The growth and electrical characteristics of vertically oriented graphene nanosheets grown by radio frequency plasma-enhanced chemical vapor deposition from C2H2 feedstock on nickel substrates and used as electrodes in symmetric electric double layer capacitors (EDLC) are presented. The nanosheets exhibited 2.7 times faster growth rate and much greater specific capacitance for a given growth time than CH4 synthesized films. Raman spectra showed that the intensity ratio of the D band to G band versus temperature initially decreased to a minimum value of 0.45 at a growth temperature of 750 °C, but increased rapidly with further temperature increase (1.15 at 850 °C). The AC specific capacitance at 120 Hz of these EDLC devices increased in a linear fashion with growth temperature, up to 265 μF/cm(2) (2 μm high film, 850 °C with 10 min growth). These devices exhibited ultrafast frequency response: the frequency response at -45° phase angle reached over 20 kHz. Consistent with the increase in D band to G band ratio, the morphology of the films became less vertical, less crystalline, and disordered at substrate temperatures of 800 °C and above. This deterioration in morphology resulted in an increase in graphene surface area and defect density, which, in turn, contributed to the increased capacitance, as well as a slight decrease in frequency response. The low equivalent series resistance varied from 0.07 to 0.08 Ω and was attributed to the significant carbon incorporation into the Ni substrate.
Ultra-fast solid electric double layer capacitors (EDLCs) have been developed in both sandwich and planar interdigitated configurations using vertically-oriented graphene nanosheet (VOGN) electrodes with a hydroxide ion-conducting tetraethylammonium hydroxide (TEAOH)-polyvinyl alcohol (PVA) polymer electrolyte. These solid-state EDLCs could be scanned at a rate of 1000 Vs-1 in cyclic voltammetry and demonstrated response times of less than 1 ms. They retained high performance over 18 months of shelf storage and after 100,000 charge/discharge cycles with limited packaging, demonstrating the high stability of TEAOH-PVA electrolyte. The solid-state capacitors are capable of
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