance of flexible solid-state capacitor

Abstract

The compositionally tunned pristine nickel cobalt layered double hydroxides (NiCoLDHs) and NiCoLDH@reduced graphene-oxide (NiCoLDH@rGO) composites generated via the simple single-pot solvothermal method. The synthesized NiCoLDH and the NiCoLDH@rGO composites were characterized through powder X-ray diffraction (XRD), Raman spectroscopy, Fourier transformed infra-red (FT-IR) spectroscopy, scanning electron microscope (SEM) equipped with energy dispersive X-ray analysis (EDAX), high-resolution transmission electron microscope (HR-TEM), and X-ray photoelectron spectroscopy (XPS) techniques. The XRD, Raman and FT-IR data confirmed the formation of the NiCoLDH with presence of carbonate and nitrate ions in the basal space. Enhanced basal length was observed for the NiCoLDH@rGO composites. The three-electrode system was constructed to analyse the cyclic voltammetry and Galvanostatic charge-discharge studies in 1 M KOH confirmed that the pristine LDHs and the composites are electrochemically active, and the capacity could be tuned by varying (Ni2+/Co3+) mole ratio or the rGO content. The charge storage kinetics in NiCoLDH@rGO was performed through Dunn's approaches and the Power Law, affirmed as the (Ni2+/Co3+) ratio or the rGO content is increased in the composite the capacitive contribution is increased for the charge storage. The NC@RG10 (NiCoLDH with 10 wt% rGO) composite electrode could deliver an enhanced specific capacity of 963C g−1 at a current rate of 1.5 A g−1. Consequently, pristine LDH or composites as positive electrode and rGO as negative electrode was fabricated using the CR-2032 coin-type hybrid capacitor. The laboratory prototype pristine hybrid capacitor (NiCoLDH|1 M KOH|rGO) delivered an enhanced specific energy of 56 Wh kg−1 at specific power of 810 W kg−1, whereas the composite hybrid device (NC@RG10|1 M KOH|rGO) having NC@RG10 electrode delivered an enhanced specific energy of 166 Wh kg−1 at specific power of 638 W kg−1. The NC@RG10 composite-based hybrid device exhibited excellent stability with coulombic efficiency as high as 99 % even at the 10,000th charge−discharge cycle. Reduced aggregation and enhanced conductivity leading to significant capacitive contribution in the NC@RG10 composite is due to the existence of rGO and responsible for the excellent charge storage performance. The fabricated hybrid capacitor powered a red LED on a single charge for 40 min. Fascinatingly, a flexible solid-state hybrid capacitor was also fabricated that delivered an impressive specific energy of 28 Wh kg−1 at a specific power of 553 W kg−1 at a 180° bent angle.